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Orbital coupling of hetero-diatomic nickel-iron site for bifunctional electrocatalysis of CO2 reduction and oxygen evolution

Author

Listed:
  • Zhiping Zeng

    (Sun Yat-sen University
    Nanyang Technological University)

  • Li Yong Gan

    (Chongqing University)

  • Hong Yang

    (Suzhou University of Science and Technology)

  • Xiaozhi Su

    (CAS)

  • Jiajian Gao

    (Nanyang Technological University)

  • Wei Liu

    (Dalian Institute of Chemical Physics, Chinese Academy of Sciences)

  • Hiroaki Matsumoto

    (Hitachi High-Technologies (Shanghai) Co. Ltd.)

  • Jun Gong

    (Nanyang Technological University)

  • Junming Zhang

    (Nanyang Technological University)

  • Weizhen Cai

    (Nanyang Technological University)

  • Zheye Zhang

    (Nanyang Technological University)

  • Yibo Yan

    (Northwestern Polytechnical University)

  • Bin Liu

    (Nanyang Technological University)

  • Peng Chen

    (Nanyang Technological University)

Abstract

While inheriting the exceptional merits of single atom catalysts, diatomic site catalysts (DASCs) utilize two adjacent atomic metal species for their complementary functionalities and synergistic actions. Herein, a DASC consisting of nickel-iron hetero-diatomic pairs anchored on nitrogen-doped graphene is synthesized. It exhibits extraordinary electrocatalytic activities and stability for both CO2 reduction reaction (CO2RR) and oxygen evolution reaction (OER). Furthermore, the rechargeable Zn-CO2 battery equipped with such bifunctional catalyst shows high Faradaic efficiency and outstanding rechargeability. The in-depth experimental and theoretical analyses reveal the orbital coupling between the catalytic iron center and the adjacent nickel atom, which leads to alteration in orbital energy level, unique electronic states, higher oxidation state of iron, and weakened binding strength to the reaction intermediates, thus boosted CO2RR and OER performance. This work provides critical insights to rational design, working mechanism, and application of hetero-DASCs.

Suggested Citation

  • Zhiping Zeng & Li Yong Gan & Hong Yang & Xiaozhi Su & Jiajian Gao & Wei Liu & Hiroaki Matsumoto & Jun Gong & Junming Zhang & Weizhen Cai & Zheye Zhang & Yibo Yan & Bin Liu & Peng Chen, 2021. "Orbital coupling of hetero-diatomic nickel-iron site for bifunctional electrocatalysis of CO2 reduction and oxygen evolution," Nature Communications, Nature, vol. 12(1), pages 1-11, December.
    • Handle: RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-021-24052-5
    DOI: 10.1038/s41467-021-24052-5
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    Cited by:

    1. Qiyou Wang & Kang Liu & Kangman Hu & Chao Cai & Huangjingwei Li & Hongmei Li & Matias Herran & Ying-Rui Lu & Ting-Shan Chan & Chao Ma & Junwei Fu & Shiguo Zhang & Ying Liang & Emiliano Cortés & Min Li, 2022. "Attenuating metal-substrate conjugation in atomically dispersed nickel catalysts for electroreduction of CO2 to CO," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    2. Xiaoran Zhang & Xiaorong Zhu & Shuowen Bo & Chen Chen & Mengyi Qiu & Xiaoxiao Wei & Nihan He & Chao Xie & Wei Chen & Jianyun Zheng & Pinsong Chen & San Ping Jiang & Yafei Li & Qinghua Liu & Shuangyin , 2022. "Identifying and tailoring C–N coupling site for efficient urea synthesis over diatomic Fe–Ni catalyst," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    3. Yumei Liu & Yun An & Jiexin Zhu & Lujun Zhu & Xiaomei Li & Peng Gao & Guanjie He & Quanquan Pang, 2024. "Integrated energy storage and CO2 conversion using an aqueous battery with tamed asymmetric reactions," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    4. Ying Zang & Di-Qiu Lu & Kun Wang & Bo Li & Peng Peng & Ya-Qian Lan & Shuang-Quan Zang, 2023. "A pyrolysis-free Ni/Fe bimetallic electrocatalyst for overall water splitting," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
    5. Ji Yang & Lu Wang & Jiawei Wan & Farid El Gabaly & Andre L. Fernandes Cauduro & Bernice E. Mills & Jeng-Lung Chen & Liang-Ching Hsu & Daewon Lee & Xiao Zhao & Haimei Zheng & Miquel Salmeron & Caiqi Wa, 2024. "Atomically synergistic Zn-Cr catalyst for iso-stoichiometric co-conversion of ethane and CO2 to ethylene and CO," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    6. Jiannan Du & Guokang Han & Wei Zhang & Lingfeng Li & Yuqi Yan & Yaoxuan Shi & Xue Zhang & Lin Geng & Zhijiang Wang & Yueping Xiong & Geping Yin & Chunyu Du, 2023. "CoIn dual-atom catalyst for hydrogen peroxide production via oxygen reduction reaction in acid," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    7. Shuo Zhang & Jianghua Wu & Mengting Zheng & Xin Jin & Zihan Shen & Zhonghua Li & Yanjun Wang & Quan Wang & Xuebin Wang & Hui Wei & Jiangwei Zhang & Peng Wang & Shanqing Zhang & Liyan Yu & Lifeng Dong , 2023. "Fe/Cu diatomic catalysts for electrochemical nitrate reduction to ammonia," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    8. Yi Wang & Rong Yang & Yajun Ding & Bo Zhang & Hao Li & Bing Bai & Mingrun Li & Yi Cui & Jianping Xiao & Zhong-Shuai Wu, 2023. "Unraveling oxygen vacancy site mechanism of Rh-doped RuO2 catalyst for long-lasting acidic water oxidation," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    9. Yuzhu Zhou & Quan Zhou & Hengjie Liu & Wenjie Xu & Zhouxin Wang & Sicong Qiao & Honghe Ding & Dongliang Chen & Junfa Zhu & Zeming Qi & Xiaojun Wu & Qun He & Li Song, 2023. "Asymmetric dinitrogen-coordinated nickel single-atomic sites for efficient CO2 electroreduction," Nature Communications, Nature, vol. 14(1), pages 1-10, December.

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