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Karimi, S., Mortazavi, Y., Khodadadi, A. A., Holmgren, A., Korelskiy, D. & Hedlund, J. (2020). Functionalization of silica membranes for CO2 separation. Separation and Purification Technology, 235, Article ID 116207.
Open this publication in new window or tab >>Functionalization of silica membranes for CO2 separation
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2020 (English)In: Separation and Purification Technology, ISSN 1383-5866, E-ISSN 1873-3794, Vol. 235, article id 116207Article in journal (Refereed) Published
Abstract [en]

Five organic CO2-philic functional groups were incorporated in silica matrixes for preparation of functionalized silica membranes to explore the CO2 separation performance. Chemical groups including acetate, trifluoromethyl, methacrylate, urea and vinyl groups were anchored in the silica network using the co-condensation method.

The information from 29Si solid-state NMR and FTIR analyses indicates the successful formation of a covalent bond between functional groups and the silica network. The thickness of the functionalized silica layers was measured by SEM and the thermal stability of the organic groups was determined by thermogravimetric analysis (TGA).

The gas permeance and mixed gas selectivity of CO2/N2 was measured in the temperature range of 253–373 K with a feed pressure of 9 bar. A maximum selectivity of as high as 10 was observed for a trifluoromethyl functionalized silica membrane with a CO2 permeance of 5.5 × 10−7 mol s−1 m−2 Pa−1. Permporometry measurements indicated that the contribution of flow through micropores to the total flow for all the functionalized silica membranes varied between 62 and 82%. All membranes were CO2 selective.

 

Place, publisher, year, edition, pages
Elsevier, 2020
Keywords
CO2 separation, Functionalized silica membrane, Co-condensation
National Category
Chemical Process Engineering
Research subject
Chemical Technology
Identifiers
urn:nbn:se:ltu:diva-76487 (URN)10.1016/j.seppur.2019.116207 (DOI)2-s2.0-85073520358 (Scopus ID)
Note

Validerad;2019;Nivå 2;2019-10-23 (johcin)

Available from: 2019-10-23 Created: 2019-10-23 Last updated: 2019-10-29Bibliographically approved
Yu, L., Holmgren, A. & Hedlund, J. (2019). A novel method for fabrication of high-flux zeolite membranes on supports with arbitrary geometry. Journal of Materials Chemistry A, 7(17), 10325-10330
Open this publication in new window or tab >>A novel method for fabrication of high-flux zeolite membranes on supports with arbitrary geometry
2019 (English)In: Journal of Materials Chemistry A, ISSN 2050-7488, Vol. 7, no 17, p. 10325-10330Article in journal (Refereed) Published
Abstract [en]

A novel procedure for the preparation of high-flux zeolite membranes was developed. This method relies on rendering the support hydrophobic, and thereby protected from the synthesis mixture and invasion of the support pores, while the cationic polymer on the surface still allowed deposition of zeolite seeds. Both high-flux MFI and CHA zeolite films were grown on both discs and tubular supports, which illustrates the applicability of the method to arbitrary membrane geometries. Typically, MFI disc membranes showed a very high CO2permeance of 85 × 10−7 mol m−2 s−1 Pa−1 and a CO2/H2 separation selectivity of 56 at 278 K and CHA disc membranes showed a very high CO2 permeance of 79 × 10−7 mol m−2 s−1 Pa−1 and a CO2/CH4 separation selectivity of 76 at 249 K. As the method is applicable to supports with complex geometries, it is suitable for preparation of membranes for industrial applications.

