Optimising surface d charge of AuPd nanoalloy catalysts for enhanced catalytic activity

Xiaojuan Zhu, Qishui Guo, Yafei Sun, Shangjun Chen, Jian-Qiang Wang, Mengmeng Wu, Wenzhao Fu, Yanqiang Tang, Xuezhi Duan, Chen De and Ying Wan ()
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Xiaojuan Zhu: Shanghai Normal University
Qishui Guo: Shanghai Normal University
Yafei Sun: Shanghai Normal University
Shangjun Chen: Shanghai Normal University
Jian-Qiang Wang: Chinese Academy of Sciences
Mengmeng Wu: Shanghai Normal University
Wenzhao Fu: East China University of Science and Technology
Yanqiang Tang: East China University of Science and Technology
Xuezhi Duan: East China University of Science and Technology
Chen De: Norwegian University of Science and Technology
Ying Wan: Shanghai Normal University

Nature Communications, 2019, vol. 10, issue 1, 1-11

Abstract: Abstract 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.

Date: 2019
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DOI: 10.1038/s41467-019-09421-5

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