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Miana, M. P., Coronas, J., Hedlund, J. & Yu, L. (2024). Highly permeable ZIF-8 membranes for C2H4/C2H6 separation in a wide temperature range. Separation and Purification Technology, 330(Part A), Article ID 125329.
Open this publication in new window or tab >>Highly permeable ZIF-8 membranes for C2H4/C2H6 separation in a wide temperature range
2024 (English)In: Separation and Purification Technology, ISSN 1383-5866, E-ISSN 1873-3794, Vol. 330, no Part A, article id 125329Article in journal (Refereed) Published
Abstract [en]

Ethylene/ethane separation is a critical and energy-consuming process in the chemical industry due to the similar properties of the compounds and the great need of ethylene for e.g., polymer production. Many materials have been studied for their implementation as membranes as an energetically favorable alternative to conventional distillation and adsorption processes. Metal-organic frameworks (MOF) have revealed promising properties as highly permeable and selective membranes. Among the most studied and promising MOF candidates is ZIF-8, known for its thermal stability and small pores connected by narrow-sized windows. In this work, we present an analysis of the influence of parameters such as temperature, feed pressure and feed flowrate on the separation of ethylene/ethane through a thin ZIF-8/alumina disc membrane. We observed that the temperature has a significant effect on the separation. The ethylene permeance increased with decreased temperature and reached 8.1 × 10−7 mol/(m2·s·Pa) at −30 °C. At this temperature, the ethylene/ethane selectivity was 2.5. The study concluded with a considerable enhancement of the permeance of ZIF-8 membranes for ethylene/ethane separations, while maintaining a good selectivity compared to the reported values in the literature. The results have important implications for the development of more cost-effective and energy-efficient membrane-based separation technologies for ethylene purification.

Place, publisher, year, edition, pages
Elsevier B.V., 2024
Keywords
Ethane, Ethylene, High permeability, Olefin/paraffin separation, Ultrathin ZIF-8 membranes
National Category
Chemical Process Engineering
Research subject
Chemical Technology
Identifiers
urn:nbn:se:ltu:diva-101873 (URN)10.1016/j.seppur.2023.125329 (DOI)2-s2.0-85173841359 (Scopus ID)
Note

Validerad;2023;Nivå 2;2023-11-08 (marisr);

License fulltext: CC BY-NC-ND

Available from: 2023-10-31 Created: 2023-10-31 Last updated: 2023-11-08Bibliographically approved
Zhou, M., Bodenmuller, N. & Hedlund, J. (2023). Enhanced bio-oil upgrading by sub-microscale dispersed silanol-free ZSM-5 nanosheets and evidence for revealing an unconventional mechanism. Chemical Engineering Journal, 478, Article ID 147457.
Open this publication in new window or tab >>Enhanced bio-oil upgrading by sub-microscale dispersed silanol-free ZSM-5 nanosheets and evidence for revealing an unconventional mechanism
2023 (English)In: Chemical Engineering Journal, ISSN 1385-8947, E-ISSN 1873-3212, Vol. 478, article id 147457Article in journal (Refereed) Published
Abstract [en]

Silanol-free ZSM-5 nanosheet with merely 35 nm thickness in the b-axis was synthesized by seeded growth from defect-free 10 nm silicalite-1 in a fluoride medium (denoted as F35). Submicron-scaled stöber sol silica beads were introduced into the gap between nanosheets to serve as a spacer for the prevention of neighboring crystals' close contact with each other, which can improve the heat and mass transportation during the catalytic reactions when compared to the aggregated zeolite crystals. Methanol-to-hydrocarbons (MTH) and model bio-oil upgrading were conducted by using dispersed F35, respectively, and the results were compared to the aggregated ZSM-5. The effluent from bio-oil upgrading through dispersed F35 contains no heavier compound, which was considered as the coke precursor, and significantly reduced amount of unreacted feeding molecule. GC–MS revealed that the coke solution from dispersed F35 contains a considerably reduced (61 %) amount of heavier carbon species. Among them, some species have molecular configurations highly consistent with the zeolite channel structure. The dispersed F35 shows a 33 % longer life in catalytic reactions and a 60 % decreased amount of external thermal cock. An unconventional ‘temperature-determined flexible channel’ mechanism that explains the ‘host–guest’ interactive behavior under catalytic reaction was proposed.

