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Coordination environment tuning of nickel sites by oxyanions to optimize methanol electro-oxidation activity

Author

Listed:
  • Shanlin Li

    (The State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences
    University of Chinese Academy of Sciences
    Beijing University of Technology)

  • Ruguang Ma

    (The State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences
    Suzhou University of Science and Technology)

  • Jingcong Hu

    (Beijing University of Technology)

  • Zichuang Li

    (The State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences
    University of Chinese Academy of Sciences)

  • Lijia Liu

    (Western University)

  • Xunlu Wang

    (The State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences
    University of Chinese Academy of Sciences)

  • Yue Lu

    (Beijing University of Technology)

  • George E. Sterbinsky

    (Advanced Photon Source, Argonne National Laboratory)

  • Shuhu Liu

    (Institute of High Energy Physics, Chinese Academy of Sciences)

  • Lei Zheng

    (Institute of High Energy Physics, Chinese Academy of Sciences)

  • Jie Liu

    (The State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences)

  • Danmin Liu

    (Beijing University of Technology)

  • Jiacheng Wang

    (The State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences
    University of Chinese Academy of Sciences
    North China University of Science and Technology)

Abstract

To achieve zero-carbon economy, advanced anode catalysts are desirable for hydrogen production and biomass upgrading powered by renewable energy. Ni-based non-precious electrocatalysts are considered as potential candidates because of intrinsic redox attributes, but in-depth understanding and rational design of Ni site coordination still remain challenging. Here, we perform anodic electrochemical oxidation of Ni-metalloids (NiPx, NiSx, and NiSex) to in-situ construct different oxyanion-coordinated amorphous nickel oxyhydroxides (NiOOH-TOx), among which NiOOH-POx shows optimal local coordination environment and boosts electrocatalytic activity of Ni sites towards selective oxidation of methanol to formate. Experiments and theoretical results demonstrate that NiOOH-POx possesses improved adsorption of OH* and methanol, and favors the formation of CH3O* intermediates. The coordinated phosphate oxyanions effectively tailor the d band center of Ni sites and increases Ni-O covalency, promoting the catalytic activity. This study provides additional insights into modulation of active-center coordination environment via oxyanions for organic molecules transformation.

Suggested Citation

  • Shanlin Li & Ruguang Ma & Jingcong Hu & Zichuang Li & Lijia Liu & Xunlu Wang & Yue Lu & George E. Sterbinsky & Shuhu Liu & Lei Zheng & Jie Liu & Danmin Liu & Jiacheng Wang, 2022. "Coordination environment tuning of nickel sites by oxyanions to optimize methanol electro-oxidation activity," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
  • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-30670-4
    DOI: 10.1038/s41467-022-30670-4
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    References listed on IDEAS

    as
    1. Jumi Bak & Hyung Bae & Sung-Yoon Chung, 2019. "Atomic-scale perturbation of oxygen octahedra via surface ion exchange in perovskite nickelates boosts water oxidation," Nature Communications, Nature, vol. 10(1), pages 1-10, December.
    2. Ning Zhang & Xiaobin Feng & Dewei Rao & Xi Deng & Lejuan Cai & Bocheng Qiu & Ran Long & Yujie Xiong & Yang Lu & Yang Chai, 2020. "Lattice oxygen activation enabled by high-valence metal sites for enhanced water oxidation," Nature Communications, Nature, vol. 11(1), pages 1-11, December.
    3. Xiaopeng Wang & Shibo Xi & Wee Siang Vincent Lee & Pengru Huang & Peng Cui & Lei Zhao & Weichang Hao & Xinsheng Zhao & Zhenbo Wang & Haijun Wu & Hao Wang & Caozheng Diao & Armando Borgna & Yonghua Du , 2020. "Materializing efficient methanol oxidation via electron delocalization in nickel hydroxide nanoribbon," Nature Communications, Nature, vol. 11(1), pages 1-9, December.
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