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Balancing hydrogen adsorption/desorption by orbital modulation for efficient hydrogen evolution catalysis

Author

Listed:
  • Feng Li

    (Ulsan National Institute of Science and Technology (UNIST))

  • Gao-Feng Han

    (Ulsan National Institute of Science and Technology (UNIST))

  • Hyuk-Jun Noh

    (Ulsan National Institute of Science and Technology (UNIST))

  • Jong-Pil Jeon

    (Ulsan National Institute of Science and Technology (UNIST))

  • Ishfaq Ahmad

    (Ulsan National Institute of Science and Technology (UNIST))

  • Shanshan Chen

    (Chongqing University
    Ulsan National Institute of Science and Technology (UNIST))

  • Changduk Yang

    (Ulsan National Institute of Science and Technology (UNIST))

  • Yunfei Bu

    (Nanjing University of Information Science and Technology)

  • Zhengping Fu

    (University of Science and Technology of China)

  • Yalin Lu

    (University of Science and Technology of China)

  • Jong-Beom Baek

    (Ulsan National Institute of Science and Technology (UNIST))

Abstract

Hydrogen adsorption/desorption behavior plays a key role in hydrogen evolution reaction (HER) catalysis. The HER reaction rate is a trade-off between hydrogen adsorption and desorption on the catalyst surface. Herein, we report the rational balancing of hydrogen adsorption/desorption by orbital modulation using introduced environmental electronegative carbon/nitrogen (C/N) atoms. Theoretical calculations reveal that the empty d orbitals of iridium (Ir) sites can be reduced by interactions between the environmental electronegative C/N and Ir atoms. This balances the hydrogen adsorption/desorption around the Ir sites, accelerating the related HER process. Remarkably, by anchoring a small amount of Ir nanoparticles (7.16 wt%) in nitrogenated carbon matrixes, the resulting catalyst exhibits significantly enhanced HER performance. This includs the smallest reported overpotential at 10 mA cm−2 (4.5 mV), the highest mass activity at 10 mV (1.12 A mgIr−1) and turnover frequency at 25 mV (4.21 H2 s−1) by far, outperforming Ir nanoparticles and commercial Pt/C.

Suggested Citation

  • Feng Li & Gao-Feng Han & Hyuk-Jun Noh & Jong-Pil Jeon & Ishfaq Ahmad & Shanshan Chen & Changduk Yang & Yunfei Bu & Zhengping Fu & Yalin Lu & Jong-Beom Baek, 2019. "Balancing hydrogen adsorption/desorption by orbital modulation for efficient hydrogen evolution catalysis," Nature Communications, Nature, vol. 10(1), pages 1-7, December.
    • Handle: RePEc:nat:natcom:v:10:y:2019:i:1:d:10.1038_s41467-019-12012-z
    DOI: 10.1038/s41467-019-12012-z
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    Cited by:

    1. Hao Tan & Bing Tang & Ying Lu & Qianqian Ji & Liyang Lv & Hengli Duan & Na Li & Yao Wang & Sihua Feng & Zhi Li & Chao Wang & Fengchun Hu & Zhihu Sun & Wensheng Yan, 2022. "Engineering a local acid-like environment in alkaline medium for efficient hydrogen evolution reaction," Nature Communications, Nature, vol. 13(1), pages 1-9, December.

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