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

Author

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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)

  • De Chen

    (Norwegian University of Science and Technology)

  • Ying Wan

    (Shanghai Normal University)

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.

Suggested Citation

  • Xiaojuan Zhu & Qishui Guo & Yafei Sun & Shangjun Chen & Jian-Qiang Wang & Mengmeng Wu & Wenzhao Fu & Yanqiang Tang & Xuezhi Duan & De Chen & Ying Wan, 2019. "Optimising surface d charge of AuPd nanoalloy catalysts for enhanced catalytic activity," Nature Communications, Nature, vol. 10(1), pages 1-11, December.
    • Handle: RePEc:nat:natcom:v:10:y:2019:i:1:d:10.1038_s41467-019-09421-5
    DOI: 10.1038/s41467-019-09421-5
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    Cited by:

    1. Xiaohui Zhang & Zhihu Sun & Rui Jin & Chuwei Zhu & Chuanlin Zhao & Yue Lin & Qiaoqiao Guan & Lina Cao & Hengwei Wang & Shang Li & Hancheng Yu & Xinyu Liu & Leilei Wang & Shiqiang Wei & Wei-Xue Li & Ju, 2023. "Conjugated dual size effect of core-shell particles synergizes bimetallic catalysis," Nature Communications, Nature, vol. 14(1), pages 1-13, December.
    2. Yueshan Xu & Daoxiong Wu & Qinghua Zhang & Peng Rao & Peilin Deng & Mangen Tang & Jing Li & Yingjie Hua & Chongtai Wang & Shengkui Zhong & Chunman Jia & Zhongxin Liu & Yijun Shen & Lin Gu & Xinlong Ti, 2024. "Regulating Au coverage for the direct oxidation of methane to methanol," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    3. Yang Yang & Xiaojuan Zhu & Lili Wang & Junyu Lang & Guohua Yao & Tian Qin & Zhouhong Ren & Liwei Chen & Xi Liu & Wei Li & Ying Wan, 2022. "Breaking scaling relationships in alkynol semi-hydrogenation by manipulating interstitial atoms in Pd with d-electron gain," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    4. Xiaorui Zhao & Xiaojuan Zhu & Kang Wang & Junqian Lv & Shangjun Chen & Guohua Yao & Junyu Lang & Fei Lv & Yinghui Pu & Ruoou Yang & Bingsen Zhang & Zheng Jiang & Ying Wan, 2022. "Palladium catalyzed radical relay for the oxidative cross-coupling of quinolines," Nature Communications, Nature, vol. 13(1), pages 1-11, December.

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