4.8 Article

Molecular co-catalyst accelerating hole transfer for enhanced photocatalytic H2 evolution

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NATURE COMMUNICATIONS
卷 6, 期 -, 页码 -

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NATURE PUBLISHING GROUP
DOI: 10.1038/ncomms9647

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资金

  1. National Basic Research Program of China [2015CB932302, 2010CB923300]
  2. National Natural Science Foundation of China [21222101, U1432133, 11132009, 21331005, 11321503, U1532265, J1030412, 21173205, 91127042]
  3. Chinese Academy of Sciences [XDB01020000]
  4. Fok Ying-Tong Education Foundation, China [141042]
  5. Fundamental Research Funds for the Central Universities [WK2060190027, WK2340000063]

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In artificial photocatalysis, sluggish kinetics of hole transfer and the resulting high-charge recombination rate have been the Achilles' heel of photocatalytic conversion efficiency. Here we demonstrate water-soluble molecules as co-catalysts to accelerate hole transfer for improved photocatalytic H-2 evolution activity. Trifluoroacetic acid (TFA), by virtue of its reversible redox couple TFA center dot/TFA(-), serves as a homogeneous co-catalyst that not only maximizes the contact areas between co-catalysts and reactants but also greatly promotes hole transfer. Thus K4Nb6017 nanosheet catalysts achieve drastically increased photocatalytic H-2 production rate in the presence of TFA, up to 32 times with respect to the blank experiment. The molecular co-catalyst represents a new, simple and highly effective approach to suppress recombination of photogenerated charges, and has provided fertile new ground for creating high-efficiency photosynthesis systems, avoiding use of noble-metal co-catalysts.

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