<p>The development of heterojunction photocatalysts with highly efficient charge separation is essential for achieving solar-driven overall water splitting without sacrificial agents. In this work, a well-defined Type-II TiO<sub>2</sub>/g-C<sub>3</sub>N<sub>4</sub> heterojunction was constructed and co-loaded with Pt nanoparticles and MnOx as hydrogen and oxygen evolution cocatalysts, respectively, forming a Pt-P/CN-MnX composite. The optimized Pt-P/CN-Mn30 sample exhibited broadened visible-light absorption (up to 600 nm) and a notably reduced charge recombination rate. Under the irradiation of simulated sunlight, it achieved a hydrogen evolution rate of 530.6 μmol·g<sup>–1</sup>·h<sup>–1</sup>, 10.3, 5.0 and 2.7 times higher than those of g-C<sub>3</sub>N<sub>4</sub>-Mn3%, P25-Pt2% and P25/CN, respectively, without sacrificial agents. Moreover, the photocatalyst retained over 79.75% of its activity after six cycles, demonstrating excellent stability. Mechanistic analysis revealed efficient spatial charge separation, with electrons transferring from g-C<sub>3</sub>N<sub>4</sub> to TiO<sub>2</sub> and holes migrating toward MnO<sub><i>x</i></sub>. These synergistic effects significantly enhanced redox kinetics. This study presents a novel dual-cocatalyst strategy for multi-interface photocatalysis and provides valuable insights into designing high-performance systems for sustainable water splitting.</p>

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Synergistic Dual-cocatalyst Modified TiO2/g-C3N4 Heterojunctions for Efficient Photocatalytic Overall Water Splitting

  • Shuilian Cheng,
  • Yuxuan Fang,
  • Siyuan Yang,
  • Qiongzhi Gao,
  • Xin Cai,
  • Shengsen Zhang

摘要

The development of heterojunction photocatalysts with highly efficient charge separation is essential for achieving solar-driven overall water splitting without sacrificial agents. In this work, a well-defined Type-II TiO2/g-C3N4 heterojunction was constructed and co-loaded with Pt nanoparticles and MnOx as hydrogen and oxygen evolution cocatalysts, respectively, forming a Pt-P/CN-MnX composite. The optimized Pt-P/CN-Mn30 sample exhibited broadened visible-light absorption (up to 600 nm) and a notably reduced charge recombination rate. Under the irradiation of simulated sunlight, it achieved a hydrogen evolution rate of 530.6 μmol·g–1·h–1, 10.3, 5.0 and 2.7 times higher than those of g-C3N4-Mn3%, P25-Pt2% and P25/CN, respectively, without sacrificial agents. Moreover, the photocatalyst retained over 79.75% of its activity after six cycles, demonstrating excellent stability. Mechanistic analysis revealed efficient spatial charge separation, with electrons transferring from g-C3N4 to TiO2 and holes migrating toward MnOx. These synergistic effects significantly enhanced redox kinetics. This study presents a novel dual-cocatalyst strategy for multi-interface photocatalysis and provides valuable insights into designing high-performance systems for sustainable water splitting.