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  • 51. Malinovskiy, Dmitry
    et al.
    Rodushkin, Ilia
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.
    Forsberg, Jerry
    Pekka, Larisa
    Luleå University of Technology.
    Andren, Henrik
    Stenberg, Anna
    Baxter, Douglas
    Öhlander, Björn
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.
    Forsling, Willis
    Pontér, Christer
    Kinetic and equilibrium Fe isotope fractionation during redox cycling of Fe in seasonally anoxic lake water2004In: 2004 Winter conference on plasma spectrochemistry: : [... Fort Lauderdale, FL, USA, January 5 - 10, 2004 ...], Cambridge: Royal Society of Chemistry, 2004Conference paper (Refereed)
  • 52. Malinovskiy, Dmitry
    et al.
    Rodushkin, Ilya
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.
    Baxter, Douglas
    Ingri, Johan
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.
    Öhlander, Björn
    Molybdenum isotope ratio measurements on geological samples by MC-ICPMS2005In: International Journal of Mass Spectrometry, ISSN 1387-3806, E-ISSN 1873-2798, Vol. 245, no 1-3, p. 94-107Article in journal (Refereed)
    Abstract [en]

    A method using multiple-collector inductively coupled plasma mass spectrometry (MC-ICPMS) for the precise measurement of Mo isotopic composition in geological samples has been developed. Purification of Mo for isotope ratio measurements was realized by ion-exchange chromatography using the chelating resin Chelex-100. This technique allows an efficient separation of Mo from an excess of Fe in samples and at the same time provides quantitative recovery of Mo. Instrumental mass discrimination is corrected by using Pd spiking and normalization to the 105Pd/104Pd ratio. Mo isotope ratios of samples are expressed in per mil relative to those of the bracketing in-house Mo standard. The long-term reproducibility at the two standard deviation level is 0.04, 0.06, 0.08 and 0.14‰ for 96Mo/95Mo, 97Mo/95Mo, 98Mo/95Mo and 100Mo/95Mo ratio measurements, respectively. The technique has been applied to measurement of the Mo isotopic composition of freshwater sediments and molybdenites. Mass-dependent variations in the isotopic composition of Mo spanning the range of 2.2‰ in terms of the 97Mo/95Mo ratio for two sediment columns from different redox environments have been resolved. These results show that Mo isotope effects induced by geochemical processes operating during weathering and transport of Mo to the oceans should be quantified in order to interpret global Mo isotope budget and make use of stable Mo isotopes as proxy for redox conditions in the geological past.

  • 53. Malinovskiy, Dmitry
    et al.
    Rodushkin, Ilya
    Moiseenko, T.
    Institute of Water Problems. Russian Academy of Science.
    Öhlander, Björn
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.
    Aqueous transport and fate of pollutants in mining area: a case study of Khibiny apatite-nepheline mines, the Kola Peninsula, Russia: a case study of Khibiny apatite-nepheline mines, the Kola Peninsula, Russia2002In: Environmental Geology, ISSN 0943-0105, E-ISSN 1432-0495, Vol. 43, no 1-2, p. 172-187Article in journal (Refereed)
    Abstract [en]

    Seven decades of mining activity on the Khibiny apatite-nepheline ore deposits and current large excavation volumes have resulted in elevated concentrations of total dissolved solids and metals in various waters near the mines. To assess the major sources of pollution inputs and fate of pollutants in watercourses draining the mine workings, snow cover, surface waters, and deposited and suspended sediments were sampled and analyzed. Water chemistry data showed that discharges of the mine wastewater are the main contributor to solute and metal loads in the streams. Atmospheric transport of metals and their accumulation in the snowpack account for a sharp increase in metal concentrations in stream waters during spring snowmelt. Data on bed and suspended sediments indicated that the streams have a low capacity of immobilization of metals. The dominant mechanism responsible for decrease in solutes in watercourses is dilution. The results demonstrated the necessity for remediation actions to address pollutant loads due to wastewater discharges

  • 54. Malinovskiy, Dmitry
    et al.
    Rodushkin, Ilya
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.
    Shcherbakova, Elena
    Ponter, Christer
    Analytica AB.
    Öhlander, Björn
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.
    Ingri, Johan
    Fractionation of Fe isotopes as a result of redox process in a basin2005In: Geohimiâ, ISSN 0016-7525, Vol. 43, no 8, p. 878-885Article in journal (Refereed)
    Abstract [en]

    This paper presents the results of a study of Fe isotope fractionation due to seasonal redox variations in water and bottom sediments (BS) of fresh-water basins. Fe isotopic ratios were measured using multicollector inductively coupled plasma mass spectrometry (MC-ICP-MS). The investigation of suspended matter (SM) at the oxic-anoxic interface showed a significant positive shift in δ56Fe values between anoxic waters with dissolved Fe(II) and SM after Fe(II) oxidation and precipitation of Fe(III) oxides. Data on Fe content and isotope composition suggest that Fe(II) oxidation is accompanied by equilibrium Fe isotope fractionation. Potentials and limitations of the use of Fe isotope data for the reconstruction of pre-existing geochemical conditions in basins are outlined

  • 55. Malinovskiy, Dmitry
    et al.
    Rodushkin, Ilya
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.
    Öhlander, Björn
    Determination of the isotopic composition of molybdenum in the bottom sediments of freshwater basins2007In: Geochemistry International, ISSN 0016-7029, E-ISSN 1556-1968, Vol. 45, no 4, p. 381-389Article in journal (Refereed)
    Abstract [en]

    This paper presents the results of measurements of the Mo isotopic composition in the bottom sediments (BS) of freshwater basins. Mo isotopic ratios were measured using a multicollector inductively coupled plasma mass spectrometer (MC ICP MS). Efficient methods were used in this study for Mo separation from the elements of the sample matrix and correction for instrumental mass discrimination. This allowed us to achieve a high accuracy of 0.06, 0.08, and 0.14‰ (2 σ) for the measurement of 97Mo/95Mo, 98Mo/95Mo, and 100Mo/95Mo, respectively. The range of variations in Mo isotope ratios observed in the collected BS columns was ∼2.2‰ in terms of δ97Mo/95Mo. The results obtained here suggest that geochemical processes occurring during Mo migration with land water can change the isotopic composition of Mo. It is pointed out that the potential use of Mo isotopic systematics for reconstructions of redox conditions in seawater over the geologic past requires the quantification of isotopic effects of Mo accompanying its migration on land and the extent of possible variations in the isotopic composition of Mo entering the ocean.

  • 56.
    Malinovskiy, Dmitry
    et al.
    Luleå University of Technology.
    Stenberg, Anna
    Luleå University of Technology.
    Rodushkin, Ilia
    Analytica AB, Luleå, Sweden .
    Andren, Henrik
    Luleå University of Technology.
    Ingri, Johan
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.
    Öhlander, Björn
    Luleå University of Technology.
    Baxter, Douglas C.
    Luleå University of Technology.
    Performance of high resolution MC-ICP-MS for Fe isotope ratio measurements in sedimentary geological materials2003In: Journal of Analytical Atomic Spectrometry, ISSN 0267-9477, E-ISSN 1364-5544, Vol. 18, no 7, p. 687-695Article in journal (Refereed)
    Abstract [en]

    High resolution MC-ICP-MS is used for the precise measurement of variations in the isotopic composition of Fe in ferromanganese concretions and sediments relative to IRMM-014 standard. The sensitivity for 56Fe in high resolution mode was 3 V per mg lm1 Fe, a figure that is comparable to those from other MC-ICP-MS instruments operated at low resolution. Incorporation of a guard electrode and the efficient ion transmission capabilities of the Neptune MC-ICP-MS instrument are responsible for the high sensitivity. It was observed that the use of HCl resulted in the formation of ClOH+, causing interference with 54Fe in particular. This acid has been preferred in some cases over HNO3 to minimize formation of ArN+, the major interferent for 54Fe. Using the high resolution mode of the Neptune, the nature of spectral interferences is unimportant as all are completely resolved and will not affect the accuracy of the determined Fe isotope ratios. As the instrument also provides flat-topped peaks, high resolution operation does not necessarily result in impaired precision, providing that higher concentrations are used to compensate for the loss in sensitivity compared with the low resolution mode. In the present work, external reproducibilities of 56Fe/54Fe and 57Fe/54Fe isotope ratios were better than 50 ppm (one standard deviation) at a concentration of 5 mg lm1. The level of instrumental mass discrimination observed for raw ratios drifted by as much as 0.09% per mass unit over a measurement session, but could be corrected on-line by simultaneous monitoring of the 62Ni/60Ni isotope ratio. Variations in the Fe concentrations or the acid strength of measurement solutions were found to affect the apparent mass discrimination. Increasing the Fe concentration caused a relative decrease in the raw 56Fe/54Fe and 57Fe/54Fe isotope ratios, thus ruling out the space charge effect as the explanation for this phenomenon. Instead, it is suggested that the larger dry aerosol particles formed at higher Fe concentrations are not completely vaporized until later in the plasma, thus reducing the relative rate of diffusional losses of lighter 54Fe from the central channel. However, application of on-line correction using Ni could adequately account for this effect. From the results for a variety of sedimentary geological materials, analysis of three-isotope data revealed that equilibrium fractionation of Fe occurred during deposition. To be able to distinguish between equilibrium and kinetic fractionation processes, it is imperative to collect accurate and precise data for the 56Fe/54Fe and 57Fe/54Fe isotope ratios. These requirements are readily fulfilled by applying high resolution MC-ICP-MS and on-line correction for instrumental mass discrimination using Ni.

