Oxide Defect Engineering Enables to Couple Solar Energy into Oxygen Activation

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• 作者：Ning Zhang ; Xiyu Li ; Huacheng Ye ; Shuangming Chen ; Huanxin Ju ; Daobin Liu ; Yue Lin ; Wei Ye ; Chengming Wang ; Qian Xu ; Junfa Zhu ; Li Song ; Jun Jiang ; Yujie Xiong
• 刊名：Journal of the American Chemical Society
• 出版年：2016
• 出版时间：July 20, 2016
• 年：2016
• 卷：138
• 期：28
• 页码：8928-8935
• 全文大小：576K
• 年卷期：0
• ISSN：1520-5126

文摘

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.