Grafting nanometer metal/oxide interface towards enhanced low-temperature acetylene semi-hydrogenation

Shihui Zou (), Baohui Lou, Kunran Yang, Wentao Yuan, Chongzhi Zhu, Yihan Zhu (), Yonghua Du (), Linfang Lu, Juanjuan Liu, Weixin Huang, Bo Yang (), Zhongmiao Gong, Yi Cui, Yong Wang, Lu Ma, Jingyuan Ma, Zheng Jiang, Liping Xiao and Jie Fan ()
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Shihui Zou: Zhejiang University
Baohui Lou: Zhejiang University
Kunran Yang: ShanghaiTech University
Wentao Yuan: Zhejiang University
Chongzhi Zhu: Zhejiang University of Technology
Yihan Zhu: Zhejiang University of Technology
Yonghua Du: Institute of Chemical and Engineering Sciences, A*STAR
Linfang Lu: Zhejiang University
Juanjuan Liu: Hangzhou Dianzi University
Weixin Huang: University of Science and Technology of China
Bo Yang: ShanghaiTech University
Zhongmiao Gong: Chinese Academy of Sciences
Yi Cui: Chinese Academy of Sciences
Yong Wang: Zhejiang University
Lu Ma: Brookhaven National Laboratory
Jingyuan Ma: Shanghai Institute of Applied Physics Chinese Academy of Sciences
Zheng Jiang: Shanghai Institute of Applied Physics Chinese Academy of Sciences
Liping Xiao: Zhejiang University
Jie Fan: Zhejiang University

Nature Communications, 2021, vol. 12, issue 1, 1-11

Abstract: Abstract Metal/oxide interface is of fundamental significance to heterogeneous catalysis because the seemingly “inert” oxide support can modulate the morphology, atomic and electronic structures of the metal catalyst through the interface. The interfacial effects are well studied over a bulk oxide support but remain elusive for nanometer-sized systems like clusters, arising from the challenges associated with chemical synthesis and structural elucidation of such hybrid clusters. We hereby demonstrate the essential catalytic roles of a nanometer metal/oxide interface constructed by a hybrid Pd/Bi2O3 cluster ensemble, which is fabricated by a facile stepwise photochemical method. The Pd/Bi2O3 cluster, of which the hybrid structure is elucidated by combined electron microscopy and microanalysis, features a small Pd-Pd coordination number and more importantly a Pd-Bi spatial correlation ascribed to the heterografting between Pd and Bi terminated Bi2O3 clusters. The intra-cluster electron transfer towards Pd across the as-formed nanometer metal/oxide interface significantly weakens the ethylene adsorption without compromising the hydrogen activation. As a result, a 91% selectivity of ethylene and 90% conversion of acetylene can be achieved in a front-end hydrogenation process with a temperature as low as 44 °C.

Date: 2021
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DOI: 10.1038/s41467-021-25984-8

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