  • 57.
    Marinov, A.
    et al.
    Racah Institute of Physics, Hebrew University of Jerusalem, Jerusalem 91904, Israel.
    Rodushkin, Ilya
    Analytica AB, S-977 75 Luleå, Aurorum 10, Sweden.
    Kashiv, Y.
    Racah Institute of Physics, Hebrew University of Jerusalem, Jerusalem 91904, Israel.
    Halicz, L.
    Geological Survey of Israel, Jerusalem 95501, 30 Malkhei Israel St., Israel.
    Segal, I.
    Geological Survey of Israel, Jerusalem 95501, 30 Malkhei Israel St., Israel.
    Pape, A.
    IPHC-UMR7178, IN2P3-CNRS/ULP, F-67037 Strasbourg Cedex 2, BP 28, France.
    Gentry, R.V.
    Earth Science Associates, Knoxville, TN 37912-0067, P. O. Box 12067, United States.
    Miller, H.W.
    Boulder, CO 80306-1092, P. O. Box 1092, United States.
    Kolb, D.
    Department of Physics, University GH Kassel, D-34109 Kassel, Germany.
    Brandt, R.
    Kernchemie, Philipps University, D-35041 Marburg, Germany.
    Reply to "Comment on `Existence of long-lived isomeric states in naturally-occurring neutron-deficient Th isotopes'"2009In: Physical Review C. Nuclear Physics, ISSN 0556-2813, E-ISSN 1089-490X, Vol. 79, no 4, p. 49802-Article in journal (Other academic)
  • 58.
    Marinov, A.
    et al.
    Racah Institute of Physics, Hebrew University of Jerusalem.
    Rodushkin, Ilya
    Kolb, D.
    Department of Physics, University GH Kassel.
    Pape, A.
    IPHC-UMR7178, IN2P3-CNRS/ULP, BP 28, F-67037 Strasbourg.
    Kashiv, Y.
    Racah Institute of Physics, Hebrew University of Jerusalem.
    Brandt, R.
    Kernchemie, Philipps University, D-35041 Marburg.
    Gentry, R V
    Earth Science Associates, P.O. Box 12067, Knoxville, Tennessee.
    Miller, H W
    Evidence for the possible existence of a long-lived superheavy nucleus with atomic mass number A=292 and atomic number Z congruent to 122 in natural Th2010In: International Journal of Modern Physics E, ISSN 0218-3013, Vol. 19, no 1, p. 131-140Article in journal (Refereed)
    Abstract [en]

    Evidence for the possible existence of a superheavy nucleus with atomic mass number A = 292 and abundance of about 1 x 10(-12) relative to Th-232 has been found in a study of natural Th using inductively coupled plasma-sector field mass spectrometry. The measured mass is different from any species with molecular mass of 292, but it matches the predictions for the mass of an isotope with atomic number Z = 122 or a nearby element. Its deduced half-life of t(1/2) >= 10(8) y suggests that a long-lived isomeric state exists in this isotope. The possibility that it might belong to a new class of long-lived high spin super- and hyperdeformed isomeric states is discussed.

  • 59.
    Marinov, Amnon
    et al.
    Racah Institute of Physics, Hebrew University of Jerusalem, Jerusalem 91904, Israel.
    Rodushkin, Ilya
    Analytica AB, S-977 75 Luleå, Aurorum 10, Sweden.
    Kashiv, Y.
    Racah Institute of Physics, Hebrew University of Jerusalem, Jerusalem 91904, Israel.
    Halicz, L.
    Geological Survey of Israel, Jerusalem 95501, 30 Malkhei Israel St., Israel.
    Segal, I.
    Geological Survey of Israel, Jerusalem 95501, 30 Malkhei Israel St., Israel.
    Pape, A.
    IPHC-UMR7178, IN2P3-CNRS/ULP, F-67037 Strasbourg cedex 2, BP 28, France.
    Gentry, R.V.
    Earth Science Associates, Knoxville, TN 37912-0067, P.O. Box 12067, United States.
    Miller, H. W.
    Boulder, CO 80306-1092, P. O. Box 1092, United States.
    Kolb, D.
    Department of Physics, University GH Kassel, D-34109 Kassel, Germany.
    Brandt, R.
    Kernchemie, Philipps University, D-35041 Marburg, Germany.
    Existence of long-lived isomeric states in naturally-occuring neutron-deficient Th isotopes2007In: Physical Review C. Nuclear Physics, ISSN 0556-2813, E-ISSN 1089-490X, Vol. 76, no 2, article id 021303Article in journal (Refereed)
    Abstract [en]

    Four long-lived neutron-deficient Th isotopes with atomic mass numbers 211 to 218 and abundances of (1-10)x10(-11) relative to Th-232 have been found in a study of naturally-occurring Th using inductively coupled plasma-sector field mass spectrometry. It is deduced that long-lived isomeric states exist in these isotopes. The hypothesis that they might belong to a new class of long-lived high spin super- and hyperdeformed isomeric states is discussed.

  • 60. Moiseenko, T.
    et al.
    Dauvalter, V.
    Rodushkin, Ilya
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.
    Geochemical migration and covariation of elements in the Imandra Lake, Barents Region1996Report (Other academic)
  • 61.
    Monti, Carlo
    et al.
    PSO Srl, Milano, Italy.
    Cavanna, Daniele
    Analytical Food Science, Barilla G. e R. Fratelli S.p.A., Parma, Italy.
    Rodushkin, Ilia
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering. ALS Scandinavia, Luleå, Sweden.
    Monti, Arianna
    PSO Srl, Milano, Italy.
    Leporati, Andrea
    Analytical Food Science, Barilla G. e R. Fratelli S.p.A., Parma, Italy.
    Suman, Michele
    Analytical Food Science, Barilla G. e R. Fratelli S.p.A., Parma, Italy; Department for Sustainable Food Process, Catholic University Sacred Heart, Piacenza, Italy.
    Determining the geographical origin of durum wheat samples by combining strontium isotope ratio and multielemental analyses2023In: Cereal Chemistry, ISSN 0009-0352, E-ISSN 1943-3638, Vol. 100, no 2, p. 522-531Article in journal (Refereed)
    Abstract [en]

    Background and objectives: Determining the geographical origin of durum wheat is an important and emerging challenge because consumers perceive added value of final products (e.g., pasta) depending on the origin. Declaration of geographical origin is also an emerging requirement of specific national regulations. Among analytical strategies for determining geographical origins of samples, isotopic techniques based on both light and radiogenic isotope targets stand out, despite limitations of applicability, validation and assessment of interyear variability.

    Findings: In this study, 87Sr/86Sr isotopic analysis was successfully used to discriminate Italian (ITA) samples versus rest-of-the world (RoW) samples and subsequently integrated with an elemental analysis (ICP‒MS) on 75 elements. A tiered approach was finally adopted in which the results of the 87Sr/86Sr analysis were input to a second step of support vector machine classification modeling (SVMC) based on the Al, Mn, Mo, P, S, Ti, Y, and Zn percentages in each sample. This model was tested against a blind group of samples with overall satisfactory performance.

    Conclusion: Valuable information from multielemental and stable isotope ratio analyses was collected for authentic samples from different Italian, European, and non-European regions harvested during different years.

    Significance and novelty: This study demonstrates the potential and validity of an innovative combined multielemental and strontium isotope ratio approach for the geographic discrimination of durum wheat on a global scale: the developed predictive model has already been routinely employed to control industrial lots.

  • 62.
    Nordblad, Fredrik
    et al.
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.
    Rodushkin, Ilya
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering. ALS Scandinavia AB, Aurorum 10, S-977 75 Luleå, Sweden.
    Engström, Emma
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering. ALS Scandinavia AB, Aurorum 10, S-977 75 Luleå, Sweden.
    Ecke, Frauke
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.
    Öhlander, Björn
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.
    Ingri, Johan
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.
    Stream water geochemistry of boron and boron isotopes in a small boreal catchment affected by a major forest fire2009In: Geochimica et Cosmochimica Acta, ISSN 0016-7037, E-ISSN 1872-9533, Vol. 73, no 13, Supp. S, p. A952-Article in journal (Other academic)
    Abstract [en]

    Previous research [1] has suggested that the boron (B) isotope system has a potential to be used as a tracer for detecting historic wood fire events. It was hypothesized that highly elevated B concentrations in sediments of a lake, accompanied by an enrichment of 10B, were a result of an urban wood fire event in the 19th century. The δ11B decrease in these sediments exceeded 9 ., coinciding with a peak in the B concentration.To evaluate this hypothesis, seasonal isotopic pattern of boron (B) was investigated during spring and summer 2007 in a small stream draining a boreal forest area which was severely burnt in a major forest fire in the summer of 2006. Dissolved (< 0.22 µm) boron concentrations of the burnt area were significantly higher compared to a non-burnt reference stream, while 11B/10B ratios were significantly lower. Dissolved δ11B differences between the reference and the burnt area stream were found to be -9 to -22 .. We interpret the elevated B concentrations, accompanied by enrichment of 10B, in the burnt stream as wood and plant ash leaching of biogenic B from the burnt forest by surface run-off. Our results suggest that a boreal forest fire event significantly increases the leached amount of isotopically lighter B in the dissolved phase of stream run-off.[1] Peltola & Åström (2006), Appl. Geochem. 21 (2006) 941-948.

  • 63.
    Nygren, Ulrika
    et al.
    Luleå University of Technology. Swedish Defence Research Agency, Division of NBC Analysis, Umeå, Sweden.
    Rodushkin, Ilya
    Analytica AB, Luleå, Sweden.
    Nilsson, Calle
    Swedish Defence Research Agency, Division of NBC Analysis, Umeå, Sweden.
    Baxter, Douglas C.
    Luleå University of Technology.
    Separation of plutonium from soil and sediment prior to determination by inductively coupled plasma mass spectrometry2003In: Journal of Analytical Atomic Spectrometry, ISSN 0267-9477, E-ISSN 1364-5544, Vol. 18, no 12, p. 1426-1434Article in journal (Refereed)
    Abstract [en]

    The purpose of this work was to develop an optimised sample-preparation procedure for the determination of Pu in soil/sediment with ICP-MS. To start with, several different procedures were screened for their ability to separate plutonium and remove uranium. After the screening, two methods were applied on one soil (IAEA Soil6) and two sediment reference materials (IAEA300 and IAEA135). These methods were based on separation of Pu using TEVA and a combination of UTEVA and TRU resins, followed by elution of Pu with 0.1% hydroxylethylidene diphosphonic acid (HEDPA). A comparison was also made between sample preparation based on acid-leaching and complete digestion using lithium borate fusion. The highest yield of Pu (80%) was found with the procedure consisting of fusion followed by TEVA, while the decontamination from U showed large variations (RSD varying from 16–52%) with all procedures. No difference in the recovery of Pu was found between the two sample preparation techniques. The results of the quantitative determination in low resolution of 239Pu and 240Pu from the UTEVA + TRU-separation were significantly higher than those obtained by the TEVA procedure. An analysis in higher mass resolution displayed interfering peaks in the mass-region of Pu, and lanthanide-containing polyatomic ions were found to be a likely cause for these interferences. The procedure based on lithium borate fusion and separation using the TEVA-resin avoided such interferences and was therefore tested for repeatability over time on IAEA300. The stability of the method was good (RSD = 2.49% (n = 8)), with the exception of one value being significantly higher than the others. This result was confirmed by analysis in higher mass-resolution, which indicates an inhomogeneous distribution of Pu in the reference material, despite a sample intake of about 1 g.

