文献类型：期刊文献

英文题名：Optimising surface d charge of AuPd nanoalloy catalysts for enhanced catalytic activity

作者：Zhu, Xiaojuan[1,2];Guo, Qishui[1,2];Sun, Yafei[1,2];Chen, Shangjun[1,2];Wang, Jian-Qiang[3];Wu, Mengmeng[1,2];Fu, Wenzhao[4];Tang, Yanqiang[4];Duan, Xuezhi[4];Chen, De[5];Wan, Ying[1,2]

机构：[1]Shanghai Normal Univ, Shanghai Key Lab Rare Earth Funct Mat, Key Lab Resource Chem, Minist Educ, Shanghai 200234, Peoples R China;[2]Shanghai Normal Univ, Dept Chem, Shanghai 200234, Peoples R China;[3]Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai Synchrotron Radiat Facil, Shanghai 201204, Peoples R China;[4]East China Univ Sci & Technol, State Key Lab Chem Engn, Shanghai 200237, Peoples R China;[5]Norwegian Univ Sci & Technol, Dept Chem Engn, N-7491 Trondheim, Norway

年份：2019

卷号：10

外文期刊名：NATURE COMMUNICATIONS

收录：;WOS:【SCI-EXPANDED(收录号:WOS:000462721900027)】；

基金：This work was supported by the National Natural Science Foundation of China (21773156, 21503136), the Ministry of Education of China (PCSIRT_IRT_16R49), the International Joint Laboratory on Resource Chemistry of China (IJLRC), the Shanghai Sci. & Tech. and Edu. Committee (17JC1404200) and the Shanghai Gaofeng & Gaoyuan Project for University Academic Program Development.

语种：英文

摘要：Understanding the catalytic mechanism of bimetallic nanocatalysts remains challenging. Here, we adopt an adsorbate mediated thermal reduction approach to yield monodispersed AuPd catalysts with continuous change of the Pd-Au coordination numbers embedded in a mesoporous carbonaceous matrix. The structure of nanoalloys is well-defined, allowing for a direct determination of the structure-property relationship. The results show that the Pd single atom and dimer are the active sites for the base-free oxidation of primary alcohols. Remarkably, the d-orbital charge on the surface of Pd serves as a descriptor to the adsorbate states and hence the catalytic performance. The maximum d-charge gain occurred in a composition with 33-50 at% Pd corresponds to up to 9 times enhancement in the reaction rate compared to the neat Pd. The findings not only open an avenue towards the rational design of catalysts but also enable the identification of key steps involved in the catalytic reactions.