期刊
CHEMICAL SCIENCE
卷 11, 期 47, 页码 12807-12815出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/d0sc04979d
关键词
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资金
- Department of Energy, National Energy Technology Laboratory, an agency of the United States Government
- Leidos Research Support Team (LRST) [89243318CFE000003]
- National Energy Technology Laboratory, U.S. Environmental Protection Agency
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC0018331]
- University of Pittsburgh
Metal-organic frameworks constructed from multiple (>= 3) components often exhibit dramatically increased structural complexity compared to their 2 component (1 metal, 1 linker) counterparts, such as multiple chemically unique pore environments and a plurality of diverse molecular diffusion pathways. This inherent complexity can be advantageous for gas separation applications. Here, we report two isoreticular multicomponent MOFs, bMOF-200 (4 components; Cu, Zn, adeninate, pyrazolate) and bMOF-201 (3 components; Zn, adeninate, pyrazolate). We describe their structures, which contain 3 unique interconnected pore environments, and we use Kohn-Sham density functional theory (DFT) along with the climbing image nudged elastic band (CI-NEB) method to predict potential H-2/CO2 separation ability of bMOF-200. We examine the H-2/CO2 separation performance using both column breakthrough and membrane permeation studies. bMOF-200 membranes exhibit a H-2/CO2 separation factor of 7.9. The pore space of bMOF-201 is significantly different than bMOF-200, and one molecular diffusion pathway is occluded by coordinating charge-balancing formate and acetate anions. A consequence of this structural difference is reduced permeability to both H-2 and CO2 and a significantly improved H-2/CO2 separation factor of 22.2 compared to bMOF-200, which makes bMOF-201 membranes competitive with some of the best performing MOF membranes in terms of H-2/CO2 separations.
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