  • 64.
    Olofsson, A
    et al.
    ALS.
    Rodushkin, Ilya
    Provenancing flint artefacts with ICP-MS using reesignatures and Pb isotopes as discriminants: preliminary results of a case study from northern Sweden2011In: Archaeometry, ISSN 0003-813X, E-ISSN 1475-4754, Vol. 53, no 6, p. 1142-1170Article in journal (Refereed)
  • 65.
    Olofsson, Rickard S.
    et al.
    Luleå University of Technology. SGAB Analytica, Luleå, Sweden.
    Rodushkin, Ilya
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering. SGAB Analytica, Luleå, Sweden.
    Axelsson, Mikael D.
    Luleå University of Technology.
    Performance characteristics of a tandem spray chamber arrangement in double focusing sector field ICP-MS2000In: Journal of Analytical Atomic Spectrometry, ISSN 0267-9477, E-ISSN 1364-5544, Vol. 15, no 6, p. 727-729Article in journal (Refereed)
    Abstract [en]

    A tandem cyclone-Scott type spray chamber configuration combined with infrared heating and a low-flow Micromist nebulizer was evaluated for the use in a ICP-SFMS sample introduction system. The system provides about a 3-fold sensitivity gain and lower oxide formation compared to the standard introduction system, although matrix-induced signal suppression is more pronounced, especially for elements with high ionization potential. The technique was evaluated by accurate analysis of riverine water reference material SLRS-3 with generally good agreement with certified and literature values. Long-term precision at a 20rµgrlm1 concentration level was 0.7% RSD in low resolution and 1.6% RSD in medium resolution. Precision in the range 0.03-0.09% RSD for lead isotope ratios at 1rµgrlm1 was obtained.

  • 66.
    Pallavicini, Nicola
    et al.
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.
    Ecke, Frauke
    Swedish University of Agricultural Sciences, Department of Wildlife, Fish and Environmental Studies.
    Engström, Emma
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.
    Baxter, Douglas
    ALS Scandinavia AB.
    Rodushkin, Ilya
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.
    A high-throughput method for the determination of Os concentrations and isotope ratio measurements in small-size biological samples2013In: Journal of Analytical Atomic Spectrometry, ISSN 0267-9477, E-ISSN 1364-5544, Vol. 28, no 10, p. 1591-1599Article in journal (Refereed)
    Abstract [en]

    An analytical method allowing multi-element characterization by external calibration, osmium (Os) concentration determination by isotope dilution (ID) and 187Os/188Os isotope abundance ratio measurement from a single sample preparation was developed. The method consists of microwave-assisted, closed-vessel acid digestion of small (0.01-0.4 g dry weight) biological samples spiked with Os solution enriched in a 190Os isotope followed by concentration and Os isotope ratio measurements using double-focusing, sector field inductively coupled plasma mass-spectrometry (ICP-SFMS) operated with methane addition to the plasma and solution nebulization (SN) sample introduction. For samples with Os content below 500 pg, complementary analysis using gas-phase introduction (GPI) on the remaining sample digests was performed. The use of disposable plastic lab ware for sample digestion and analysis by SN ICP-SFMS circumvents Os carry-over effects and improves the sample throughput and cost-efficiency of the method. For a 0.1 g dried sample, Os method limits of detection (MLODs) of 2 pg g -1 and 0.2 pg g-1 were obtained using SN or GPI, respectively. Long-term reproducibility of 187Os/188Os isotope abundance ratio measurements using the GPI approach was better than 1.5% RSD for our in-house control sample (moose kidney) with an Os concentration of approximately 5 pg g-1. Os data for several commercially available reference materials of biological or plant origin (not certified for Os) are presented. The method was used in the large scale bio-monitoring of free-living bank voles from an area affected by anthropogenic Os emissions.

  • 67.
    Pallavicini, Nicola
    et al.
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering. ALS Laboratory Group, ALS Scandinavia AB, Luleå, Sweden.
    Engström, Emma
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering. ALS Laboratory Group, ALS Scandinavia AB, Luleå, Sweden.
    Baxter, Douglas C.
    ALS Laboratory Group, ALS Scandinavia AB, Luleå, Sweden.
    Öhlander, Björn
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.
    Ingri, Johan
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.
    Hawley, Scott
    Department of Earth Sciences, Durham University, Durham, UK.
    Hirst, Catherine
    Department of Geosciences, Natural History Museum, Stockholm, Sweden.
    Rodushkina, Katerina
    Department of Chemistry, Uppsala University, Uppsala, Sweden.
    Rodushkin, Ilya
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering. ALS Laboratory Group, ALS Scandinavia AB, Luleå, Sweden.
    Ranges of B, Cd, Cr, Cu, Fe, Pb, Sr, Tl, and Zn Concentrations and Isotope Ratios in Environmental Matrices from an Urban Area2018In: Journal of Spectroscopy, ISSN 2314-4920, E-ISSN 2314-4939, p. 1-17, article id 7408767Article in journal (Refereed)
    Abstract [en]

    Isotopic information may provide powerful insight into the elemental cycling processes which occur in natural compartments. Further implementation of isotopic techniques in natural sciences requires a better understanding of the range of elemental and isotopic compositional variability in environmental matrices. This study assesses the local-scale concentration and isotopic composition variability of nine elements: boron (B), cadmium (Cd), chromium (Cr), copper (Cu), iron (Fe), lead (Pb), strontium (Sr), thallium (Tl), and zinc (Zn) in lysimetric waters, mushrooms, litter, needles, leaves, and lichens. Sequential extractions were also performed on soil samples from 6 depth profiles providing more detailed information on the variability of elemental concentrations and isotope ratios between the elemental pools present in soil. For most of the sample types studied the range of isotopic variability between samples spans almost the entire ranges reported in the literature for natural samples. These results represent a starting point for discussing the role of natural variability in isotopic studies (for example, as a limiting factor in the use of isotopic mixing models) and a baseline for future in-depth studies examining the controls on isotope fraction in natural systems

  • 68.
    Pallavicini, Nicola
    et al.
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering. ALS Laboratory Group, ALS Scandinavia AB, Aurorum 10, S-977 75 Luleå, Sweden.
    Engström, Emma
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering. ALS Laboratory Group, ALS Scandinavia AB, Aurorum 10, S-977 75 Luleå, Sweden.
    Baxter, Douglas C.
    ALS Laboratory Group, ALS Scandinavia AB, Aurorum 10, S-977 75 Luleå, Sweden.
    Öhlander, Björn
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.
    Ingri, Johan
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.
    Rodushkin, Ilia
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering. ALS Laboratory Group, ALS Scandinavia AB, Aurorum 10, S-977 75 Luleå, Sweden.
    Cadmium isotope ratio measurements in environmental matrices by MC-ICP-MS2014In: Journal of Analytical Atomic Spectrometry, ISSN 0267-9477, E-ISSN 1364-5544, Vol. 29, no 9, p. 1570-1584Article in journal (Refereed)
    Abstract [en]

    Various stages of an analytical method for high-precision cadmium (Cd) isotope ratio measurements by MC-ICP-MS (sample preparation, matrix separation, instrumental analysis and data evaluation) were critically evaluated and optimized for the processing of carbon-rich environmental samples. Overall reproducibility of the method was assessed by replicate preparation and Cd isotope ratio measurements in various environmental matrices (soil, sediment, Fe-Mn nodules, sludge, kidney, liver, leaves) and was found to be better than 0.1‰ (2σ for δ114Cd/110Cd) for the majority of samples. Cd isotope ratio data for several commercially-available reference materials are presented and compared with previously published results where available. The method was used in a pilot study focusing on the assessment of factors affecting Cd isotope composition in tree leaves. A summary of results obtained for a large number (n > 80) of birch (Betula pubescenes) leaves collected from different locations in Sweden and through the entire growing season is presented and potential reasons for observed variability in Cd isotope composition are discussed. Seasonal dynamics of element concentrations and isotope compositions in leaves were also compared for Os, Pb, Zn and Cd.

  • 69.
    Pontér, Simon
    et al.
    Department of Environmental Science and Analytical Chemistry, Stockholm University, SE-11418 Stockholm, Sweden.
    Pallavicini, Nicola
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering. ALS Laboratory Group, ALS Scandinavia AB, Aurorum 10, S-977 75 Luleå, Sweden.
    Engström, Emma
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering. ALS Laboratory Group, ALS Scandinavia AB, Aurorum 10, S-977 75 Luleå, Sweden.
    Baxter, Douglas
    ALS Laboratory Group, ALS Scandinavia AB, Aurorum 10, S-977 75 Luleå, Sweden.
    Rodushkin, Ilia
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering. ALS Laboratory Group, ALS Scandinavia AB, Aurorum 10, S-977 75 Luleå, Sweden.
    Chromium isotope ratio measurements in environmental matrices by MC-ICP-MS2016In: Journal of Analytical Atomic Spectrometry, ISSN 0267-9477, E-ISSN 1364-5544, Vol. 31, no 7, p. 1464-1471Article in journal (Refereed)
    Abstract [en]

    An analytical procedure consisting of high pressure/temperature acid digestion using an UltraCLAVE system and a one pass, single column matrix separation using DOWEX AG 1X8 anion exchange resin was applied to the determination of Cr concentrations and δ53Cr in chromites, soils, and biological matrices (epiphytic lichens and mosses) using a combination of ICP-SFMS and MC-ICP-MS. The overall reproducibility of the method was assessed by replicate preparation and Cr isotope ratio measurements performed by different operators in multiple analytical sessions over a few months and was found to be 0.11‰ (2σ). The accuracy was evaluated using commercially available reference materials for which measured data were compared with certified values (for Cr concentrations) and previously published results (for isotope data). The results demonstrate a uniform Cr isotope composition in soil depth profiles sampled in different urban environments. A strong negative correlation between δ53Cr and Cr concentrations in lichens and mosses indicates that airborne Cr from local anthropogenic source(s) is depleted in heavy isotopes.

  • 70.
    Pontér, Simon
    et al.
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering. ALS Laboratory Group, ALS Scandinavia AB, Aurorum 10, S-977 75 Luleå, Sweden.
    Rodushkin, Ilia
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering. ALS Laboratory Group, ALS Scandinavia AB, Aurorum 10, S-977 75 Luleå, Sweden.
    Engström, Emma
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering. ALS Laboratory Group, ALS Scandinavia AB, Aurorum 10, S-977 75 Luleå, Sweden.
    Rodushkina, Katerina
    ALS Laboratory Group, ALS Scandinavia AB, Aurorum 10, S-977 75 Luleå, Sweden.
    Paulukat, Cora
    ALS Laboratory Group, ALS Scandinavia AB, Aurorum 10, S-977 75 Luleå, Sweden.
    Peinerud, Elsa
    Luossavaara-Kiirunavaara AB, S-981 86 Kiruna, Sweden.
    Widerlund, Anders
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.
    Early diagenesis of uranium in lakes receiving deep groundwater from the Kiruna mine, northern Sweden2021In: Science of the Total Environment, ISSN 0048-9697, E-ISSN 1879-1026, Vol. 793, article id 148441Article in journal (Refereed)
    Abstract [en]

    The uranium (U) concentrations and isotopic composition of waters and sediment cores were used to investigate the transport and accumulation of U in a water system (tailings pond, two lakes, and the Kalix River) receiving mine waters from the Kiruna mine. Concentrations of dissolved U decrease two orders of magnitude between the inflow of mine waters and in the Kalix River, while the concentration of the element bound to particulate matter increases, most likely due to sorption on iron‑manganese hydroxides and organic matter. The vertical distribution of U in the water column differs between two polluted lakes with a potential indication of dissolved U supply from sediment's pore waters at anoxic conditions. Since the beginning of exposure in the 1950s, U concentrations in lake sediments have increased >20-fold, reaching concentrations above 50 μg g-1. The distribution of anthropogenic U between the lakes does not follow the distribution of other mine water contaminants, with a higher relative proportion of U accumulating in the sediments of the second lake.

