In situ tuning of electronic structure of catalysts using controllable hydrogen spillover for enhanced selectivity

Mi Xiong, Zhe Gao (), Peng Zhao, Guofu Wang, Wenjun Yan, Shuangfeng Xing, Pengfei Wang, Jingyuan Ma, Zheng Jiang, Xingchen Liu, Jiping Ma, Jie Xu and Yong Qin ()
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Mi Xiong: Chinese Academy of Sciences
Zhe Gao: Chinese Academy of Sciences
Peng Zhao: Chinese Academy of Sciences
Guofu Wang: Chinese Academy of Sciences
Wenjun Yan: Chinese Academy of Sciences
Shuangfeng Xing: Chinese Academy of Sciences
Pengfei Wang: Chinese Academy of Sciences
Jingyuan Ma: Chinese Academy of Sciences
Zheng Jiang: Chinese Academy of Sciences
Xingchen Liu: Chinese Academy of Sciences
Jiping Ma: Chinese Academy of Sciences
Jie Xu: Chinese Academy of Sciences
Yong Qin: Chinese Academy of Sciences

Nature Communications, 2020, vol. 11, issue 1, 1-10

Abstract: Abstract In situ tuning of the electronic structure of active sites is a long-standing challenge. Herein, we propose a strategy by controlling the hydrogen spillover distance to in situ tune the electronic structure. The strategy is demonstrated to be feasible with the assistance of CoOx/Al2O3/Pt catalysts prepared by atomic layer deposition in which CoOx and Pt nanoparticles are separated by hollow Al2O3 nanotubes. The strength of hydrogen spillover from Pt to CoOx can be precisely tailored by varying the Al2O3 thickness. Using CoOx/Al2O3 catalyzed styrene epoxidation as an example, the CoOx/Al2O3/Pt with 7 nm Al2O3 layer exhibits greatly enhanced selectivity (from 74.3% to 94.8%) when H2 is added. The enhanced selectivity is attributed to the introduction of controllable hydrogen spillover, resulting in the reduction of CoOx during the reaction. Our method is also effective for the epoxidation of styrene derivatives. We anticipate this method is a general strategy for other reactions.

Date: 2020
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DOI: 10.1038/s41467-020-18567-6

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