Metal/oxide interfacial effects on the selective oxidation of primary alcohols

Guofeng Zhao, Fan Yang, Zongjia Chen, Qingfei Liu, Yongjun Ji, Yi Zhang, Zhiqiang Niu (), Junjie Mao, Xinhe Bao, Peijun Hu and Yadong Li ()
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Guofeng Zhao: Tsinghua University
Fan Yang: State Key Laboratory of Catalysis, CAS Center for Excellence in Nanoscience, Dalian Institute of Chemical Physics, Chinese Academy of Sciences
Zongjia Chen: Key Laboratory for Advanced Materials, Center for Computational Chemistry and Research Institute of Industrial Catalysis, East China University of Science and Technology
Qingfei Liu: State Key Laboratory of Catalysis, CAS Center for Excellence in Nanoscience, Dalian Institute of Chemical Physics, Chinese Academy of Sciences
Yongjun Ji: Tsinghua University
Yi Zhang: State Key Laboratory of Catalysis, CAS Center for Excellence in Nanoscience, Dalian Institute of Chemical Physics, Chinese Academy of Sciences
Zhiqiang Niu: Tsinghua University
Junjie Mao: Tsinghua University
Xinhe Bao: State Key Laboratory of Catalysis, CAS Center for Excellence in Nanoscience, Dalian Institute of Chemical Physics, Chinese Academy of Sciences
Peijun Hu: Key Laboratory for Advanced Materials, Center for Computational Chemistry and Research Institute of Industrial Catalysis, East China University of Science and Technology
Yadong Li: Tsinghua University

Nature Communications, 2017, vol. 8, issue 1, 1-8

Abstract: Abstract A main obstacle in the rational development of heterogeneous catalysts is the difficulty in identifying active sites. Here we show metal/oxide interfacial sites are highly active for the oxidation of benzyl alcohol and other industrially important primary alcohols on a range of metals and oxides combinations. Scanning tunnelling microscopy together with density functional theory calculations on FeO/Pt(111) reveals that benzyl alcohol enriches preferentially at the oxygen-terminated FeO/Pt(111) interface and undergoes readily O–H and C–H dissociations with the aid of interfacial oxygen, which is also validated in the model study of Cu2O/Ag(111). We demonstrate that the interfacial effects are independent of metal or oxide sizes and the way by which the interfaces were constructed. It inspires us to inversely support nano-oxides on micro-metals to make the structure more stable against sintering while the number of active sites is not sacrificed. The catalyst lifetime, by taking the inverse design, is thereby significantly prolonged.

Date: 2017
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DOI: 10.1038/ncomms14039

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