    Concentrations of redox-sensitive elements in the sediment core as well as Fe isotopic composition were used to re-construct past redox-conditions potentially controlling early diagenesis of U in surface sediments. Two analytical techniques (ICP-SFMS and MC-ICP-MS) were used for the determination of U isotopic composition, providing an extra dimension in the understanding of processes in the system. The (234 U)/(238 U) activity ratio (AR) is rather uniform in the tailings pond but varies considerably in water and lake sediments providing a potential tracer for U transport from the Kiruna mine through the water system, and U immobilization in sediments. The U mass balance in the Rakkurijoki system as well as the amount of anthropogenic U accumulated in lake sediments were evaluated, indicating the immobilization in the two lakes of 170 kg and 285 kg U, respectively.

  • 71.
    Pontér, Simon
    et al.
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering. ALS Laboratory Group, ALS Scandinavia AB, Aurorum 10, S-977 75 Luleå, Sweden.
    Sutliff-Johansson, Stacy
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.
    Engström, Emma
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering. ALS Laboratory Group, ALS Scandinavia AB, Aurorum 10, S-977 75 Luleå, Sweden.
    Widerlund, Anders
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.
    Mäki, Anna
    Vatten & Miljökonsulterna AB, Aurorum 2, S-977 75 Luleå, Sweden.
    Rodushkina, Katerina
    ALS Laboratory Group, ALS Scandinavia AB, Aurorum 10, S-977 75 Luleå, Sweden.
    Paulukat, Cora
    ALS Laboratory Group, ALS Scandinavia AB, Aurorum 10, S-977 75 Luleå, Sweden.
    Rodushkin, Ilia
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering. ALS Laboratory Group, ALS Scandinavia AB, Aurorum 10, S-977 75 Luleå, Sweden.
    Evaluation of a Multi-Isotope Approach as a Complement to Concentration Data within Environmental Forensics2021In: Minerals, E-ISSN 2075-163X, Vol. 11, no 1, article id 37Article in journal (Refereed)
    Abstract [en]

    Heavy metal contamination was identified in groundwater monitoring wells surrounding a waste deposit facility at the Rönnskär Cu–Pb–Zn smelter in Skellefteå, Northern Sweden, as well as in brackish water and sediments from the nearby harbor. Following an investigative study of the surrounding area, brackish water from the Baltic Sea and sediments from a nearby harbor were also determined to be contaminated. This study investigated the ranges of isotopic compositions of four elements (Cd, Cu, Pb, and Zn) in smelter materials (ores, products, and waste) and polluted groundwater sediments of the affected area. The study’s objective was to evaluate the variability of the polluting source and identify possible isotope fractionation. This study further assesses the viability of using isotopic information to identify the source of the pollutant. These data were used in combination with multi-element screening analysis and multivariate statistical techniques. Expanding the number of elements utilized in isotope tracing empowers our abilities to decipher the source(s) and the extent of environmental exposure from contamination events related to mining and refining operations.

  • 72.
    Pérez Rodríguez, Nathalie
    et al.
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.
    Langella, Francesca
    Institute for Microbiology, Friedrich-Schiller-University, 07740, Jena, Germany.
    Rodushkin, Ilya
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering. Research and Development, ALS Scandinavia AB, Aurorum 10, 97775, Luleå, Sweden.
    Engström, Emma
    Research and Development, ALS Scandinavia AB, Aurorum 10, 97775, Luleå, Sweden.
    Kothe, Erika
    Institute for Microbiology, Friedrich-Schiller-University, 07740, Jena, Germany.
    Alakangas, Lena
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.
    Öhlander, Björn
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.
    The role of bacterial consortium and organic amendment in Cu and Fe isotope fractionation in plants on a polluted mine site2014In: Environmental Science and Pollution Research, ISSN 0944-1344, E-ISSN 1614-7499, Vol. 21, no 11, p. 6836-6844Article in journal (Refereed)
    Abstract [en]

    Copper and iron isotope fractionation by plant uptake and translocation is a matter of current research. As a way to apply the use of Cu and Fe stable isotopes in the phytoremediation of contaminated sites, the effects of organic amendment and microbial addition in a mine spoiled soil seeded with Helianthus annuus in pot experiments and field trials were studied. Results show that the addition of a microbial consortium of ten bacterial strains has an influence on Cu and Fe isotope fractionation by the uptake and translocation in pot experiments, with an increase in average of 0.99‰ for the δ65Cu values from soil to roots. In the field trial, the amendment with the addition of bacteria and mycorrhiza as single and double inoculation enriches the leaves in 65Cu compared to the soil. As a result of the same trial, the δ56Fe values in the leaves are lower than those from the bulk soil, although some differences are seen according to the amendment used. Siderophores, possibly released by the bacterial consortium, can be responsible for this change in the Cu and Fe fractionation. The overall isotopic fractionation trend for Cu and Fe does not vary for pots and field experiments with or without bacteria. However variations in specific metabolic pathways related to metal-organic complexation and weathering can modify particular isotopic signatures.

  • 73.
    Qvarforth, A.
    et al.
    Department of Biology and Environmental Science, Linnaeus University, Kalmar, Sweden.
    Lundgren, M.
    Department of Biology and Environmental Science, Linnaeus University, Kalmar, Sweden.
    Rodushkin, Ilia
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering. ALS Laboratory Group, ALS Scandinavia AB, Luleå, Sweden.
    Engström, Emma
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering. ALS Laboratory Group, ALS Scandinavia AB, Luleå, Sweden.
    Paulukat, C.
    ALS Laboratory Group, ALS Scandinavia AB, Luleå, Sweden.
    Hough, R. L.
    The James Hutton Institute, Craigiebuckler, Aberdeen, UK.
    Moreno-Jiménez, E.
    Univ Autonoma Madrid, Fac Sci, Dept Agr & Food Chem, Madrid, Spain; Department of Biology, Chemistry, Pharmacy, Institute of Biology, Freie Universität Berlin, Berlin, Germany; Berlin‐Brandenburg Institute of Advanced Biodiversity Research, Berlin, Germany; Department of Environmental Geosciences, Faculty of Environmental Sciences, Czech University of Life Sciences Prague, Czech Republic.
    Beesley, L.
    The James Hutton Institute, Craigiebuckler, Aberdeen, UK; Department of Environmental Geosciences, Faculty of Environmental Sciences, Czech University of Life Sciences Prague, Czech Republic.
    Trakal, L.
    Department of Environmental Geosciences, Faculty of Environmental Sciences, Czech University of Life Sciences Prague, Czech Republic.
    Augustsson, A.
    Department of Biology and Environmental Science, Linnaeus University, Kalmar, Sweden.
    Future food contaminants: An assessment of the plant uptake of Technology-critical elements versus traditional metal contaminants2022In: Environment International, ISSN 0160-4120, E-ISSN 1873-6750, Vol. 169, article id 107504Article in journal (Refereed)
    Abstract [en]

    Technology-critical elements (TCEs) include most rare earth elements (REEs), the platinum group elements (PGEs), and Ga, Ge, In, Nb, Ta, Te, and Tl. Despite increasing recognition of their prolific release into the environment, their soil to plant transfer remains largely unknown. This paper provides an approximation of the potential for plant uptake by calculating bioconcentration factors (BCFs), defined as the concentration in edible vegetable tissues relative to that in cultivation soil. Here data were obtained from an indoor cultivation experiment growing lettuce, chard, and carrot on 22 different European urban soils. Values of BCFs were determined from concentrations of TCEs in vegetable samples after digestion with concentrated HNO3, and from concentrations in soil determined after 1) Aqua Regia digestion and, 2) diluted (0.1 M) HNO3 leaching. For comparison, BCFs were also determined for 5 traditional metal contaminants (TMCs; As, Cd, Cu, Pb, and Zn). The main conclusions of the study were that: 1) BCF values for the REEs were consistently low in the studied vegetables;2) the BCFs for Ga and Nb were low as well;3) the BCFs for Tl were high relative to the other measured TCEs and the traditional metal contaminants; and 4) mean BCF values for the investigated TCEs were generally highest in chard and lowest in carrot. These findings provide initial evidence that there are likely to be real and present soil-plant transfer of TCEs, especially in the case of Tl. Improvements in analytical methods and detection limits will allow this to be further investigated in a wider variety of edible plants so that a risk profile may be developed.

  • 74.
    Rapa, Mattia
    et al.
    Department of Management, Sapienza University of Rome, Rome, Italy.
    Ferrante, Marco
    Trace Technologies S.r.l, Nereto, Italy.
    Rodushkin, Ilia
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering. ALS Scandinavia AB, Luleå, Sweden.
    Paulukat, Cora
    ALS Scandinavia AB, Luleå, Sweden.
    Conti, Marcelo Enrique
    Department of Management, Sapienza University of Rome, Rome, Italy.
    Heavy metals, rare earth elements and isotopic fingerprint of Venetian Protected Designation of Origin sparkling wines2023In: British Food Journal, ISSN 0007-070X, E-ISSN 1758-4108, Vol. 125, no 7, p. 2644-2662Article in journal (Refereed)
    Abstract [en]

    Purpose:

    World imports of Italian sparkling wines fell by 9% in value and 5% in quantities. In view of this, the quality characterisation of these products is desirable to increase their market value and restore their global visibility.

    Design/methodology/approach:

    For this purpose, in this paper, heavy metals (Cd, Co, Cr, Cu, Fe, Ga, Hf, Hg, Mn, Mo, Nb, Ni, Pb, Re, Sb, Sn, Ta, Th, Tl, U, W, V, Zn, Zr), rare Earth elements (REEs) (Ce, Dy, Er, Eu, Gd, Ho, La, Lu, Nd, Pr, Sm, Tb, Tm, Yb) and isotopes ratio (208Pb/206Pb, 207Pb/206Pb, 206Pb/204Pb, 208Pb/207Pb, 87Sr/86Sr) were analysed in Italian sparkling wines with Protected Designation of Origin (PDO) certification by High Resolution Inductively Coupled Plasma Mass Spectrometry (HR-ICP-MS) and MultiCollector Inductively Coupled Plasma Mass Spectrometer (MC-ICP-MS). The samples were produced in the Veneto region, and they were compared to white and red wines from the same area.

