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Enhancement of CH3CO* adsorption by editing d-orbital states of Pd to boost C-C bond cleavage of ethanol eletrooxidation

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Abstract

Improving the complete ethanol electrooxidation on Pd-based catalysts in alkaline media has drawn widely attention due to the high mass energy density. However, the weak adsorption energy of CH3CO* on Pd restricts the C-C bond cleavage. Inspired by the molecular orbital theory, we proposed the d-state-editing strategy to construct more unoccupied d-states of Pd for the enhanced interaction with CH3CO* to break C-C bonds. As expected, the reduced number of eg electrons and more unoccupied d-states of Pd successfully formed on as-prepared porous RhAu-PdCu nanosheets (PNSs). Theoretical calculations show that the optimized d-states of RhAu-PdCu PNS can effectively improve the adsorption of CH3CO* and drastically reduce the energy barrier of C-C bond cleavage, thus boosting the complete oxidation of ethanol. The charge ratio of C1 pathway on RhAu-PdCu PNSs is 51.5%, more than 2 times higher than that of Pd NSs. Our finding provides an innovative perspective for the design of highly-efficient noble-based electrocatalysts.

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Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (22209039) and Top-notch Personnel Fund of Henan Agricultural University (30500682).

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Authors and Affiliations

  1. College of Sciences, Henan Agricultural University, Zhengzhou, 450000, China

    Yuchen Qin, Fengqi Wang, Pei Liu, Guangce Jiang, Lijie Liu, Xiaobiao Liu, Xin Zheng & Yunlai Ren

  2. Tianjin Key Laboratory of Molecular Optoelectronic Sciences, Department of Chemistry, School of Science, Tianjin University & Collaborative Innovation Center of Chemical Science and Engineering, Tianjin, 300072, China

    Junjun Li & Zhicheng Zhang

  3. College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, China

    Jinyu Ye

  4. Department of Analysis, Sinopec Engineering Group Luoyang R&D Center of Technology, Luoyang, 471000, China

    Qian Wang

  5. School of Chemical and Material Engineering, Jiangnan University, Wuxi, 214211, China

    Yao Wang

  6. Shandong Provincial Key Laboratory of Chemical Energy Storage and Novel Cell Technology, Liaocheng University, Liaocheng, 252000, China

    Pengfang Zhang

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  1. Yuchen Qin
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  2. Fengqi Wang
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  10. Xiaobiao Liu
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Correspondence to Yuchen Qin or Zhicheng Zhang.

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Supporting information The supporting information is available online at chem.scichina.com and link.springer.com/journal/11426. The supporting materials are published as submitted, without typesetting or editing. The responsibility for scientific accuracy and content remains entirely with the authors.

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11426_2023_1756_MOESM1_ESM.pdf

Enhancement of CH3CO* Adsorption by Editing d-Orbital States of Pd to Boost C-C Bond Cleavage of Ethanol Eletrooxidation

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Qin, Y., Wang, F., Liu, P. et al. Enhancement of CH3CO* adsorption by editing d-orbital states of Pd to boost C-C bond cleavage of ethanol eletrooxidation. Sci. China Chem. 67, 696–704 (2024). https://doi.org/10.1007/s11426-023-1756-8

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  • DOI: https://doi.org/10.1007/s11426-023-1756-8

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