Place, publisher, year, edition, pages
Royal Society of Chemistry, 2019
National Category
Chemical Process Engineering
Research subject
Chemical Technology
Identifiers
urn:nbn:se:ltu:diva-73583 (URN)10.1039/C9TA00789J (DOI)000472183200016 ()2-s2.0-85064990509 (Scopus ID)
Note

Validerad;2019;Nivå 2;2019-06-24 (johcin)

Available from: 2019-04-11 Created: 2019-04-11 Last updated: 2019-07-10Bibliographically approved
Faisal, A., Holmlund, M., Ginesy, M., Holmgren, A., Enman, J., Hedlund, J. & Grahn, M. (2019). Recovery of l-Arginine from Model Solutions and Fermentation Broth Using Zeolite-Y Adsorbent. ACS Sustainable Chemistry & Engineering, 7(9), 8900-8907
Open this publication in new window or tab >>Recovery of l-Arginine from Model Solutions and Fermentation Broth Using Zeolite-Y Adsorbent
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2019 (English)In: ACS Sustainable Chemistry & Engineering, ISSN 2168-0485, Vol. 7, no 9, p. 8900-8907Article in journal (Refereed) Published
Abstract [en]

Arginine was produced via fermentation of sugars using the engineered microorganism Escherichia coli. Zeolite-Y adsorbents in the form of powder and extrudates were used to recover arginine from both a real fermentation broth and aqueous model solutions. An adsorption isotherm was determined using model solutions and zeolite-Y powder. The saturation loading was determined to be 0.2 g/g using the Sips model. Arginine adsorbed from a real fermentation broth using either zeolite-Y powder or extrudates both showed a maximum loading of 0.15 g/g at pH 11. This adsorbed loading is very close to the corresponding value obtained from the model solution showing that under the experimental conditions the presence of additional components in the broth did not have a significant effect on the adsorption of arginine. Furthermore, a breakthrough curve was determined for extrudates using a 1 wt % arginine model solution. The selectivity for arginine over ammonia and alanine from the real fermentation broth at pH 11 was 1.9 and 8.3, respectively, for powder, and 1.0, and 4.1, respectively, for extrudates. To the best of our knowledge, this is the first time recovery of arginine from real fermentation broths using any type of adsorbent has been reported.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2019
Keywords
Arginine, FAU, Fermentation broth, Escherichia coli, Adsorption, Selectivity, Breakthrough
National Category
Chemical Process Engineering Bioprocess Technology
Research subject
Chemical Technology; Biochemical Process Engineering
Identifiers
urn:nbn:se:ltu:diva-73954 (URN)10.1021/acssuschemeng.9b00918 (DOI)000467351200095 ()2-s2.0-85065476739 (Scopus ID)
Note

Validerad;2019;Nivå 2;2019-05-27 (oliekm)

Available from: 2019-05-15 Created: 2019-05-15 Last updated: 2019-08-19Bibliographically approved
Shah, F. U., Holmgren, A., Rutland, M. W., Glavatskih, S. & Antzutkin, O. (2018). Interfacial Behavior of Orthoborate Ionic Liquids at Inorganic Oxide Surfaces Probed by NMR, IR and Raman Spectroscopy. The Journal of Physical Chemistry C, 122(34), 19687-19698
Open this publication in new window or tab >>Interfacial Behavior of Orthoborate Ionic Liquids at Inorganic Oxide Surfaces Probed by NMR, IR and Raman Spectroscopy
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2018 (English)In: The Journal of Physical Chemistry C, ISSN 1932-7447, E-ISSN 1932-7455, Vol. 122, no 34, p. 19687-19698Article in journal (Refereed) Published
Abstract [en]

Absorption modes and reactivity of non-halogenated ionic liquids (ILs) at inorganic oxide surfaces of γ-Al2O3, MgO and SiO2 particles were characterized using multinuclear (11B, 31P and 29Si) solid-state magic-angle-spinning NMR, FTIR and Raman spectroscopy. ILs are composed of the trihexyl(tetradecyl)phosphonium cation, [P6,6,6,14]+, and bis(mandelato)borate, [BMB]-, or bis(salicylato)borate, [BScB]-, anions. Spectroscopic measurements were performed on room temperature (298 K) samples and samples exposed to 15 hours of heating at 373 K. The single pulse 11B NMR data of heated [P6,6,6,14][BMB] mixed with the inorganic oxides showed a significant change in spectra of the anion for all three oxides. In contrast, no such spectral changes were detected for heated [P6,6,6,14][BScB] mixed with the inorganic oxides. 31P MAS NMR data for the IL/metal oxide systems revealed interactions between [P6,6,6,14]+ and the surfaces of oxides. A significant intensity of 31P CP-MAS NMR signals indicated a low mobility of cations in these systems. The existence of strongly adhered surface layers of ILs on SiO2 particles was also confirmed by 1H-29Si CP-MAS NMR spectroscopy. FTIR and Raman spectroscopic data revealed strong interactions between the anions and the inorganic surfaces and there is strong correlation with the data obtained from NMR spectroscopy. Although their chemical structures are rather similar, the [BScB]- anion is more stable than the [BMB]- anion at the inorganic oxide surface.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2018
National Category
Physical Chemistry Chemical Process Engineering
Research subject
Chemistry of Interfaces; Chemical Technology
Identifiers
urn:nbn:se:ltu:diva-70194 (URN)10.1021/acs.jpcc.8b06049 (DOI)000443923500041 ()2-s2.0-85052316588 (Scopus ID)
Note