    Findings:

    Sparkling wines present a characteristic elemental pattern compared to white and red ones, with lower content of heavy metals and higher content in REEs. The ratio 87Sr/86Sr resulted in a powerful micro-scale geographical origins marker while Pb ratios as winemaking process one, both useful to prevent possible frauds. Multivariate data analyses, such as PCA and PLS-DA, were used to develop a model of recognition of Venetian sparkling wines.

    Originality/value:

    The good classification of sparkling wines was achieved (95%), proving the suitable use of these analytes as markers for recognising sparkling wines and their geographical origin verification. To the best of the authors’ knowledge, this is the first study investigating heavy metals, REEs and isotopes in Venetian sparkling wine for their recognition.

  • 75.
    Rapa, Mattia
    et al.
    Department of Management, Sapienza University of Rome, Rome, Italy.
    Ferrante, Marco
    Trace Technologies S.r.l., Nereto, Teramo, Italy.
    Rodushkin, Ilia
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering. ALS Laboratory Group, ALS Scandinavia AB, Luleå, Sweden.
    Paulukat, Cora
    ALS Laboratory Group, ALS Scandinavia AB, Luleå, Sweden.
    Conti, Marcelo Enrique
    Department of Management, Sapienza University of Rome, Rome, Italy.
    Venetian Protected Designation of origin wines traceability: Multi-elemental, isotopes and chemometric analysis2023In: Food Chemistry, ISSN 0308-8146, E-ISSN 1873-7072, Vol. 404, no Part B, article id 134771Article in journal (Refereed)
    Abstract [en]

    The traceability and authentication of PDOs wines are important issues for safeguarding their production and distribution systems. This paper evaluated seven Venetian PDO wines, i.e., Amarone, Bardolino, Custoza, Pinot Grigio, Recioto, Soave and Valpolicella. For this purpose, 219 wine samples from the Veneto region were characterised by determining 63 elements and six isotope ratios by HR-ICP-MS and MC-ICP-MS. Chemometric tools highlighted As, Ca, Cs, δ11B and 87Sr/86Sr as the most informative variables to differentiate the PDOs. Seven classification methods, such as Linear Discriminant Analysis, Quadratic Discriminant Analysis, k-Nearest Neighbours, Naïve Bayes, Random Forest, Artificial Neural Networking, and Support Vector Machine were tested and perform a correct classification for Amarone, Bardolino, Pinot Grigio and Recioto PDOs. This paper successfully proposes for the first time advanced traceability tools of seven Venetian PDO by the use of an integrated approach of multi-elemental and isotopes followed by chemometrics analysis.

  • 76.
    Reynolds, Ben C.
    et al.
    IGMR, Erdwissenschaften, ETH Zürich.
    Aggarwal, Jugdeep
    Keck Isotope Laboratory, Department of Earth Sciences, University of California.
    Andre, Luc
    Department of Geology, Musée Royal de l'Afrique Centrale, Leuvensesteenweg.
    Baxter, Douglas
    Beucher, Charlotte
    Department of Ecology Evolution and Marine Biology, Marine Science Institute, University of California.
    Brzezinski, Mark A.
    Department of Ecology Evolution and Marine Biology, Marine Science Institute, University of California.
    Engström, Emma
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering.
    Georg, R. Bastian
    IGMR, Erdwissenschaften, ETH Zürich.
    Land, Magnus
    Department of Geology and Geochemistry, Laboratory for Isotope Geology, Stockholm University.
    Leng, Melanie J.
    NERC Isotope Geosciences Laboratory, British Geological Survey, Keyworth, Nottingham.
    Opfergelt, Sophie
    Department of Geology, Musée Royal de l'Afrique Centrale, Leuvensesteenweg.
    Rodushkin, Ilya
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.
    Sloane, Hilary J.
    NERC Isotope Geosciences Laboratory, British Geological Survey, Keyworth, Nottingham.
    van den Boorn, Sander H. J. M.
    Department of Earth Sciences, Utrecht University.
    Vroon, Pieter Z.
    Department of Petrology, FALW, Vrije Universiteit, De Boelelaan.
    Cardinal, Damien
    Department of Geology, Musée Royal de l'Afrique Centrale, Leuvensesteenweg.
    An inter-laboratory comparison of Si isotope reference materials2007In: Journal of Analytical Atomic Spectrometry, ISSN 0267-9477, E-ISSN 1364-5544, Vol. 22, no 5, p. 561-568Article in journal (Refereed)
    Abstract [en]

    Three Si isotope materials have been used for an inter-laboratory comparison exercise to ensure reproducibility between international laboratories investigating natural Si isotope variations using a variety of chemical preparation methods and mass spectrometric techniques. These proposed standard reference materials are (i) IRMM-018 (a SiO2 standard), (ii) Big-Batch (a fractionated SiO2 material prepared at the University of California Santa Barbara), and (iii) Diatomite (a natural diatomite sample originally deposited as marine biogenic opal). All analyses are compared with the international Si standard NBS28 (RM8546) and are in reasonable agreement (<+/- 0.22 parts per thousand. 1 sigma(SD) delta Si-30) given the different measurement techniques involved. These methods include both acid and alkaline dissolution/fusion, Si separation using cation exchange, selective co-precipitation, and gas-source versus plasma-ionization (high and low resolution) mass-spectrometric techniques. The average delta Si-30 for Diatomite, IRMM-018, and Big-Batch are + 1.26 parts per thousand, -1.65 parts per thousand and -10.48 parts per thousand, respectively, with corresponding delta Si-9 values of + 0.64 parts per thousand, -0.85 parts per thousand and -5.35 parts per thousand for the same standards, respectively. For the most fractionated standard (Big-Batch), results demonstrate a kinetic mass-dependent fractionation effect for atomic Si (i.e., delta Si-29 similar to 0.51 x delta Si-30). There is almost no statistical difference between the mean values obtained by each participating laboratory, with the notable exception of the IRMM-018 standard. This effect could be caused by heterogeneity or contamination of this standard. The results for the other two standards indicate that data sets produced using any of the methods employed in this study will have similar precision and differences are limited to 0.2 parts per thousand in mean delta Si-30 values for a given sample between laboratories, or differences of 0.13 parts per thousand. in mean delta Si-29 values.

  • 77.
    Riber, Christian
    et al.
    Environment & Resources DTU, Bygningstorvet, Building 115,Technical University of Denmark, DK 2800 Kongens Lyngby, Denmark.
    Rodushkin, Ilia
    Analytica AB, Aurorum 10, S-977 75, Luleå, Sweden.
    Spliid, Henrik
    Institute of Mathematical Modelling, Technical University of Denmark,DK 2800, Kongens Lyngby, Denmark.
    Christensen, Thomas H.
    Environment & Resources DTU, Bygningstorvet, Building 115,Technical University of Denmark, DK 2800 Kongens Lyngby, Denmark.
    Method for fractional solid-waste sampling and chemical analysis2007In: International Journal of Environmental Analytical Chemistry, ISSN 0306-7319, E-ISSN 1029-0397, Vol. 87, no 5, p. 321-335Article in journal (Refereed)
    Abstract [en]

    Chemical characterization of solid waste is a demanding task due to the heterogeneity of the waste. This article describes how 45 material fractions hand-sorted from Danish household waste were subsampled and prepared for chemical analysis of 61 substances. All material fractions were subject to repeated particle-size reduction, mixing, and mass reduction until a sufficiently small but representative sample was obtained for digestion prior to chemical analysis. The waste-fraction samples were digested according to their properties for maximum recognition of all the studied substances. By combining four subsampling methods and five digestion methods, paying attention to the heterogeneity and the material characteristics of the waste fractions, it was possible to determine 61 substances with low detection limits, reasonable variance, and high accuracy. For most of the substances of environmental concern, the waste-sample concentrations were above the detection limit (e.g. Cd > 0.001 mg kg(-1), Cr > 0.01 mg kg(-1), Hg > 0.002 mg kg(-1), Pb > 0.005 mg kg(-1)). The variance was in the range of 5-100%, depending on material fraction and substance as documented by repeated sampling of two highly different material fractions ('Vegetable food' and 'Shoes, leather, etc.'). Statistical analysis showed for the 'Vegetable food' that the variance could not be attributed to a single step in the procedure, whereas in the case of 'Shoes, leather, etc.', the first coarse shredding was the main source of variance (20-85% of the overall variation). Only by increasing the sample size significantly can this variance be reduced. The accuracy and short-term reproducibility of the chemical characterization were good, as determined by the analysis of several relevant certified reference materials. Typically, six to eight different certified reference materials representing a range of concentrations levels and matrix characteristics were included. Based on the documentation provided, the methods introduced were considered satisfactory for characterization of the chemical composition of waste-material fractions.

  • 78.
    Rodríguez, Nathalie Pérez
    et al.
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.
    Adlassnig, Wolfram
    Core Facility Cell Imaging and Ultrastructure Research, Univeristy of Vienna.
    Rodushkin, Ilya
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.
    Alakangas, Lena
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.
    Öhlander, Björn
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.
    Isotopic fractionation of Cu in biofilms from a historic mining site2013In: Mineralogical magazine, ISSN 0026-461X, E-ISSN 1471-8022, Vol. 77, no 5, p. 1950-Article in journal (Refereed)
  • 79.
    Rodríguez, Nathalie Pérez
    et al.
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.
    Engström, Emma
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.
    Rodushkin, Ilya
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.
    Nason, Peter
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.
    Alakangas, Lena
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.
    Öhlander, Björn
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.
    Copper and iron isotope fractionation in mine tailings at the Laver and Kristineberg mines, northern Sweden2013In: Applied Geochemistry, ISSN 0883-2927, E-ISSN 1872-9134, Vol. 32, p. 204-215Article in journal (Refereed)
    Abstract [en]

    Previous research has shown that Cu and Fe isotopes are fractionated by dissolution and precipitation reactions driven by changing redox conditions. In this study, Cu isotope composition (65Cu/63Cu ratios) was studied in profiles through sulfide-bearing tailings at the former Cu mine at Laver and in a pilot-scale test cell at the Kristineberg mine, both in northern Sweden. The profile at Kristineberg was also analysed for Fe isotope composition (56Fe/54Fe ratios). At both sites sulfide oxidation resulted in an enrichment of the lighter Cu isotope in the oxidised zone of the tailings compared to the original isotope ratio, probably due to preferential losses of the heavier Cu isotope into the liquid phase during oxidation of sulfides. In a zone with secondary enrichment of Cu, located just below the oxidation front at Laver, δ65Cu (compared to ERM-AE633) was as low as -4.35 ± 0.02‰, which can be compared to the original value of 1.31 ± 0.03‰ in the unoxidised tailings. Precipitation of covellite in the secondary Cu enrichment zone explains this fractionation. The Fe isotopic composition in the Kristineberg profile is similar in the oxidised zone and in the unoxidised zone, with average δ56Fe values (relative to the IRMM-014) of -0.58± 0.06‰ and -0.49 ± 0.05‰, respectively. At the well-defined oxidation front, δ56Fe was less negative, -0.24 ± 0.01 ‰. Processes such as Fe(II)-Fe(III) equilibrium and precipitation of Fe-(oxy)hydroxides at the oxidation front are assumed to cause this Fe isotope fractionation. This field study provides additional support for the importance of redox processes for the isotopic composition of Cu and Fe in natural systems.