Place, publisher, year, edition, pages
Elsevier, 2023
Keywords
ZSM-5, Bio-oil upgrading, Deoxygenation, Methanol-to-hydrocarbons, Coke reduction
National Category
Chemical Process Engineering
Research subject
Chemical Technology
Identifiers
urn:nbn:se:ltu:diva-102653 (URN)10.1016/j.cej.2023.147457 (DOI)
Funder
Swedish Research CouncilSwedish Research Council FormasBio4Energy
Note

Validerad;2023;Nivå 2;2023-11-22 (joosat);

CC BY 4.0 License

Available from: 2023-11-22 Created: 2023-11-22 Last updated: 2023-11-22Bibliographically approved
Yu, L., Kyriazidou, I., Zhou, M. & Hedlund, J. (2023). Highly permeable DDR membranes. Journal of Membrane Science, 687, Article ID 122039.
Open this publication in new window or tab >>Highly permeable DDR membranes
2023 (English)In: Journal of Membrane Science, ISSN 0376-7388, E-ISSN 1873-3123, Vol. 687, article id 122039Article in journal (Refereed) Published
Abstract [en]

In this study, DDR membranes with a layer thickness of approximately 700 nm were studied for separation feeds comprising mixtures of CO2 and CH4. The membranes displayed the highest CO2 over CH4 permselectivity and CO2 permeability reported in literature. This was ascribed to a defect-free and ultra-thin zeolite film as well as an open and highly permeable support. For equimolar mixtures, the highest CO2 over CH4 permselectivity of 727 was observed when the pressure at the feed side was 5 bar(a) and the permeate pressure was 1 bar(a) at 25 °C. At these conditions, the CO2 permeability was very high at 45 × 10−7 mol/(m2 s Pa). Separation experiments for 80/20 and 20/80 mixtures were also performed, and in these cases, CO2 over CH4 permselectivities of 1011 and 622 were observed, respectively. For all feeds, the membrane permselectivity decreased slightly at higher temperature and in all cases, higher permselectivity was observed when vacuum was applied at the permeate side. One-stage membrane processes for upgrading biogas to biomethane at three different operating pressures were designed based on the experimental data. In all cases, a quite low membrane area, methane slip and power need were observed.

Place, publisher, year, edition, pages
Elsevier B.V., 2023
Keywords
Biogas, Biomethane, CO2 separation, DDR zeolite membrane, High permeability
National Category
Chemical Process Engineering
Research subject
Chemical Technology
Identifiers
urn:nbn:se:ltu:diva-101337 (URN)10.1016/j.memsci.2023.122039 (DOI)2-s2.0-85169829212 (Scopus ID)
Funder
Swedish Research Council FormasSwedish Research CouncilBio4Energy
Note

Validerad;2023;Nivå 2;2023-09-13 (joosat);

CC BY-NC-ND 4.0 License

Available from: 2023-09-13 Created: 2023-09-13 Last updated: 2023-09-13Bibliographically approved
Yu, L. & Hedlund, J. (2023). Large and Highly Selective and Permeable CHA Zeolite Membranes. Industrial & Engineering Chemistry Research, 62(39), 16058-16069
Open this publication in new window or tab >>Large and Highly Selective and Permeable CHA Zeolite Membranes
2023 (English)In: Industrial & Engineering Chemistry Research, ISSN 0888-5885, E-ISSN 1520-5045, Vol. 62, no 39, p. 16058-16069Article in journal (Refereed) Published
Abstract [en]

