期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 60, 期 21, 页码 11688-11694出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202016673
关键词
binding site control; CO2; C2H2 separation; inverse selectivity; porous coordination polymers; ultramicroporous materials
资金
- National Natural Science Foundation of China [21906120, 51978491]
- Japan Society for the Promotion of Science (JSPS) [JP18H05262, JP19K15584]
- Japan Synchrotron Radiation Research Institute (JASRI) [2019B1296, 2020A1412, 2020A0617]
This study demonstrates the importance of controlling gas sorption through simple pore modification for molecular recognition and industrial separation processes, and presents a strategy for enhancing CO2/C2H2 selectivity by designing channel pores to increase CO2 adsorption while suppressing C2H2 adsorption. The newly synthesized ultramicroporous PCPs show high CO2 uptake and CO2/C2H2 volume uptake ratio, with breakthrough separation performances and remarkable stability for C2H2 purification from CO2/C2H2 mixtures.
Controlling gas sorption by simple pore modification is important in molecular recognition and industrial separation processes. In particular, it is challenging to realize the inverse selectivity, which reduces the adsorption of a high-affinity gas and increases the adsorption of a low-affinity gas. Herein, an opposite action strategy is demonstrated for boosting CO2/C2H2 selectivity in porous coordination polymers (PCPs). A precise steric design of channel pores using an amino group as an additional interacting site enabled the synergetic increase in CO2 adsorption while suppressing the C2H2 adsorption. Based on this strategy, two new ultramicroporous PCP physisorbents that are isostructural were synthesised. They exhibited the highest CO2 uptake and CO2/C2H2 volume uptake ratio at 298 K. Origin of this specific selectivity was verified by detailed density functional theory calculations. The breakthrough separation performances with remarkable stability and recyclability of both the PCPs render them relevant materials for C2H2 purification from CO2/C2H2 mixtures.
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