  • 80.
    Rodríguez, Nathalie Pérez
    et al.
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.
    Sany, Seyed Mohammad Khoshkhoo
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Minerals and Metallurgical Engineering.
    Sandström, Åke
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Minerals and Metallurgical Engineering.
    Rodushkin, Ilia
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering. ALS Laboratory Group, ALS Scandinavia AB, Aurorum 10, S-977 75 Luleå, Sweden.
    Alakangas, Lena
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.
    Öhlander, Björn
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.
    Isotopic signature of Cu and Fe during bioleaching and electrochemical leaching of a chalcopyrite concentrate2015In: International Journal of Mineral Processing, ISSN 0301-7516, E-ISSN 1879-3525, Vol. 134, p. 58-65Article in journal (Refereed)
    Abstract [en]

    Bioleaching is an important process in metallurgy and in environmental sciences, either for the acquisition of metals or for the formation of acid rock drainage. In this study the implications of the processes during bioleaching of a pyritic chalcopyrite concentrate were analysed regarding its Cu and Fe isotope fractionation. The development of the redox potential during the bioleaching experiment was then simulated in an electrochemical cell in absence of microorganisms to investigate the effect of microbial activity on the Cu and Fe isotope fractionations. The leaching experiments were performed for 28 days at 45 °C with a solid content of 2.5% (w/v) at pH 1.5. It was found that Cu dissolution efficiency was similar in both experiments and the leaching curves were linear with no sign of passivation due to presence of pyrite. The heavy Cu isotope (δ65Cu) was leached more easily and as a result the leachate was enriched with the heavy Cu isotope at the beginning of both experiments and as the leaching progressed δ65Cu values in the leachate became similar to the ones of the chalcopyrite concentrate, confirming an equilibrium fractionation happening in a closed system. There was no distinct difference in the Cu and Fe isotope fractionations in absence and presence of microorganisms. Finally based on Cu and Fe isotope signatures, a simplified method is suggested for the estimation of the leaching extent during the oxidisation of sulphide materials in natural systems.

  • 81.
    Rodushkin, Ilia
    et al.
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.
    Axelsson, Mikael D.
    SGAB Analytica.
    Application of double focusing sector field ICP-MS for multielemental characterization of human hair and nails: Part I: Analytical methodology2000In: Science of the Total Environment, ISSN 0048-9697, E-ISSN 1879-1026, Vol. 250, no 1-3, p. 83-100Article in journal (Refereed)
    Abstract [en]

    The capabilities of double focusing sector field inductively coupled plasma mass spectrometry (ICP-SMS) for the determination of 71 elements in hair and nails were studied. A microwave-assisted digestion procedure with nitric acid and hydrogen peroxide as well as direct sampling of the nails by laser ablation (LA) have been tested. Examples of spectral interferences are given and different correction procedures are discussed. Method detection limits below ng g-1 were obtained for 39 elements investigated by using high-purity reagents and by taking special care to prevent contamination during preparation. However, these detection limits were insufficient for detection of some platinum group elements in the majority of the samples. The accuracy of the analytical procedure was estimated by analysis of the GBW07601 certified reference material as well as by participation in an interlaboratory comparison program. The reproducibility was assessed from replicate analysis (including sample preparation) and was found to be, as average values for all elements, 9-10% R.S.D. and 18-19% R.S.D. for hair and nails, respectively. Contribution from exogenous deposition was evaluated by analyzing samples before and after washing, as well as by studying spatial element distribution along hair and nails. It was found that even after sample washing, many elements are enriched in the surface of the nail.

  • 82.
    Rodushkin, Ilia
    et al.
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.
    Axelsson, Mikael D.
    SGAB Analytica.
    Application of double focusing sector field ICP-MS for multielemental characterization of human hair and nails: Part II: A study of the inhabitants of northern Sweden2000In: Science of the Total Environment, ISSN 0048-9697, E-ISSN 1879-1026, Vol. 262, no 1-2, p. 21-36Article in journal (Refereed)
    Abstract [en]

    Double-focusing sector-field, inductively coupled plasma-mass spectrometry was used for the determination of 71 elements in scalp hair and fingernail samples from an urban population group living in the north-east of Sweden. Samples (n=114 for hair and n=96 for nails) were taken from subjects without known occupational exposure to metals. From these results, concentration ranges were calculated and compared with published intervals. Statistical analysis was used to elucidate differences according to sex, age and smoking habit. It was found that significant correlations exist between different elements in hair and nails, as well as between hair and nail concentrations for several elements. Strong positive correlation for Hg, Cd, Pb, Sb and Bi levels between these media confirms that both can be used for exposure assessment for these elements. Several examples on the use of distribution patterns for the rare-earth elements (REE) and of Pb isotope ratios for assessment of exposure are given.

  • 83.
    Rodushkin, Ilia
    et al.
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.
    Axelsson, Mikael D.
    SGAB Analytica.
    Application of double focusing sector field ICP-MS for multielemental characterization of human hair and nails: Part III: Direct analysis by laser ablation2003In: Science of the Total Environment, ISSN 0048-9697, E-ISSN 1879-1026, Vol. 305, no 1-3, p. 23-39Article in journal (Refereed)
    Abstract [en]

    The capabilities of laser ablation double focusing sector field inductively coupled plasma mass spectrometry for the determination of 55 elements in nails and hair were studied. Quantification was performed by external calibration using in-house matrix-matched standards in tablet form following correction for variations in ablation efficiency by internal standardization using a matrix element (S). For nails, intra-individual long- and short-term chronological variations as well as depth distribution patterns were studied. For the majority of elements tested, significant enrichment was found in the surface of the nail. Element distributions along a hair strand were investigated with a spatial resolution of 2.5 mm.

  • 84.
    Rodushkin, Ilia
    et al.
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering. ALS Laboratory Group, ALS Scandinavia AB, Luleå, Sweden.
    Engström, Emma
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering. ALS Laboratory Group, ALS Scandinavia AB, Luleå, Sweden.
    Pontér, Simon
    SKB, Svensk Kärnbränslehantering AB, Stockholm, Sweden.
    Pennisi, Maddalena
    Istituto di Geoscienze e Georisorse, CNR, Pisa, Italy.
    Elemental stable isotope assessment of groundwater contamination: Recent developments2022In: Current Opinion in Environmental Science & Health, ISSN 2468-5844, Vol. 26, article id 100330Article, review/survey (Refereed)
    Abstract [en]

    Anthropogenic contamination of water resources remains a severe environmental concern on a global scale. Radiogenic and stable isotope measurements (especially for light elements) constitute well-known tools for the identification of pollution sources and thus have considerable potential in prevention and remediation efforts. Recent instrumental and methodological advances have extended the isotope ‘toolbox’ to include a significant number of new stable isotope systems, which in turn resulted in rapid growth of studies using these novel tracers in the field of environmental forensics. Isotopic fractionation, occurring during post-release transformation of contaminants, offers an additional benefit of possibility to study the fate of pollutants in aquatic systems. This review will focus on selected relevant studies in the field and present future trends and development.

  • 85.
    Rodushkin, Ilia
    et al.
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.
    Nordlund, Peter
    Analytica AB.
    Engström, Emma
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.
    Baxter, Douglas
    Improved multi-elemental analyses by inductively coupled plasma-sector field mass spectrometry through methane addition to the plasmat2005In: Journal of Analytical Atomic Spectrometry, ISSN 0267-9477, E-ISSN 1364-5544, Vol. 20, no 11, p. 1250-1255Article in journal (Refereed)
    Abstract [en]

    Changes in the analytical performance of double focusing sector field inductively coupled plasma mass spectrometry (ICP-SFMS) caused by addition of methane to the argon gas ICP were studied for approximately 100 isotopes of 70 elements. The parameters under consideration included instrumental background, analyte sensitivity, precision and formation of spectral interferences as functions of methane flow added to the sample gas. It was shown that for many analytes the capabilities of ICP-SFMS significantly improve by virtue of enhanced sensitivity and reduction of polyatomic interferences. In contrast to quadrupole-based ICP-MS, these gains in instrumental performance do not compromise multi-element capabilities given that the amount of methane is carefully optimized. The accuracy of the results for the determination of 50 elements in water samples was evaluated using the certified reference materials SLRS-4 and SLEW-2.

  • 86.
    Rodushkin, Ilia
    et al.
    ALS Scandinavia AB.
    Pallavicini, Nicola
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.
    Engström, Emma
    ALS Scandinavia AB.
    Sörlin, Dieke
    ALS Scandinavia AB.
    Öhlander, Björn
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.
    Ingri, Johan
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.
    Baxter, Douglas C.
    ALS Scandinavia AB.
    Assessment of the natural variability of B, Cd, Cu, Fe, Pb, Sr, Tl and Zn concentrations and isotopic compositions in leaves, needles and mushrooms using single sample digestion and two-column matrix separation2016In: Journal of Analytical Atomic Spectrometry, ISSN 0267-9477, E-ISSN 1364-5544, Vol. 31, no 1, p. 220-233Article in journal (Refereed)
    Abstract [en]

    An analytical procedure allowing multi-elemental analyses and isotope ratio measurements of eight of these (B, Cd, Cu, Fe, Pb, Sr, Tl and Zn) in matrices relevant for bio-monitoring using a single highpressure acid digestion was developed. Method blanks, separation efficiency of matrix elements, repeatability and reproducibility were evaluated using sets of preparation blanks, certified reference materials and duplicate samples prepared and analyzed over a period of several months. The method was used to assess the natural variability of concentrations and isotopic compositions in bio-indicators (tree leaves, needles and mushrooms, over 240 samples) collected mainly from a confined area in North-East Sweden. Ranges found from leaves and needles were compared with data obtained for limited numbers of samples collected in Spain, Italy, France, United Kingdom and Iceland.

  • 87.
    Rodushkin, Ilia
    et al.
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.
    Stenberg, Anna
    Andren, Henrik
    Malinovskiy, Dmitry
    Baxter, Douglas
    Isotopic fractionation during diffusion of transition metal ions in solution2004In: Analytical Chemistry, ISSN 0003-2700, E-ISSN 1520-6882, Vol. 76, no 7, p. 2148-2151Article in journal (Refereed)
    Abstract [en]

    Isotope ratios and elemental concentrations were measured in aqueous solutions sampled at varying distances from sources of Fe or Zn ions. The measurements reveal fractionation of isotopes resulting from pure diffusion in solution. Our data demonstrate that diffusion alone can cause changes in 56Fe/54Fe and 66Zn/64Zn isotope ratios in excess of -0.3”. These findings thus confirm previous suspicions that transport processes contribute to observed variations in isotopic compositions. Diffusion must therefore be considered when attempting to make inferences from isotope measurements on samples originating from aqueous systems where concentration gradients may develop.