Large (100 cm2 membrane area) tubular chabazite (CHA) zeolite membranes (450 nm thick) were experimentally evaluated for the separation of CO2/CH4 in an industrial laboratory. An industrially relevant feed flow rate of 250 Ndm3/min was used. The feed pressure and temperature were varied in the ranges of 5–18 bar and 292–318 K, respectively. For a CO2/CH4 feed with a molar ratio of 1:1, the experimental CO2/CH4 selectivity was high at 205, and the CO2 permeance arrived at 52 × 10–7 mol/(m2·s·Pa) at 5 bar and 292 K. As far as we know, there is no report in the literature on large CHA membranes with such high permeability and selectivity. A high CO2/CH4 selectivity was also observed for a 1:4 CO2/CH4 feed. However, as indicated by mathematical modeling, concentration polarization was still an issue for membrane performance, especially at high operating pressures, even though the flow rate of the feed was relatively high. Without concentration polarization, the theoretical CO2/CH4 selectivity was 41% higher than the experimental value for a 1:1 CO2/CH4 feed at 18 bar. The corresponding CO2 permeance without concentration polarization was 23% higher than the experimentally observed value, reaching 34 × 10–7 mol/(m2·s·Pa). CHA membrane processes for the removal of CO2 from CH4 were designed, and the electricity consumption and module cost of the process were also estimated. All of the results in this study indicate a great potential of the large CHA membranes for biogas and natural gas upgrading; however, concentration polarization should be minimized in industrial processes.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2023
National Category
Chemical Process Engineering
Research subject
Chemical Technology
Identifiers
urn:nbn:se:ltu:diva-101436 (URN)10.1021/acs.iecr.3c02016 (DOI)2-s2.0-85174252538 (Scopus ID)
Funder
Swedish Research CouncilThe Kempe Foundations, JCK-1904.1Bio4Energy
Note

Validerad;2023;Nivå 2;2023-11-09 (hanlid);

Full text license: CC BY

Available from: 2023-09-25 Created: 2023-09-25 Last updated: 2023-11-09Bibliographically approved
Thoresen, P. P., Fahrni, J., Lange, H., Hertzog, J., Carre, V., Zhou, M., . . . Matsakas, L. (2023). On the understanding of bio-oil formation from the hydrothermal liquefaction of organosolv lignin isolated from softwood and hardwood sawdust. Sustainable Energy & Fuels, 7(22), 5361-5373
Open this publication in new window or tab >>On the understanding of bio-oil formation from the hydrothermal liquefaction of organosolv lignin isolated from softwood and hardwood sawdust
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2023 (English)In: Sustainable Energy & Fuels, E-ISSN 2398-4902, Vol. 7, no 22, p. 5361-5373Article in journal (Refereed) Published
Abstract [en]

Conversion of organosolv lignins isolated with and without an inorganic acid catalyst (H2SO4) from hard- and softwood (birch and spruce) into bio-oil through hydrothermal liquefaction has been investigated. Furthermore, fractions of the isolated bio-oils were catalytically deoxygenated to improve the bio-oil properties. As elucidated through NMR, both biomass source and extraction mode influence the bio-oil product distribution. Depending on whether the lignins carry a high content of native structures, or are depolymerized and subsequently condensed in the presence of sugar dehydration products, will dictate heavy oil (HO) and light oil (LO) distribution, and skew the HO product composition, which again will influence the requirements upon catalytical deoxygenation.

Place, publisher, year, edition, pages
Royal Soc Chemistry, 2023
National Category
Bioprocess Technology Wood Science
Research subject
Biochemical Process Engineering; Chemical Technology
Identifiers
urn:nbn:se:ltu:diva-101956 (URN)10.1039/d3se00976a (DOI)001080742900001 ()2-s2.0-85174410902 (Scopus ID)
Projects
Upgrading of organosolv lignin to jet fuel (GOLdJET FUEL)Eco-efficient biorefinery for competitive production of green renewable shipping fuels (ECO-FORCE FUELS)
Funder
Swedish Energy Agency, 2019-005832; 2022-201046
Note

Validerad;2023;Nivå 2;2023-11-14 (marisr);

Funder: European Regional Development Fund (FEDER); general council of Moselle, Region Grand Est, Metz Metropole; University of Lorraine (RESEX project);

