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Metal/oxide interfacial effects on the selective oxidation of primary alcohols  ( SCI-EXPANDED收录)  

文献类型:期刊文献

英文题名:Metal/oxide interfacial effects on the selective oxidation of primary alcohols

作者:Zhao, Guofeng[1];Yang, Fan[2];Chen, Zongjia[3,4,5];Liu, Qingfei[2,6];Ji, Yongjun[1];Zhang, Yi[2,6];Niu, Zhiqiang[1];Mao, Junjie[1];Bao, Xinhe[2];Hu, Peijun[3,4,5];Li, Yadong[1,7]

机构:[1]Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China;[2]Chinese Acad Sci, Dalian Inst Chem Phys, CAS Ctr Excellence Nanosci, State Key Lab Catalysis, Dalian 116023, Peoples R China;[3]East China Univ Sci & Technol, Ctr Computat Chem, Key Lab Adv Mat, Shanghai 200237, Peoples R China;[4]East China Univ Sci & Technol, Res Inst Ind Catalysis, Shanghai 200237, Peoples R China;[5]Queens Univ Belfast, Sch Chem & Chem Engn, Belfast BT9 5AG, Antrim, North Ireland;[6]Univ Chinese Acad Sci, Beijing 100049, Peoples R China;[7]Tsinghua Univ, Collaborat Innovat Ctr Nanomat Sci & Engn, Beijing 100084, Peoples R China

年份:2017

卷号:8

外文期刊名:NATURE COMMUNICATIONS

收录:;WOS:【SCI-EXPANDED(收录号:WOS:000392155200001)】;

基金:This work was supported by the National Natural Science Foundation of China (21521091, 21131004, 21390393, 21303195, 21473191, U1463202), Ministry of Science and Technology of China (2013CB933100) and Strategic Priority Research Program of the Chinese Academy of Sciences (XDB17020200). We also appreciate Lin Hu, Jinlong Yang, Yanggang Wang and Jun Li for helpful discussions.

语种:英文

摘要: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.

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