  • 88.
    Rodushkin, Ilia
    et al.
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.
    Ödman, Fredrik
    SGAB Analytica.
    Application of inductively coupled plasma sector field mass spectrometry for elemental analysis of urine2001In: Journal of Trace Elements in Medicine and Biology, ISSN 0946-672X, E-ISSN 1878-3252, Vol. 14, no 4, p. 241-247Article in journal (Refereed)
    Abstract [en]

    An analytical method using double focusing sector field inductively - coupled plasma mass spectrometry (sector field ICPMS) for rapid simultaneous determination of 42 elements in urine is described. Sample preparation consisted of 20-fold dilution with 0.14 mol/l nitric acid in ultrapure water. The importance of controlling possible contamination sources at different sample preparation and analysis stages in order to achieve adequate method detection limits (DL) is emphasized. Correction for matrix effects was made using indium and lutetium as internal standards. Different approaches for accuracy assessment in urine analysis are evaluated. Additional information on trace element concentrations in a urine reference material is given. Between-batch precision was assessed from the analysis of separately prepared aliquots of the reference material and was better than 10% RSD for 32 of the elements. The robustness of the procedure was tested by analysis of about 250 samples in one analytical run lasting more than 50 hours. A statistical summary of results for 19 urine samples from non-exposed subjects is presented. For a majority of the elements tested concentrations were higher than the detection limit of the method.

  • 89.
    Rodushkin, Ilia
    et al.
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering. SGAB Analytica, Luleå, Sweden.
    Ödman, Fredrik
    Luleå University of Technology. SGAB Analytica, Luleå, Sweden.
    Appelblad, Petra K.
    Luleå University of Technology.
    Multielement determination and lead isotope ratio measurement in alcoholic beverages by high-resolution inductively coupled plasma mass spectrometry1999In: Journal of Food Composition and Analysis, ISSN 0889-1575, E-ISSN 1096-0481, Vol. 12, no 4, p. 243-257Article in journal (Refereed)
    Abstract [en]

    The analytical performance of inductively coupled plasma mass spectrometry (ICP-MS) for the inorganic analysis of alcoholic beverages was evaluated using double-focusing sector field ICP-MS (ICP-SMS). No sample pre-treatment other than acidification and dilution was carried out. Though aspiration of ethanol-containing solutions into the ICP caused significant matrix effects, accurate results could be obtained by using matrix-matched blanks and standards. Method detection limits reach the fg mL-1range for elements with high m/z ratios which makes the technique especially useful for determination of such low-abundant elements as REE, actinide elements, etc., in this sample type. Between-run reproducibility better than 10% RSD was found for the majority of the elements even at ultra-trace concentrations. The precision in lead isotope ratio measurements is superior to that obtained with quadrupole systems (ICP-QMS) and an uncertainty of about 0.06% RSD can be routinely obtained. Measured ratios for wines of European origin are in good agreement with previously published results obtained by thermal ionization mass spectrometry (TIMS). The robustness of the analytical procedure was tested by analysis of a wide range of alcoholic beverages from the Swedish market. Average elemental concentrations found in wines, whiskies and spiced strong aperitifs are also given.

  • 90.
    Rodushkin, Ilia
    et al.
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering. Svensk Grundämnesanalys AB, Luleå, Sweden.
    Ödman, Fredrik
    Luleå University of Technology. Svensk Grundämnesanalys AB, Luleå, Sweden.
    Branth, Stefan
    Department of Medical Sciences, Nutrition, Uppsala University, Uppsala, Sweden.
    Multielement analysis of whole blood by high resolution inductively coupled plasma mass spectrometry1999In: Fresenius' Journal of Analytical Chemistry, ISSN 0937-0633, E-ISSN 1432-1130, Vol. 364, no 4, p. 338-346Article in journal (Refereed)
    Abstract [en]

    An analytical method using double focusing sector field inductively coupled plasma mass spectrometry (ICP-SMS) for rapid simultaneous determination of 50 elements in digested human blood is described. Sample preparation consisted of microwave digestion with nitric acid followed by dilution with ultrapure water. The importance of controlling possible contamination sources at different sample preparation and analysis stages in order to achieve adequate method detection limits (MDL) is emphasised. Correction for matrix effects was made using scandium, indium and lutecium as internal standards. Accuracy of the data for elements suffering from spectral interferences was improved by applying either a high resolution capability of the ICP-SMS or mathematical corrections. Different approaches for accuracy assessment in blood analysis are evaluated. Additional information on trace elements concentration in selected blood reference materials is given. The between-batch precision was assessed from replicate analysis (including sample preparation) of reference materials and was better than 10% RSD for 21 elements and better than 30% RSD for 36 elements under consideration. A statistical summary for results obtained for 31 blood samples from non-exposed subjects is presented. The majority of elements tested was found in the samples at concentrations higher than MDL.

  • 91.
    Rodushkin, Ilia
    et al.
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering. SGAB Analytica, Luleå, Sweden.
    Ödman, Fredrik
    Luleå University of Technology. SGAB Analytica, Luleå, Sweden.
    Holmström, Henning
    Luleå University of Technology.
    Multi-element analysis of wild berries from northern Sweden by ICP techniques1999In: Science of the Total Environment, ISSN 0048-9697, E-ISSN 1879-1026, Vol. 231, no 1, p. 53-65Article in journal (Refereed)
    Abstract [en]

    In this study, the abundances of 60 chemical elements were determined in berries of blueberry (Vaccinium myrtillus) and lingonberry (Vaccinium vitis-idaea) by a combination of inductively coupled plasma atomic emission spectrometry (ICP-AES) and inductively coupled plasma double focusing sector field mass spectrometry (ICP-SMS). Samples of both species were collected at 35 sites in northern Sweden. The sites are related to four zones representing areas affected by different types of human activity as well as an adjacent reference area. Special care was taken to keep sample contamination during sampling and sample preparation as low as possible. Different approaches such as use of an internal quality control sample, spike recovery tests and comparison between different analytical techniques, were used to ensure the quality of the results. Variations in element concentrations within individual sampling sites were estimated, based upon in-site duplicate sampling and analysis. The contribution from surface contamination to total berry concentrations was assessed by analysis of samples before and after rinsing with water. A comparison of the two species showed that, in spite of very similar concentrations for the majority of the elements, the highest Tl, Sr and Ba values were found in lingonberry while the highest Cl and Re concentrations were found in blueberry. The highest total concentrations of Ag, As, Be, Bi, Br, Cd, Hg, I, Ni, Pb, Sb and Tl were found in berries from mining areas, whereas those of Li, V, Hf, W, Ta and REE were found in the vicinity of high-traffic roads.

  • 92.
    Rodushkin, Ilya
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.
    Capabilities of high resolution inductively coupled plasma mass spectrometry for trace element determination in plant sample digests1998In: Fresenius' Journal of Analytical Chemistry, ISSN 0937-0633, E-ISSN 1432-1130, Vol. 362, no 6, p. 541-546Article in journal (Refereed)
    Abstract [en]

    The analytical performance of inductively coupled plasma mass spectrometry (ICP-MS) for the analysis of plant sample digests was evaluated using double focusing sector field ICP-MS (ICP-SMS). Instrumental detection limits of ICP-SMS are superior to those obtained by quadrupole systems (ICP-QMS) and reach the fg mL-1 range for elements with high m/z ratios. Matrix effects caused by a plant digest after sample preparation resulting in 200-fold dilution were found to be negligible. The usefulness of high mass resolution for overcoming some spectral interferences is demonstrated. Mathematical correction possibilities could be necessary to improve accuracy. The concentrations of more than 20 elements can be determined in 5 min and only one internal standard is necessary to correct for instrumental drift.

  • 93.
    Rodushkin, Ilya
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.
    Isotope ratio measurements using sector-field ICP-MS2006In: 3rd Nordic conference on plasma spectrochemistry: plasma spectrochemical abstracts, Amherst, Mass: ICP Information Newsletter, Inc , 2006Conference paper (Other academic)
    Abstract [en]

    Isotope ratio measurements are required for a variety of applications: accurate quantification of element concentrations using isotope dilution; tracer experiments using enriched isotope spikes in environmental, biological or medical sciences; determination of isotope abundances of radiogenic elements and their products in the nuclear industry, in environmental studies (e.g. for tracing pollution sources) and for geological age determination (dating); investigations of isotope variations of stable isotopes in nature. During the last two decades, inductively coupled plasma mass spectrometry (ICP-MS) has been increasingly used for such applications, becoming a significant complement to thermal ionization mass spectrometry (TIMS). The short course will be focused on accurate and precise isotope ratio measurements using double-focusing sector field ICP-MS (ICP-SFMS). Equipped with a single ion collector, this technique provides short-term precision in the 0.02%-0.1% RSD range at best. Developed a decade ago, multi-collector ICP-MS (MC-ICP-MS) allows significant improvements in precision down to a few ppm. However, high precision does not always guarantee high accuracy. In order to obtain true isotope ratios, measured ratios have to be corrected for all possible spectral interferences on analyte masses; for detector ‘dead time' (for detectors operated in ion-counting mode) and ‘sag' of electronic circuits; for mass bias; for possible blank contribution. Different approaches for performing such corrections will be discussed. The accuracy of isotope ratios measured by single collector ICP-SFMS in a variety of samples will be illustrated using results from several international performance evaluation exercises.

  • 94.
    Rodushkin, Ilya
    et al.
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering. SGAB Analytica, Luleå, Sweden.
    Axelsson, Mikael D.
    Luleå University of Technology.
    Burman, Erik
    Luleå University of Technology. SGAB Analytica, Luleå Sweden.
    Multielement analysis of coal by ICP techniques using solution nebulization and laser ablation2000In: Talanta: The International Journal of Pure and Applied Analytical Chemistry, ISSN 0039-9140, E-ISSN 1873-3573, Vol. 51, no 4, p. 743-759Article in journal (Refereed)
    Abstract [en]

    The combination of inductively coupled plasma atomic emission spectrometry and high resolution inductively coupled plasma mass spectrometry for the determination of 70 elements in coal were studied. Four microwave-assisted digestion procedures with different dissolution mixtures (nitric and hydrofluoric acids, aqua regia and hydrogen peroxide), lithium metaborate fusion with and without previous sample ashing as well as direct sampling by laser ablation (LA) have been tested. Examples of spectral interferences are given and different correction procedures are discussed. Detection limits in the low ng g-1 range were obtained for most of the elements investigated by using high-purity reagents and by taking special care to prevent sample contamination during preparation. The precision was assessed from replicate analysis (including sample preparation) of coal samples and was found to be, as average values far all elements, 4-5% RSD and 10-15% RSD for procedures including sample digestion and LA sampling, respectively. The accuracy of the overall analytical procedures was estimated by analysis of certified reference materials and of a coal sample obtained from the Interlab Trace round robin test. Among the dissolution mixtures tested, the combination of nitric and hydrofluoric acids with hydrogen peroxide provide the best agreement with certified, recommended, literature-compiled or consensus values, though fusion is necessary to obtain quantitative recoveries for Si, Cr, Hf, W, Zr, Y. In general, results obtained by LA fall within ±20% of those obtained after digestion.

