Monte Carlo Simulations Probing the Adsorptive Separation of Hydrogen Sulfide/Methane Mixtures Using All-Silica Zeolites
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Selective removal of hydrogen sulfide (H2S) from sour natural gas mixtures is one of the key challenges facing the natural gas industry. Adsorption and pervaporation processes utilizing nanoporous materials, such as zeolites, can be alternatives to highly energy-intensive amine-based absorption processes. In this work, the adsorption behavior of binary mixtures containing H2S and methane (CH4) in seven different all-silica zeolite frameworks (CHA, DDR, FER, IFR, MFI, MOR, and MWW) is investigated using Gibbs ensemble Monte Carlo simulations at two temperatures (298 and 343 K) and pressures ranging from 1 to 50 bar. The simulations demonstrate high selectivities that, with the exception of MOR, increase with increasing H2S concentration due to favorable sorbate-sorbate interactions. The simulations indicate significant inaccuracies of predictions using unary adsorption data and ideal adsorbed solution theory. In addition, the adsorption of binary H2S/H2O mixtures in MFI is considered to probe whether the presence of H2S induces coadsorption and reduces the hydrophobic character of all-silica zeolites. The simulations show preferential adsorption of H2S from moist gases with a selectivity of about 18 over H2O.
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Pure silica CHA and MFI zeolites are promising candidates for H2S removal.
“Promising candidates from these studies are pure silica CHA and MFI zeolites.587−589”
From Zeolites in Adsorption Processes: State of the Art and Future Prospects (2022) · cites this paper as [587]
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- Authors
- Shah, M. S., Tsapatsis, M., & Siepmann, J. I.
- Affiliations
- University of Minnesota (US)
- Department of Chemical Engineering and Materials Science, University of Minnesota, 421 Washington Avenue SE, Minneapolis, Minnesota 55455-0132, United States
- Corresponding author
- Siepmann, J. Ilja
- Venue
- Langmuir
- Publisher
- American Chemical Society (ACS)
- Published
- 2015-10-27
- Volume
- 31
- Issue
- 44
- Pages
- 12268-12278
- ISSN
- 0743-7463 (ISSN-L)
- 1520-5827
- OpenAlex
- W2197027196
- Cited by
- 46
- References
- 36
- Citations by year
- 2026: 2 · 2025: 3 · 2024: 7 · 2023: 2 · 2022: 6 · 2021: 3 · 2020: 5 · 2019: 4 · 2018: 4 · 2017: 5 · 2016: 5
- FWCI
- 1.92
- Type
- journal article
- Language
- en
- Open access
- green
- www.osti.gov
- Locations
- Langmuir (publishedVersion)
- PubMed (publishedVersion)
- OSTI OAI (U.S. Department of Energy Office of Scientific and Technical Information) (submittedVersion)
- Funders
- Basic Energy Sciences (DE-FG02-12ER16362)
- Topics
- Physical Sciences › Chemistry › Inorganic Chemistry › Zeolite Catalysis and Synthesis
- Physical Sciences › Engineering › Mechanical Engineering › Membrane Separation and Gas Transport
- Physical Sciences › Engineering › Mechanical Engineering › Carbon Dioxide Capture Technologies
- Keywords
- hydrogen sulfide removal, all-silica zeolites, adsorption selectivity, natural gas desulfurization, binary gas mixtures, zeolite hydrophobicity, ideal adsorbed solution theory, MFI zeolite, MWW zeolite, MOR zeolite, FER zeolite, DDR zeolite, CHA zeolite, Gibbs ensemble Monte Carlo
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