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Turning main-group element magnesium into a highly active electrocatalyst for oxygen reduction reaction

Author

Listed:
  • Shuai Liu

    (University of Science and Technology of China)

  • Zedong Li

    (University of Science and Technology of China)

  • Changlai Wang

    (University of Science and Technology of China)

  • Weiwei Tao

    (Boston University)

  • Minxue Huang

    (University of Science and Technology of China)

  • Ming Zuo

    (University of Science and Technology of China)

  • Yang Yang

    (University of Science and Technology of China)

  • Kang Yang

    (University of Science and Technology of China)

  • Lijuan Zhang

    (Shanghai Institute of Applied Physics)

  • Shi Chen

    (University of Science and Technology of China)

  • Pengping Xu

    (University of Science and Technology of China)

  • Qianwang Chen

    (University of Science and Technology of China
    Academy of Sciences)

Abstract

It is known that the main-group metals and their related materials show poor catalytic activity due to a broadened single resonance derived from the interaction of valence orbitals of adsorbates with the broad sp-band of main-group metals. However, Mg cofactors existing in enzymes are extremely active in biochemical reactions. Our density function theory calculations reveal that the catalytic activity of the main-group metals (Mg, Al and Ca) in oxygen reduction reaction is severely hampered by the tight-bonding of active centers with hydroxyl group intermediate, while the Mg atom coordinated to two nitrogen atoms has the near-optimal adsorption strength with intermediate oxygen species by the rise of p-band center position compared to other coordination environments. We experimentally demonstrate that the atomically dispersed Mg cofactors incorporated within graphene framework exhibits a strikingly high half-wave potential of 910 mV in alkaline media, turning a s/p-band metal into a highly active electrocatalyst.

Suggested Citation

  • Shuai Liu & Zedong Li & Changlai Wang & Weiwei Tao & Minxue Huang & Ming Zuo & Yang Yang & Kang Yang & Lijuan Zhang & Shi Chen & Pengping Xu & Qianwang Chen, 2020. "Turning main-group element magnesium into a highly active electrocatalyst for oxygen reduction reaction," Nature Communications, Nature, vol. 11(1), pages 1-11, December.
    • Handle: RePEc:nat:natcom:v:11:y:2020:i:1:d:10.1038_s41467-020-14565-w
    DOI: 10.1038/s41467-020-14565-w
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    Cited by:

    1. Minmin Yan & Zengxi Wei & Zhichao Gong & Bernt Johannessen & Gonglan Ye & Guanchao He & Jingjing Liu & Shuangliang Zhao & Chunyu Cui & Huilong Fei, 2023. "Sb2S3-templated synthesis of sulfur-doped Sb-N-C with hierarchical architecture and high metal loading for H2O2 electrosynthesis," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    2. Xiao Zhou & Yuan Min & Changming Zhao & Cai Chen & Ming-Kun Ke & Shi-Lin Xu & Jie-Jie Chen & Yuen Wu & Han-Qing Yu, 2024. "Constructing sulfur and oxygen super-coordinated main-group electrocatalysts for selective and cumulative H2O2 production," Nature Communications, Nature, vol. 15(1), pages 1-13, December.
    3. Yifan Li & Aijian Huang & Lingxi Zhou & Bohan Li & Muyun Zheng & Zewen Zhuang & Chang Chen & Chen Chen & Feiyu Kang & Ruitao Lv, 2024. "Main-group element-boosted oxygen electrocatalysis of Cu-N-C sites for zinc-air battery with cycling over 5000 h," Nature Communications, Nature, vol. 15(1), pages 1-13, December.
    4. Fenghui Ye & Shishi Zhang & Qingqing Cheng & Yongde Long & Dong Liu & Rajib Paul & Yunming Fang & Yaqiong Su & Liangti Qu & Liming Dai & Chuangang Hu, 2023. "The role of oxygen-vacancy in bifunctional indium oxyhydroxide catalysts for electrochemical coupling of biomass valorization with CO2 conversion," Nature Communications, Nature, vol. 14(1), pages 1-14, December.

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