Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 55, Issue 36, Pages 10776-10780Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201604313
Keywords
bioinspired catalysts; epoxides; flexible MOFs; pore opening; switchable catalysts
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Funding
- Center for Gas Separations Relevant to Clean Energy Technologies, an Energy Frontier Research Center - U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC0001015]
- Hydrogen and Fuel Cell Program [DE-EE-0007049]
- National Science Foundation [CHE-1300787]
- Welch Foundation [A-0648]
- U.S. Department of Energy Office of Fossil Energy, National Energy Technology Laboratory [DE-FE0026472]
- ConocoPhillips
- Dow Chemical Graduate Fellowship
- Division Of Chemistry
- Direct For Mathematical & Physical Scien [1300787] Funding Source: National Science Foundation
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Flexible metal-organic frameworks (MOFs) are highly desirable in host-guest chemistry owing to their almost unlimited structural/functional diversities and stimuli-responsive pore architectures. Herein, we designed a flexible Zr-MOF system, namely PCN-700 series, for the realization of switchable catalysis in cycloaddition reactions of CO2 with epoxides. Their breathing behaviors were studied by successive single-crystal X-ray diffraction analyses. The breathing amplitudes of the PCN-700 series were modulated through pre-functionalization of organic linkers and post-synthetic linker installation. Experiments and molecular simulations confirm that the catalytic activities of the PCN-700 series can be switched on and off upon reversible structural transformation, which is reminiscent of sophisticated biological systems such as allosteric enzymes.
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