Tuning crystal-phase of bimetallic single-nanoparticle for catalytic hydrogenation

Shuang Liu, Yong Li (), Xiaojuan Yu, Shaobo Han, Yan Zhou, Yuqi Yang, Hao Zhang, Zheng Jiang (), Chuwei Zhu, Wei-Xue Li, Christof Wöll, Yuemin Wang () and Wenjie Shen ()
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Shuang Liu: Chinese Academy of Sciences
Yong Li: Chinese Academy of Sciences
Xiaojuan Yu: Karlsruhe Institute of Technology
Shaobo Han: Chinese Academy of Sciences
Yan Zhou: Chinese Academy of Sciences
Yuqi Yang: Chinese Academy of Sciences
Hao Zhang: Chinese Academy of Sciences
Zheng Jiang: Chinese Academy of Sciences
Chuwei Zhu: University of Science and Technology of China
Wei-Xue Li: University of Science and Technology of China
Christof Wöll: Karlsruhe Institute of Technology
Yuemin Wang: Karlsruhe Institute of Technology
Wenjie Shen: Chinese Academy of Sciences

Nature Communications, 2022, vol. 13, issue 1, 1-10

Abstract: Abstract Bimetallic nanoparticles afford geometric variation and electron redistribution via strong metal-metal interactions that substantially promote the activity and selectivity in catalysis. Quantitatively describing the atomic configuration of the catalytically active sites, however, is experimentally challenged by the averaging ensemble effect that is caused by the interplay between particle size and crystal-phase at elevated temperatures and under reactive gases. Here, we report that the intrinsic activity of the body-centered cubic PdCu nanoparticle, for acetylene hydrogenation, is one order of magnitude greater than that of the face-centered cubic one. This finding is based on precisely identifying the atomic structures of the active sites over the same-sized but crystal-phase-varied single-particles. The densely-populated Pd-Cu bond on the chemically ordered nanoparticle possesses isolated Pd site with a lower coordination number and a high-lying valence d-band center, and thus greatly expedites the dissociation of H2 over Pd atom and efficiently accommodates the activated H atoms on the particle top/subsurfaces.

Date: 2022
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DOI: 10.1038/s41467-022-32274-4

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