期刊
ACS APPLIED MATERIALS & INTERFACES
卷 10, 期 19, 页码 16628-16635出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.8b03358
关键词
metal-organic frameworks; molecular sieving; gas adsorption; carbon dioxide; methane; separation
资金
- Zhejiang Provincial Natural Science Foundation of China [LZ18B060001]
- National Natural Science Foundation of China [2172560321436010]
- National Program for Support of Topnotch Young Professionals
- Welch Foundation [AX-1730]
The separation of carbon dioxide (CO2) from hydrocarbons is a critical process for the production of clean energy and high-purity chemicals. Adsorption based on molecular sieving is an energy-saving separation process; however, most of molecular sieves with narrow and straight pore channels exhibit low CO, uptake capacity. Here, we 30 report that a twofold interpenetrated copper coordination network with a consecutive pocket-like pore structure, namely, SIFSIX-14-Cu-i (SIFSIX = hexafluorosilicate, 14 = 4,4'azopyridine, i = interpenetrated) is a remarkable CO2/CH4 molecular sieving adsorbent which completely blocks the larger CH4 molecule with unprecedented selectivity, whereas it has excellent CO, uptake (172.7 cm(3)/cm(3)) under the ambient condition. The exceptional separation performance of SIFSIX-14-Cu-i is attributed to its unique pore shape and functional pore surface, which combine a contracted pore window (3.4 angstrom) and a relatively large pore cavity decorated with high density of inorganic anions. Dispersion-corrected density functional theory calculation and neutron powder diffraction were performed to understand the CO2 binding sites. The practical feasibility of SIFSIX-14-Cu-i for CO2/CH4 mixtures separation was validated by experimental breakthrough tests. This study not only demonstrates the great potential of SIFSIX-14-Cu-i for CO2 separation but also provides important clues for other gas separations.
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