期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 55, 期 22, 页码 6411-6416出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201600431
关键词
hydrogen evolution reaction; metal-organic frameworks; photocatalysis; polyoxometalate
资金
- U.S. National Science Foundation [DMR-1308229]
- National Natural Science Foundation of China [21471126, 21422106]
- State Scholarship Fund from the China Scholarship Council (CSC)
- Division Of Materials Research
- Direct For Mathematical & Physical Scien [1308229] Funding Source: National Science Foundation
Metal-organic frameworks (MOFs) provide a tunable platform for hierarchically integrating multiple components to effect synergistic functions that cannot be achieved in solution. Here we report the encapsulation of a Ni-containing polyoxometalate (POM) [Ni-4(H2O)(2)(PW9O34)(2)](10-) (Ni4P2) into two highly stable and porous phosphorescent MOFs. The proximity of Ni4P2 to multiple photosensitizers in Ni4P2@MOF allows for facile multi-electron transfer to enable efficient visible-light-driven hydrogen evolution reaction (HER) with turnover numbers as high as 1476. Photophysical and electrochemical studies established the oxidative quenching of the excited photosensitizer by Ni4P2 as the initiating step of HER and explained the drastic catalytic activity difference of the two POM@MOFs. Our work shows that POM@MOF assemblies not only provide a tunable platform for designing highly effective photocatalytic HER catalysts but also facilitate detailed mechanistic understanding of HER processes.
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