Validerad;2018;Nivå 2;2018-10-05 (johcin)

Available from: 2018-08-01 Created: 2018-08-01 Last updated: 2018-12-14Bibliographically approved
Farzaneh, A., DeJaco, R. F., Ohlin, L., Holmgren, A., Siepmann, J. I. & Grahn, M. (2017). Comparative Study of the Effect of Defects on Selective Adsorption of Butanol from Butanol/Water Binary Vapor Mixtures in Silicalite-1 Films. Langmuir, 33(34), 8420-8427
Open this publication in new window or tab >>Comparative Study of the Effect of Defects on Selective Adsorption of Butanol from Butanol/Water Binary Vapor Mixtures in Silicalite-1 Films
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2017 (English)In: Langmuir, ISSN 0743-7463, E-ISSN 1520-5827, Vol. 33, no 34, p. 8420-8427Article in journal (Refereed) Published
Abstract [en]

A promising route for sustainable 1-butanol (butanol) production is ABE (acetone, butanol, ethanol) fermentation. However, recovery of the products is challenging because of the low concentrations obtained in the aqueous solution, thus hampering large-scale production of biobutanol. Membrane and adsorbent-based technologies using hydrophobic zeolites are interesting alternatives to traditional separation techniques (e.g., distillation) for energy-efficient separation of butanol from aqueous mixtures. To maximize the butanol over water selectivity of the material, it is important to reduce the number of hydrophilic adsorption sites. This can, for instance, be achieved by reducing the density of lattice defect sites where polar silanol groups are found. The density of silanol defects can be reduced by preparing the zeolite at neutral pH instead of using traditional synthesis solutions with high pH. In this work, binary adsorption of butanol and water in two silicalite-1 films was studied using in situ attenuated total reflectance-Fourier transform infrared (ATR-FTIR) spectroscopy under equal experimental conditions. One of the films was prepared in fluoride medium, whereas the other one was prepared at high pH using traditional synthesis conditions. The amounts of water and butanol adsorbed from binary vapor mixtures of varying composition were determined at 35 and 50 °C, and the corresponding adsorption selectivities were also obtained. Both samples showed very high selectivities (100-23 000) toward butanol under the conditions studied. The sample having low density of defects, in general, showed ca. a factor 10 times higher butanol selectivity than the sample having a higher density of defects at the same experimental conditions. This difference was due to a much lower adsorption of water in the sample with low density of internal defects. Analysis of molecular simulation trajectories provides insights on the local selectivities in the zeolite channel network and at the film surface.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2017
National Category
Chemical Process Engineering
Research subject
Chemical Technology
Identifiers
urn:nbn:se:ltu:diva-65148 (URN)10.1021/acs.langmuir.7b02097 (DOI)000409292500008 ()28767246 (PubMedID)2-s2.0-85028620796 (Scopus ID)
Note

Validerad;2017;Nivå 2;2017-09-05 (rokbeg)