License fulltext: CC BY

Available from: 2023-10-31 Created: 2023-10-31 Last updated: 2023-11-14Bibliographically approved
Hedlund, J., Zhou, M., Faisal, A., Öhrman, O. G. .., Finelli, V., Signorile, M., . . . Grahn, M. (2022). Controlling diffusion resistance, selectivity and deactivation of ZSM-5 catalysts by crystal thickness and defects. Journal of Catalysis, 410, 320-332
Open this publication in new window or tab >>Controlling diffusion resistance, selectivity and deactivation of ZSM-5 catalysts by crystal thickness and defects
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2022 (English)In: Journal of Catalysis, ISSN 0021-9517, E-ISSN 1090-2694, Vol. 410, p. 320-332Article in journal (Refereed) Published
Abstract [en]

A systematic investigation of two sets of defect free and defective ZSM-5 crystals with controlled thickness (T) between 30 and 400 nm and of their performances in methanol conversion was reported for the first time in the present work. The defect free ZSM-5 crystals with a thickness of 35 nm are by far the smallest ever reported and displayed superior activity, stability and selectivity to slower diffusing compounds, which resulted in high yield of e.g. gasoline and the 1,2,4-trimethylbenzene isomer with high octane number, as compared to the other studied catalysts. Almost only products forming in the zeolite pores were detected and consequently, the external surface must be nearly inactive. Strong correlations between T and deactivation rate were observed. Thick crystals deactivated much faster than thin crystals, probably due to formation of carbon species in the zeolite pores, which results in pronounced percolation effects and faster deactivation of the former. At comparable thickness, crystals with defects deactivated much faster than defect free crystals, due to formation of additional small molecular coke species in the former. Strong correlations between T and selectivity were also observed and assigned to control of diffusion resistance by crystal thickness.

Place, publisher, year, edition, pages
Elsevier, 2022
Keywords
H-ZSM-5, Defects, Gasoline, Deactivation, MTG
National Category
Chemical Process Engineering Biochemistry and Molecular Biology
Research subject
Chemical Technology
Identifiers
urn:nbn:se:ltu:diva-90477 (URN)10.1016/j.jcat.2022.04.013 (DOI)000799277700003 ()2-s2.0-85129698365 (Scopus ID)
Funder
Swedish Research Council, 2014-04585_VRBio4EnergySwedish Energy Agency, P41164-1
Note

Validerad;2022;Nivå 2;2022-06-01 (hanlid)

Available from: 2022-05-02 Created: 2022-05-02 Last updated: 2023-09-05Bibliographically approved
Yu, L., Nobandegani, M. & Hedlund, J. (2022). Industrially relevant CHA membranes for CO2/CH4 separation. Journal of Membrane Science, 641, Article ID 119888.
Open this publication in new window or tab >>Industrially relevant CHA membranes for CO2/CH4 separation
2022 (English)In: Journal of Membrane Science, ISSN 0376-7388, E-ISSN 1873-3123, Vol. 641, article id 119888Article in journal (Refereed) Published
Abstract [en]

In the present work, single channel tubular zeolite CHA membranes with a length of 50 cm and a membrane area of 100 cm2 were evaluated by SEM and permeation experiments with single components and industrially relevant humid mixtures. The membranes comprised well-intergrown and smooth CHA films with a thickness of <500 nm supported on the inside of a highly porous tube. For single component permeation, a very low SF6 permeance of 4.5 × 10−10 mol/(m2‧s‧Pa) was observed, which indicated nearly defect free membranes. On the contrary, the membranes displayed a very high CO2 permeance of 128 × 10−7 mol/(m2‧s‧Pa), which illustrated the very high permeability of the CHA pores. Finally, the membranes displayed excellent selectivity for separation of industrially relevant CO2/CH4/H2O mixtures, which was attributed to selective interaction between the CO2 molecules and the polar water molecules in the pores. The highest observed CO2/CH4 separation selectivity was as high as 198 in combination with a CO2 permeance of 14 × 10−7 mol/(m2‧s‧Pa) at a feed pressure of 600 kPa (including 2.2 kPa water) and 293K. The corresponding CO2 flux was 0.39 mol/(m2‧s) and the corresponding CO2/CH4 separation factor was 162. The observed membrane performance was reduced by concentration polarisation due to the limited feed flow in the experimental setup. The corresponding selectivity and CO2 permeance corrected for concentration polarisation were as high as 236 and 16 × 10−7 mol/(m2‧s‧Pa), and the corrected CO2 flux was 0.44 mol/(m2‧s) and corrected separation factor was 198. An estimate showed that even at a low feed pressure of 500 kPa, it would be sufficient with as few as 64 membranes for processing of a feed of 100 Nm3/h raw biogas, i.e. the capacity of a typical biogas plant at a large farm, to biomethane with high purity. These results illustrated that the membranes are promising candidates for industrial separation of CO2 from e.g. natural gas and biogas.

