Probing Metal–Organic Framework Design for Adsorptive Natural Gas Purification

Joshi, Jayraj N.; Zhu, Guanghui; Lee, Jason J.; Carter, Eli A.; Jones, Christopher W.; Lively, Ryan P.; Walton, Krista S.

doi:10.1021/acs.langmuir.8b00889

Title: Probing Metal–Organic Framework Design for Adsorptive Natural Gas Purification

Journal Article · Sun Jun 26 00:00:00 EDT 2016 · Langmuir

DOI:https://doi.org/10.1021/acs.langmuir.8b00889· OSTI ID:1470678

Joshi, Jayraj N. ^[1];

^[1]; Lee, Jason J. ^[1]; Carter, Eli A. ^[1];

^[1];

^[1]

Georgia Inst. of Technology, Atlanta, GA (United States). School of Chemical and Biomolecular Engineering

Parent and amine-functionalized analogues of metal–organic frameworks (MOFs), UiO-66(Zr), MIL-125(Ti), and MIL-101(Cr), were evaluated for their hydrogen sulfide (H₂S) adsorption efficacy and post-exposure acid gas stability. Adsorption experiments were conducted through fixed-bed breakthrough studies utilizing multicomponent 1% H₂S/99% CH₄ and 1% H₂S/10% CO₂/89% CH₄ natural gas simulant mixtures. Instability of MIL-101(Cr) materials after H₂S exposure was discovered through powder X-ray diffraction and porosity measurements following adsorbent pelletization, whereas other materials retained their characteristic properties. Linker-based amine functionalities increased H₂S breakthrough times and saturation capacities from their parent MOF analogues. Competitive CO₂ adsorption effects were mitigated in mesoporous MIL-101(Cr) and MIL-101–NH₂(Cr), in comparison to microporous UiO-66(Zr) and MIL-125(Ti) frameworks. This result suggests that the installation of H₂S binding sites in large-pore MOFs could potentially enhance H₂S selectivity. In situ Fourier transform infrared measurements in 10% CO₂ and 5000 ppm H₂S environments suggest that framework hydroxyl and amine moieties serve as H₂S physisorption sites. In conclusion, results from this study elucidate design strategies and stability considerations for engineering MOFs in sour gas purification applications.

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Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Center for Understanding and Control of Acid Gas-induced Evolution of Materials for Energy (UNCAGE-ME)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0012577

OSTI ID:: 1470678

Journal Information:: Langmuir, Vol. 34, Issue 29; Related Information: UNCAGE-ME partners with Georgia Institute of Technology (lead); Lehigh University; Oak Ridge National Laboratory; University of Alabama; University of Florida; University of Wisconsin; Washington University in St. Louis; ISSN 0743-7463

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 48 works

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Title: Probing Metal–Organic Framework Design for Adsorptive Natural Gas Purification

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