Available from: 2017-08-17 Created: 2017-08-17 Last updated: 2018-07-10Bibliographically approved
Grahn, M., Higman, C., Holmgren, A. & Hedlund, J. (2017). Efficient syngas upgrading with high flux zeolite membranes. In: 34th Annual International Pittsburgh Coal Conference: Coal - Energy, Environment and Sustainable Development, PCC 2017. Paper presented at 34th Annual International Pittsburgh Coal Conference: Coal - Energy, Environment and Sustainable Development, PCC 2017, Pittsburgh, United States, 5-8 September 2017. International Pittsburgh Coal Conference
Open this publication in new window or tab >>Efficient syngas upgrading with high flux zeolite membranes
2017 (English)In: 34th Annual International Pittsburgh Coal Conference: Coal - Energy, Environment and Sustainable Development, PCC 2017, International Pittsburgh Coal Conference , 2017Conference paper, Published paper (Refereed)
Place, publisher, year, edition, pages
International Pittsburgh Coal Conference, 2017
National Category
Chemical Engineering
Research subject
Chemical Technology; Chemical Technology
Identifiers
urn:nbn:se:ltu:diva-69010 (URN)
Conference
34th Annual International Pittsburgh Coal Conference: Coal - Energy, Environment and Sustainable Development, PCC 2017, Pittsburgh, United States, 5-8 September 2017
Available from: 2018-05-31 Created: 2018-05-31 Last updated: 2018-05-31Bibliographically approved
Ohlin, L., Farzaneh, A., Holmgren, A., Hedlund, J. & Grahn, M. (2017). Ternary Adsorption of Methane, Water and Carbon Dioxide in Zeolite Na-ZSM-5 Studied Using in Situ ATR-FTIR Spectroscopy. The Journal of Physical Chemistry C, 121(27), 14703-14711
Open this publication in new window or tab >>Ternary Adsorption of Methane, Water and Carbon Dioxide in Zeolite Na-ZSM-5 Studied Using in Situ ATR-FTIR Spectroscopy
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2017 (English)In: The Journal of Physical Chemistry C, ISSN 1932-7447, E-ISSN 1932-7455, Vol. 121, no 27, p. 14703-14711Article in journal (Refereed) Published
Abstract [en]

The main component in biogas and natural gas is methane but these gases also contain water and carbon dioxide that often have to be removed in order to increase the calorific value of the gas. Membrane and adsorbent-based technologies using zeolites are interesting alternatives for efficient separation of these components. To develop efficient processes, it is essential to know the adsorption properties of the zeolite. In the present work, adsorption of methane, carbon dioxide and water from ternary mixtures in high silica zeolite Na-ZSM-5 was studied using in-situ ATR (Attenuated Total Reflection) – FTIR (Fourier Transform Infrared) spectroscopy. Adsorbed concentrations were extracted from the infrared spectra and the obtained loadings were compared to values predicted by the Ideal Adsorbed Solution Theory (IAST). The IAST could not fully capture the adsorption behavior of this ternary mixture, indicating that the adsorbed phase is not behaving as an ideal mixture. The CO2/CH4 adsorption selectivities determined for the ternary mixtures were compared to selectivities determined for binary mixtures in our previous work, indicating that the presence of water slightly improves the CO2/CH4 adsorption selectivity at lower temperatures. Further, the results show that water and carbon dioxide are adsorbed preferentially over methane in high silica zeolite Na-ZSM-5.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2017
National Category
Chemical Process Engineering
Research subject
Chemical Technology
Identifiers
urn:nbn:se:ltu:diva-64397 (URN)10.1021/acs.jpcc.7b04405 (DOI)000405761600035 ()2-s2.0-85024101175 (Scopus ID)
Note

Validerad;2017;Nivå 2;2017-08-08 (rokbeg)

Available from: 2017-06-22 Created: 2017-06-22 Last updated: 2018-05-28Bibliographically approved
Farzaneh, A., Zhou, M., Antzutkin, O., Bacsik, Z., Hedlund, J., Holmgren, A. & Grahn, M. (2016). Adsorption of Butanol and Water Vapors in Silicalite‑1 Films with a Low Defect Density. Langmuir, 32, 11789-11798
Open this publication in new window or tab >>Adsorption of Butanol and Water Vapors in Silicalite‑1 Films with a Low Defect Density
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2016 (English)In: Langmuir, ISSN 0743-7463, E-ISSN 1520-5827, Vol. 32, p. 11789-11798Article in journal (Refereed) Published
Abstract [en]