Place, publisher, year, edition, pages
Elsevier, 2022
Keywords
Tubular zeolite CHA membrane, Scale-up, Industrially relevant gas separation, Natural gas, Biogas
National Category
Chemical Process Engineering
Research subject
Chemical Technology
Identifiers
urn:nbn:se:ltu:diva-87332 (URN)10.1016/j.memsci.2021.119888 (DOI)000705872500002 ()2-s2.0-85115369262 (Scopus ID)
Funder
Swedish Research CouncilSwedish Research Council FormasThe Kempe Foundations, JCK-1904.1Bio4Energy
Note

Validerad;2021;Nivå 2;2021-10-04 (alebob)

Available from: 2021-10-04 Created: 2021-10-04 Last updated: 2022-02-20Bibliographically approved
Nobandegani, M., Yu, L. & Hedlund, J. (2022). Mass transport of CO2 over CH4 controlled by the selective surface barrier in ultra-thin CHA membranes. Microporous and Mesoporous Materials, 332, Article ID 111716.
Open this publication in new window or tab >>Mass transport of CO2 over CH4 controlled by the selective surface barrier in ultra-thin CHA membranes
2022 (English)In: Microporous and Mesoporous Materials, ISSN 1387-1811, E-ISSN 1873-3093, Vol. 332, article id 111716Article in journal (Refereed) Published
Abstract [en]

The adsorption and mass transport of CO2 and CH4 in CHA zeolite were studied experimentally. First, large and well-defined CHA crystals with varying Si/Al ratios and morphologies ideal for adsorption studies were prepared. Then, adsorption isotherms were measured, and adsorption parameters were estimated from the data. In the next step, permeation experiments for pure components and mixtures were conducted for a defect-free CHA membrane with a Si/Al ratio of 80 and a thickness of 600 nm over a wide temperature range. A maximum selectivity of 243 in combination with a CO2 permeance of 70 × 10−7 mol/(m2 s Pa) was observed for a feed of an equimolar CO2/CH4 mixture at 273 K and 5.5 bar. Finally, a simple model accounting for adsorption and diffusion through the surface barriers and the interior of the pores of the membrane was fitted to the permeation data. The fitted model indicated that the surface barrier was a surface diffusion process at the pore mouth with higher activation energy than the diffusion process within the pores. The model also showed that the highly selective mass transport in the membrane was mostly a result of a selective surface barrier and, to a lesser extent, a result of adsorption selectivity.

Place, publisher, year, edition, pages
Elsevier, 2022
Keywords
Activation energy, Adsorption, Mass transport, Surface barrier, Surface diffusion
National Category
Chemical Process Engineering
Research subject
Chemical Technology
Identifiers
urn:nbn:se:ltu:diva-89075 (URN)10.1016/j.micromeso.2022.111716 (DOI)000761764300006 ()2-s2.0-85123872231 (Scopus ID)
Funder
Swedish Research Council FormasSwedish Research CouncilBio4Energy
Note

Validerad;2022;Nivå 2;2022-02-21 (hanlid)

Available from: 2022-02-01 Created: 2022-02-01 Last updated: 2022-07-04Bibliographically approved
Yu, L., Mayne, B., Nobandegani, M. S., Grekou, T. & Hedlund, J. (2022). Recovery of helium from natural gas using MFI membranes. Journal of Membrane Science, 644, Article ID 120113.
Open this publication in new window or tab >>Recovery of helium from natural gas using MFI membranes
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2022 (English)In: Journal of Membrane Science, ISSN 0376-7388, E-ISSN 1873-3123, Vol. 644, article id 120113Article in journal (Refereed) Published
Abstract [en]

