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<p>The H<sub>2</sub>-evolution kinetics play a pivotal role in governing the photocatalytic hydrogen-evolution process. However, achieving precise regulation of the H-adsorption and H-desorption equilibrium (H<sub>ads</sub>/H<sub>des</sub>) still remains a great challenge. Herein, we propose a fine-tuning <i>d</i>-<i>p</i> hybridization strategy to precisely optimize the H<sub>ads</sub>/H<sub>des</sub> kinetics in a Ni-B<sub><i>x</i></sub> modified CdS photocatalyst (Ni-B<sub><i>x</i></sub>/CdS). X-ray absorption fine-structure spectroscopy and theoretical calculations reveal that increasing B-atom amount in the Ni-B<sub><i>x</i></sub> cocatalyst gradually strengthens the <i>d</i>-<i>p</i> orbital interaction between Ni<sub>3<i>d</i></sub> and B<sub>2<i>p</i></sub>, resulting in a consecutive <i>d</i>-band broadening and controllable <i>d</i>-band center on Ni active sites. The above consecutive <i>d</i>-band optimization allows for precise modulation of the H<sub>ads</sub>/H<sub>des</sub> dynamics in the Ni-B<sub><i>x</i></sub>/CdS, ultimately demonstrating a remarkable H<sub>2</sub>-evolution activity of 13.4 mmol g<sup>-1</sup> h<sup>-1</sup> (AQE = 56.1 %). The femtosecond transient absorption spectroscopy further confirms the rapid electron-transfer dynamics in the Ni-B<sub><i>x</i></sub>/CdS photocatalyst. This work provides insights into the optimal design of prospective H<sub>2</sub>-evolution catalysts.</p>

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Fine-tuning d-p hybridization in Ni-Bx cocatalyst for enhanced photocatalytic H2 production

  • 期刊论文

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  • 发表日期：

    2025年1月22日

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  • Haoyu Long,
  • Xidong Zhang,
  • Zhenyi Zhang,
  • Jianjun Zhang,
  • Jiaguo Yu,
  • Huogen Yu

摘要

The H2-evolution kinetics play a pivotal role in governing the photocatalytic hydrogen-evolution process. However, achieving precise regulation of the H-adsorption and H-desorption equilibrium (Hads/Hdes) still remains a great challenge. Herein, we propose a fine-tuning d-p hybridization strategy to precisely optimize the Hads/Hdes kinetics in a Ni-Bx modified CdS photocatalyst (Ni-Bx/CdS). X-ray absorption fine-structure spectroscopy and theoretical calculations reveal that increasing B-atom amount in the Ni-Bx cocatalyst gradually strengthens the d-p orbital interaction between Ni3d and B2p, resulting in a consecutive d-band broadening and controllable d-band center on Ni active sites. The above consecutive d-band optimization allows for precise modulation of the Hads/Hdes dynamics in the Ni-Bx/CdS, ultimately demonstrating a remarkable H2-evolution activity of 13.4 mmol g-1 h-1 (AQE = 56.1 %). The femtosecond transient absorption spectroscopy further confirms the rapid electron-transfer dynamics in the Ni-Bx/CdS photocatalyst. This work provides insights into the optimal design of prospective H2-evolution catalysts.