Pure silica zeolites are potentially hydrophobic and have therefore been considered to be interesting candidates for separating alcohols, e.g., 1-butanol, from water. Zeolites are traditionally synthesized at high pH, leading to the formation of intracrystalline defects in the form of silanol defects in the framework. These silanol groups introduce polar adsorption sites into the framework, potentially reducing the adsorption selectivity toward alcohols in alcohol/water mixtures. In contrast, zeolites prepared at neutral pH using the fluoride route contain significantly fewer defects. Such crystals should show a much higher butanol/water selectivity than crystals prepared in traditional hydroxide (OH−) media. Moreover, silanol groups are present at the external surface of the zeolite crystals; therefore, minimizing the external surface of the studied adsorbent is important. In this work, we determine adsorption isotherms of 1-butanol and water in silicalite-1 films prepared in a fluoride (F−) medium using in situ attenuated total reflectance−Fourier transform infrared (ATR−FTIR) spectroscopy. This film was composed of well intergrown, plate-shaped b-oriented crystals, resulting in a low external area. Single-component adsorption isotherms of 1-butanol and water were determined in the temperature range of 35− 80 °C. The 1-butanol isotherms were typical for an adsorbate showing a high affinity for a microporous material and a large increase in the amount adsorbed at low partial pressures of 1-butanol. The Langmuir−Freundlich model was successfully fitted to the 1-butanol isotherms, and the heat of adsorption was determined. Water showed a very low affinity for the adsorbent, and the amounts adsorbed were very similar to previous reports for large silicalite-1 crystals prepared in a fluoride medium. The sample also adsorbed much less water than did a reference silicalite-1(OH−) film containing a high density of internal defects.The results show that silicalite-1 films prepared in a F− medium with a low density of defects and external area are very promising for the selective recovery of 1-butanol from aqueous solutions.

National Category
Other Chemical Engineering Chemical Process Engineering
Research subject
Chemical Technology; Chemistry of Interfaces
Identifiers
urn:nbn:se:ltu:diva-60688 (URN)10.1021/acs.langmuir.6b03326 (DOI)000388156000009 ()2-s2.0-84995812342 (Scopus ID)
Note

Validerad; 2016; Nivå 2; 2016-12-02 (andbra)

Available from: 2016-11-25 Created: 2016-11-25 Last updated: 2018-07-10Bibliographically approved
Yang, X., He, J., Sun, Z., Holmgren, A. & Wang, D. (2016). Effect of phosphate on heterogeneous Fenton oxidation of catechol by nano-Fe3O4: Inhibitor or stabilizer? (ed.). Journal of Environmental Sciences(China), 39, 69-76
Open this publication in new window or tab >>Effect of phosphate on heterogeneous Fenton oxidation of catechol by nano-Fe3O4: Inhibitor or stabilizer?
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2016 (English)In: Journal of Environmental Sciences(China), ISSN 1001-0742, E-ISSN 1878-7320, Vol. 39, p. 69-76Article in journal (Refereed) Published
Abstract [en]

The effect of phosphate on adsorption and oxidation of catechol, 1,2-dihydroxybenzene, in a heterogeneous Fenton system was investigated. In situ attenuated total reflectance infrared spectroscopy (ATR-FTIR) was used to monitor the surface speciation at the nano-Fe3O4 catalyst surface. The presence of phosphate decreased the removal rate of catechol and the abatement of dissolved organic compounds, as well as the decomposition of H2O2. This effect of phosphate was mainly due to its strong reaction with surface sites on the iron oxide catalyst. At neutral and acid pH, phosphate could displace the adsorbed catechol from the surface of catalyst and also could compete for surface sites with H2O2. In situ IR spectra indicated the formation of iron phosphate precipitation at the catalyst surface. The iron phosphate surface species may affect the amount of iron atoms taking part in the catalytic decomposition of H2O2 and formation of hydroxyl radicals, and inhibit the catalytic ability of Fe3O4 catalyst. Therefore, phosphate ions worked as stabilizer and inhibitor in a heterogeneous Fenton reaction at the same time, in effect leading to an increase in oxidation efficiency in this study. However, before use of phosphate as pH buffer or H2O2 stabilizer in a heterogeneous Fenton system, the possible inhibitory effect of phosphate on the actual removal of organic pollutants should be fully considered.