The development of more efficient technology for the production of helium from natural gas is pressing as the current resources are dwindling. In the present work, ultra-thin MFI membranes were evaluated for the separation of an equimolar CH4/N2/He mixture in a wide temperature range 120–293K. The membrane was highly selective towards CH4 and N2 at all the investigated conditions, which resulted in a helium rich retentate. The observed selectivity should be a result of selective adsorption of CH4 and N2. A maximum (CH4+N2)/He separation factor of 152 was observed at 153 K and a feed pressure of 3 bar and a permeate pressure of 0.2 bar. At these conditions, separation factors were 265 and 38 for CH4/He and N2/He, respectively, and the CH4 and N2 fluxes were 1.12 and 0.16 mol/(m2⋅s), respectively. To the best of our knowledge, these are the best results reported in the open literature for the recovery of helium from natural gas using membrane technology. The high selectivity and flux indicated that the ultra-thin MFI membranes are a promising candidate for efficient helium production from natural gas.

Place, publisher, year, edition, pages
Elsevier, 2022
Keywords
High-flux MFI membrane, Natural gas, Helium production, Methane, Nitrogen
National Category
Chemical Process Engineering
Research subject
Chemical Technology
Identifiers
urn:nbn:se:ltu:diva-87961 (URN)10.1016/j.memsci.2021.120113 (DOI)000788512800002 ()2-s2.0-85119933714 (Scopus ID)
Funder
Swedish Research CouncilSwedish Research Council FormasThe Kempe Foundations, JCK-1904.1Bio4Energy
Note

Validerad;2022;Nivå 2;2022-03-04 (hanlid)

Available from: 2021-11-22 Created: 2021-11-22 Last updated: 2022-05-12Bibliographically approved
Hedlund, J., Nobandegani, M. S. & Yu, L. (2022). The origin of the surface barrier in nanoporous materials. Journal of Membrane Science, 641, Article ID 119893.
Open this publication in new window or tab >>The origin of the surface barrier in nanoporous materials
2022 (English)In: Journal of Membrane Science, ISSN 0376-7388, E-ISSN 1873-3123, Vol. 641, article id 119893Article in journal (Refereed) Published
Abstract [en]

Surface barriers are influencing the mass transfer in nanopores, but their origin is unclear and can be quite different in different materials. For MFI and CHA membranes studied here, we show that the surface barrier may be a surface diffusion process with higher activation energy than the surface diffusion process in the pores, but other possible mechanisms such as pore blocking and pore narrowing has not been ruled out. The higher activation energy is probably a result of less interaction between adsorbed molecules at the pore mouth than inside the pores, i.e. the barrier is simply a geometrical effect in these materials. For pure components at low concentration in MFI zeolite, we found that barrier is proportional to the product of the molecular weight and heat of desorption. For MFI and CHA zeolite, we observed that the barrier is a function of concentration and approach zero at high concentration and that the barriers of the components become more similar due to interaction between the components in mixtures, which explains the high and selective mass transfer displayed by these nanoporous materials at high concentration.

Place, publisher, year, edition, pages
Elsevier, 2022
Keywords
Surface barrier, Nanoporous materials, Mass transfer, Surface diffusion, Activation energy
National Category
Chemical Process Engineering
Research subject
Chemical Technology
Identifiers
urn:nbn:se:ltu:diva-87194 (URN)10.1016/j.memsci.2021.119893 (DOI)000705871700004 ()2-s2.0-85115774975 (Scopus ID)
Funder
Swedish Research CouncilSwedish Research Council FormasBio4Energy
Note

Validerad;2021;Nivå 2;2021-10-01 (alebob)

Available from: 2021-09-23 Created: 2021-09-23 Last updated: 2022-02-20Bibliographically approved
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ORCID iD: ORCID iD iconorcid.org/0000-0003-1053-4623

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