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

Author

Listed:
  • Mi Xiong

    (Chinese Academy of Sciences
    University of 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
    University of 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
    University of Chinese Academy of Sciences)

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.

Suggested Citation

  • Mi Xiong & Zhe Gao & Peng Zhao & Guofu Wang & Wenjun Yan & Shuangfeng Xing & Pengfei Wang & Jingyuan Ma & Zheng Jiang & Xingchen Liu & Jiping Ma & Jie Xu & Yong Qin, 2020. "In situ tuning of electronic structure of catalysts using controllable hydrogen spillover for enhanced selectivity," Nature Communications, Nature, vol. 11(1), pages 1-10, December.
    • Handle: RePEc:nat:natcom:v:11:y:2020:i:1:d:10.1038_s41467-020-18567-6
    DOI: 10.1038/s41467-020-18567-6
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    Cited by:

    1. Jie Dai & Yinlong Zhu & Yu Chen & Xue Wen & Mingce Long & Xinhao Wu & Zhiwei Hu & Daqin Guan & Xixi Wang & Chuan Zhou & Qian Lin & Yifei Sun & Shih-Chang Weng & Huanting Wang & Wei Zhou & Zongping Sha, 2022. "Hydrogen spillover in complex oxide multifunctional sites improves acidic hydrogen evolution electrocatalysis," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    2. Zhida Gu & Mengke Li & Cheng Chen & Xinglong Zhang & Chengyang Luo & Yutao Yin & Ruifa Su & Suoying Zhang & Yu Shen & Yu Fu & Weina Zhang & Fengwei Huo, 2023. "Water-assisted hydrogen spillover in Pt nanoparticle-based metal–organic framework composites," Nature Communications, Nature, vol. 14(1), pages 1-13, December.

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