4.8 Article

Oxide Defect Engineering Enables to Couple Solar Energy into Oxygen Activation

期刊

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 138, 期 28, 页码 8928-8935

出版社

AMER CHEMICAL SOC
DOI: 10.1021/jacs.6b04629

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资金

  1. 973 Program [2014CB848900]
  2. NSFC [21471141, U1532135, 11375198, 11574280, U1532112]
  3. Recruitment Program of Global Experts
  4. CAS Hundred Talent Program
  5. Hefei Science Center CAS [2015HSC-UP009]
  6. Fundamental Research Funds for the Central Universities [WK2060190025]

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Modern development of chemical manufacturing requires a substantial reduction in energy consumption and catalyst cost. Sunlight-driven chemical transformation by metal oxides holds great promise for this goal; however, it remains a grand challenge to efficiently couple solar energy into many catalytic reactions. Here we report that defect engineering on oxide catalyst can serve as a versatile approach to bridge light harvesting with surface reactions by ensuring species chemisorption. The chemisorption not only spatially enables the transfer of photoexcited electrons to reaction species, but also alters the form of active species to lower the photon energy requirement for reactions. In a proof of concept, oxygen molecules are activated into superoxide radicals on defect-rich tungsten oxide through visible-near-infrared illumination to trigger organic aerobic couplings of amines to corresponding imines. The excellent efficiency and durability for such a highly important process in chemical transformation can otherwise be virtually impossible to attain by counterpart materials.

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