National Category
Chemical Process Engineering
Research subject
Chemical Technology
Identifiers
urn:nbn:se:ltu:diva-3649 (URN)10.1016/j.jes.2015.11.007 (DOI)000371515800010 ()26899646 (PubMedID)2-s2.0-84975686849 (Scopus ID)17710f51-ae53-4111-8d07-1716c18064b6 (Local ID)17710f51-ae53-4111-8d07-1716c18064b6 (Archive number)17710f51-ae53-4111-8d07-1716c18064b6 (OAI)
Note

Validerad; 2016; Nivå 2; 20151223 (andbra); Bibliografisk uppgift: 40th Anniversary of RCEES

Available from: 2016-09-29 Created: 2016-09-29 Last updated: 2019-08-23Bibliographically approved
Ohlin, L., Berezovsky, V., Öberg, S., Farzaneh, A., Holmgren, A. & Grahn, M. (2016). Effect of Water on the Adsorption of Methane and Carbon Dioxide in Zeolite Na-ZSM-5 Studied Using in Situ ATR-FTIR Spectroscopy. The Journal of Physical Chemistry C, 120(51), 29144-29152
Open this publication in new window or tab >>Effect of Water on the Adsorption of Methane and Carbon Dioxide in Zeolite Na-ZSM-5 Studied Using in Situ ATR-FTIR Spectroscopy
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2016 (English)In: The Journal of Physical Chemistry C, ISSN 1932-7447, E-ISSN 1932-7455, Vol. 120, no 51, p. 29144-29152Article in journal (Refereed) Published
Abstract [en]

Methane is the main component in biogas and natural gas along with contaminants such as water and carbon dioxide. Separation of methane from these contaminants is therefore an important step in the upgrading process. Zeolite adsorbents and zeolite membranes have great potential to be cost-efficient candidates for upgrading biogas and natural gas, and in both of these applications, knowing the nature of the competitive adsorption is of great importance to further develop the properties of the zeolite materials. The binary adsorption of methane and carbon dioxide in zeolites has been studied to some extent, but the influence of water has been much less studied. In the present work, in situ ATR (attenuated total reflection)–FTIR (Fourier transform infrared) spectroscopy was used to study the adsorption of water/methane and water/carbon dioxide from binary mixtures in a high-silica Na-ZSM-5 zeolite film at various gas compositions and temperatures. Adsorbed concentrations for all species were determined from the recorded IR spectra, and the experimental values were compared to values predicted using the ideal adsorbed solution theory (IAST). At lower temperatures (35, 50, and 85 °C), the IAST was able to predict the binary adsorption of water and methane, whereas the values predicted by the IAST deviated from the experimental data at the highest temperature (120 °C). For the binary adsorption of water and carbon dioxide, the IAST could not predict the adsorption values accurately. This discrepancy was assigned to the particular adsorption behavior of water in high-silica MFI forming clusters at hydrophilic sites. However, the predicted values did follow the same trend as the experimental values. The adsorption selectivity was determined, and it was found that the H2O/CH4 adsorption selectivity was decreasing with increasing water content in the gas phase at low temperatures whereas the selectivity was increasing at higher temperatures. The H2O/CO2 adsorption selectivity was increasing with increasing water content at all temperatures.

National Category
Chemical Process Engineering Other Physics Topics
Research subject
Chemical Technology; Applied Physics
Identifiers
urn:nbn:se:ltu:diva-61272 (URN)10.1021/acs.jpcc.6b09224 (DOI)000391160400028 ()2-s2.0-85008428222 (Scopus ID)
Note

Validerad; 2017; Nivå 2; 2017-01-11 (rokbeg)

Available from: 2016-12-27 Created: 2016-12-27 Last updated: 2018-07-10Bibliographically approved
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Identifiers
ORCID iD: ORCID iD iconorcid.org/0000-0001-9794-8305

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