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<p>The rational design of co-catalysts with broad spectral response and efficient charge separation remains a critical challenge in photocatalysis. In this study, we propose a dual-functional modification strategy integrating defect engineering and transition metal cluster anchoring to construct a high-performance ACNNS/Ni composite. Ultrathin g-C<sub>3</sub>N<sub>4</sub> nanosheets (CNNS) were first etched with NH<sub>4</sub>F to create surface defects, serving as anchoring sites for uniformly dispersing Ni clusters. These defects not only enhanced intrinsic photocatalytic activity but also enabled stable Ni cluster loading, forming a Schottky barrier at the Ni/g-C<sub>3</sub>N<sub>4</sub> interface to facilitate electron transfer and suppress recombination. The optimized ACNNS/Ni exhibited a narrowed bandgap (2.37 eV vs. 2.65 eV for pristine CNNS), extended visible-light absorption to 477 nm, and achieved a remarkable hydrogen evolution rate of&#xa0;2.85 mmol/(g&#xa0;h)&#xa0;under simulated sunlight—5.82 times higher&#xa0;than pure CNNS. Notably, the defect-rich structure and Ni clusters synergistically improved charge separation efficiency, as evidenced by a&#xa0;12-fold increase&#xa0;in photocurrent density and reduced charge transfer resistance. Furthermore, cyclic tests confirmed robust stability, retaining 82% activity after five cycles. This work highlights the significance of “defect engineering-metal cluster anchoring” in tailoring heterojunction systems, offering a universal pathway for developing transition metal-modified 2D photocatalysts with broad spectral utilization and high quantum efficiency.</p>

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Defect-engineered ultrathin g-C3N4 nanosheets anchored with nickel clusters via dual-functional modification for synergistically enhanced photocatalytic hydrogen evolution

  • 期刊论文

  • 发表日期：

    2025年6月26日

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  • Yinghan Cao,
  • Dongmei Yang,
  • Yuhao Wang,
  • Fengda Xiang,
  • Jingtong Han,
  • Pengcheng Wu,
  • Keliang Wu

摘要

The rational design of co-catalysts with broad spectral response and efficient charge separation remains a critical challenge in photocatalysis. In this study, we propose a dual-functional modification strategy integrating defect engineering and transition metal cluster anchoring to construct a high-performance ACNNS/Ni composite. Ultrathin g-C3N4 nanosheets (CNNS) were first etched with NH4F to create surface defects, serving as anchoring sites for uniformly dispersing Ni clusters. These defects not only enhanced intrinsic photocatalytic activity but also enabled stable Ni cluster loading, forming a Schottky barrier at the Ni/g-C3N4 interface to facilitate electron transfer and suppress recombination. The optimized ACNNS/Ni exhibited a narrowed bandgap (2.37 eV vs. 2.65 eV for pristine CNNS), extended visible-light absorption to 477 nm, and achieved a remarkable hydrogen evolution rate of 2.85 mmol/(g h) under simulated sunlight—5.82 times higher than pure CNNS. Notably, the defect-rich structure and Ni clusters synergistically improved charge separation efficiency, as evidenced by a 12-fold increase in photocurrent density and reduced charge transfer resistance. Furthermore, cyclic tests confirmed robust stability, retaining 82% activity after five cycles. This work highlights the significance of “defect engineering-metal cluster anchoring” in tailoring heterojunction systems, offering a universal pathway for developing transition metal-modified 2D photocatalysts with broad spectral utilization and high quantum efficiency.