  • 95.
    Rodushkin, Ilya
    et al.
    Analytica AB, Luleå, Sweden.
    Axelsson, Mikael D.
    Luleå University of Technology.
    Malinovskiy, Dmitry
    Luleå University of Technology.
    Baxter, Douglas C.
    Luleå University of Technology.
    Analyte- and matrix-dependent elemental response variations in laser ablation inductively coupled plasma mass spectrometry: Part 1. The roles of plasma and ion sampling conditions2002In: Journal of Analytical Atomic Spectrometry, ISSN 0267-9477, E-ISSN 1364-5544, Vol. 17, no 10, p. 1223-1230Article in journal (Refereed)
    Abstract [en]

    Elemental response variations as a function of carrier gas flow rate in laser ablation inductively coupled plasma mass spectrometry (LA-ICP-MS) were studied for a wide range of analytes. The effects of rf power, focus lens settings, thermodynamic properties of analytes and sample matrix were thoroughly examined. It was found that, with the experimental set-up used for this work, processes occurring in the ICP, rather than during ablation and transport, play the decisive role in determining the shapes of flow rate plots observed with LA. Responses for analytes of lower nominal masses and vaporization enthalpies peak at consistently higher flow rates (1.15 1 min-1) than other elements, independent of matrix. On the other hand, the magnitude of the maximum sensitivity is matrix dependent, even for these elements. Involatile elements display much broader maxima at considerably lower flow rates; the more refractory the matrix, the lower the optimum flow rate. This behaviour is consistent with the residence time in the ICP necessary to maximize the efficiency of analyte ion production. The existence of inter-elemental differences in the locations of zones of maximum ion densities formed in the ICP can thus be related to the times required for vaporization of any given analyte from the particles produced by LA. Such differences may be responsible for numerous fractionation effects mentioned in the LA literature. It is also demonstrated that the ion sampling process can affect the shapes of the flow rate plots, potentially shifting the apparent position of the optimum flow rate and confounding the interpretation of inter-element response differences.

  • 96.
    Rodushkin, Ilya
    et al.
    Analytica AB, Luleå, Sweden.
    Axelsson, Mikael D.
    Luleå University of Technology.
    Malinovskiy, Dmitry
    Luleå University of Technology.
    Baxter, Douglas C.
    Luleå University of Technology.
    Analyte- and matrix-dependent elemental response variations in laser ablation inductively coupled plasma mass spectrometry: Part 2. Implications for multi-element analyses2002In: Journal of Analytical Atomic Spectrometry, ISSN 0267-9477, E-ISSN 1364-5544, Vol. 17, no 10, p. 1231-1239Article in journal (Refereed)
    Abstract [en]

    Given that laser ablation inductively coupled plasma mass spectrometry (LA-ICP-MS) has the potential to directly determine the concentrations of some 80 elements in solid samples, the fact that most applications are limited to considerably smaller numbers of analytes is indicative of the inherent problems with calibration. These stem from elemental response variations, both between analytes in any given sample and between matrices for any given analyte. Although response variations are often attributed to differences in ablation or transport efficiencies, there have also been indications that some degree of elemental fractionation may occur in the ICP. The results of the present investigations demonstrate that the ICP is the predominant source of fractionation, and thus response variations are related to the thermodynamic properties of the elements and their host particles. By studying analyte response as a function of carrier gas flow rate (so called flow rate plots) in 16 matrices, patterns in the behaviour of the elements in LA-ICP-MS could be clearly discerned and used for classification. Three groups of elements displaying consistent behavioural patterns over all matrices were identified from these studies: Group A, comprising refractory elements with high oxide bond dissociation enthalpies; Group B, including the rare and heavier alkaline earth (Ca, Sr, Ba) elements; and Group C, consisting of volatile or low mass elements. As each group exhibits decidedly different optimum flow rates and flow rate plot shapes which, with the exception of the group C elements, also depend on the matrix, the utility of LA-ICP-MS for multi-element analyses is severely compromised. In fact, quantitative determination of a wide range of analytes demands that calibration factors be established for at least one element from each group, as well as for all elements that could not be satisfactorily classified. This classification may serve as a guide in the selection of suitable internal standards for LA-ICP-MS, at least for certain groups of analytes. Examples are also given showing how flow rate plots can be employed to predict the adequacy of selected internal standards or solid standard materials for calibration

  • 97.
    Rodushkin, Ilya
    et al.
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.
    Baxter, Douglas
    Engström, Emma
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.
    Inorganic constituents of nuts and seeds2011In: Nuts and Seeds in Health and Disease Prevention, Elsevier, 2011, p. 65-72Chapter in book (Refereed)
    Abstract [en]

    This chapter presents data on the inorganic components of hazelnuts, walnuts, almonds, pecans, cashews, Brazil nuts, pistachios, pine nuts, peanuts, coconuts, pumpkin seeds, and sunflower seeds. Based on average consumption data for nuts and seeds, their nutritional significance and toxicological relevance in dietary intake are discussed.

  • 98.
    Rodushkin, Ilya
    et al.
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.
    Baxter, Douglas
    ALS Scandinavia AB.
    Engström, Emma
    Hoogewerff, J.
    Centre for Forensic Provenancing, School of Chemistry University of East Anglia, Norwich.
    Horn, P.
    München University.
    Papesch, W.
    Austrian Research Center Seibersdorf (ARCS).
    Watling, J.
    Centre for Forensic Science, University of Western Australia, Perth.
    Latkoczy, C.
    Swiss Federal Institute of Technology (ETH).
    van der Peijl, G.
    Netherlands Forensic Institute, The Hague.
    Berends-Montero, S.
    Netherlands Forensic Institute, The Hague.
    Ehleringer, J.
    University of Utah, Biology Department.
    Zdanowicz, V.
    Bureau of Customs and Border Protection, 7501 Boston Boulevard, Springfield.
    Elemental and isotopic characterization of cane and beet sugars2011In: Journal of Food Composition and Analysis, ISSN 0889-1575, E-ISSN 1096-0481, Vol. 24, no 1, p. 70-78Article in journal (Refereed)
    Abstract [en]

    An interlaboratory program designed to assess the feasibility of using multi-element and isotopic measurements for determining the geographic origin of sugars permitted an intercomparison of the performance (in terms of limits of detection, reproducibility and bias) of various analytical techniques: inductively coupled plasma (ICP)-optical emission spectrometry (OES); different variations of ICP-mass spectrometry (MS): quadrupole (QMS), sector-field (SFMS) and multi-collector (MC-ICP-MS); thermal ionization MS (TIMS); and isotope ratio MS (IRMS). These various methods were applied to cane (raw and refined) and beet (refined) sugars from different origins. Concentrations of 63 elements and isotope ratios of Pb, Sr and C in sugar samples are reported. Determining the geographic origin of sugars appears feasible using elemental fingerprinting

  • 99.
    Rodushkin, Ilya
    et al.
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.
    Bergman, T.
    BD Fisk AB, Luleå.
    Douglas, G.
    Kalix kommun, Kalix.
    Engström, Emma
    Sörlin, D.
    ALS Analytica AB, Luleå.
    Baxter, Douglas
    Authentication of Kalix (NE Sweden) vendace caviar using inductively coupled plasma-based analytical techniques: evaluation of different approaches2007In: Analytica Chimica Acta, ISSN 0003-2670, E-ISSN 1873-4324, Vol. 583, no 2, p. 310-318Article in journal (Refereed)
    Abstract [en]

    Different analytical approaches for origin differentiation between vendace and whitefish caviars from brackish- and freshwaters were tested using inductively coupled plasma double focusing sector field mass spectrometry (ICP-SFMS) and multi-collector inductively coupled plasma mass spectrometry (MC-ICP-MS). These approaches involve identifying differences in elemental concentrations or sample-specific isotopic composition (Sr and Os) variations. Concentrations of 72 elements were determined by ICP-SFMS following microwave-assisted digestion in vendace and whitefish caviar samples from Sweden (from both brackish and freshwater), Finland and USA, as well as in unprocessed vendace roe and salt used in caviar production. This data set allows identification of elements whose contents in caviar can be affected by salt addition as well as by contamination during production and packaging. Long-term method reproducibility was assessed for all analytes based on replicate caviar preparations/analyses and variations in element concentrations in caviar from different harvests were evaluated. The greatest utility for differentiation was demonstrated for elements with varying concentrations between brackish and freshwaters (e.g. As, Br, Sr). Elemental ratios, specifically Sr/Ca, Sr/Mg and Sr/Ba, are especially useful for authentication of vendace caviar processed from brackish water roe, due to the significant differences between caviar from different sources, limited between-harvest variations and relatively high concentrations in samples, allowing precise determination by modern analytical instrumentation. Variations in the 87Sr/86Sr ratio for vendace caviar from different harvests (on the order of 0.05-0.1%) is at least 10-fold less than differences between caviar processed from brackish and freshwater roe. Hence, Sr isotope ratio measurements (either by ICP-SFMS or by MC-ICP-MS) have great potential for origin differentiation. On the contrary, it was impossible to differentiate between Swedish caviar processed from brackish water roe and Finnish freshwater caviar based solely on 187Os/188Os ratios.

  • 100.
    Rodushkin, Ilya
    et al.
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.
    Engström, Emma
    Luleå University of Technology, Department of Civil, Environmental and Natural Resources Engineering, Geosciences and Environmental Engineering.
    Baxter, D.C.
    ALS Scandinavia AB.
    Isotopic analyses by ICP-MS in clinical samples2013In: Analytical and Bioanalytical Chemistry, ISSN 1618-2642, E-ISSN 1618-2650, Vol. 405, no 9, p. 2785-2797Article in journal (Refereed)
    Abstract [en]

    This critical review focuses on inductively coupled plasma mass spectrometry (ICP-MS) based applications for isotope abundance ratio measurements in various clinical samples relevant to monitoring occupational or environmental exposure, human provenancing and reconstruction of migration pathways as well as metabolic research. It starts with a brief overview of recent advances in ICP-MS instrumentation, followed by selected examples that cover the fields of accurate analyte quantification using isotope dilution, tracer studies in nutrition and toxicology, and areas relying upon natural or man-made variations in isotope abundance ratios (Pb, Sr, actinides and stable heavy elements). Finally, some suggestions on future developments in the field are provided

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