Probing Metal–Organic Framework Design for Adsorptive Natural Gas Purification
Abstract
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.
- Authors:
-
[1];
[1];
[1];
[1]
- Georgia Inst. of Technology, Atlanta, GA (United States). School of Chemical and Biomolecular Engineering
- Publication Date:
- Research Org.:
- Energy Frontier Research Centers (EFRC) (United States). Center for Understanding and Control of Acid Gas-induced Evolution of Materials for Energy (UNCAGE-ME)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1470678
- Grant/Contract Number:
- SC0012577
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Langmuir
- Additional Journal Information:
- Journal Volume: 34; Journal 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; Journal ID: ISSN 0743-7463
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; catalysis (heterogeneous); defects; membrane; carbon capture; materials and chemistry by design; synthesis (novel materials); synthesis (self-assembly); synthesis (scalable processing)
Citation Formats
Joshi, Jayraj N., Zhu, Guanghui, Lee, Jason J., Carter, Eli A., Jones, Christopher W., Lively, Ryan P., and Walton, Krista S. Probing Metal–Organic Framework Design for Adsorptive Natural Gas Purification. United States: N. p., 2016.
Web. doi:10.1021/acs.langmuir.8b00889.
Joshi, Jayraj N., Zhu, Guanghui, Lee, Jason J., Carter, Eli A., Jones, Christopher W., Lively, Ryan P., & Walton, Krista S. Probing Metal–Organic Framework Design for Adsorptive Natural Gas Purification. United States. https://doi.org/10.1021/acs.langmuir.8b00889
Joshi, Jayraj N., Zhu, Guanghui, Lee, Jason J., Carter, Eli A., Jones, Christopher W., Lively, Ryan P., and Walton, Krista S. Sun .
"Probing Metal–Organic Framework Design for Adsorptive Natural Gas Purification". United States. https://doi.org/10.1021/acs.langmuir.8b00889. https://www.osti.gov/servlets/purl/1470678.
@article{osti_1470678,
title = {Probing Metal–Organic Framework Design for Adsorptive Natural Gas Purification},
author = {Joshi, Jayraj N. and Zhu, Guanghui and Lee, Jason J. and Carter, Eli A. and Jones, Christopher W. and Lively, Ryan P. and Walton, Krista S.},
abstractNote = {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.},
doi = {10.1021/acs.langmuir.8b00889},
journal = {Langmuir},
number = 29,
volume = 34,
place = {United States},
year = {Sun Jun 26 00:00:00 EDT 2016},
month = {Sun Jun 26 00:00:00 EDT 2016}
}
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