物理化学学报 >> 2026, Vol. 42 >> Issue (1): 100154.doi: 10.1016/j.actphy.2025.100154

论文 上一篇    下一篇

自集成黑色NiO团簇与ZnIn2S4微球实现S型电子转移机制下光热辅助制氢

葛成艳1, 胡佳伟2, 刘星雨2, 宋玉玺2, 刘超2,*(), 邹志刚3   

  1. 1 盐城工学院, 化学化工学院, 江苏 盐城 224051
    2 盐城工学院, 材料科学与工程学院, 江苏 盐城 224051
    3 南京大学, 环境材料与再生能源研究中心(ERERC), 江苏 南京 210093
  • 收稿日期:2025-06-29 修回日期:2025-08-04 录用日期:2025-08-07 发布日期:2025-11-01
  • 通讯作者: 刘超, Email: cliu@ycit.edu.cn

Self-integrated black NiO clusters with ZnIn2S4 microspheres for photothermal-assisted hydrogen evolution by S-scheme electron transfer mechanism

Chengyan Ge1, Jiawei Hu2, Xingyu Liu2, Yuxi Song2, Chao Liu2,*(), Zhigang Zou3   

  1. 1 School of Chemistry and Chemical Engineering, Yancheng Institute of Technology, Yancheng 224051, Jiangsu Province, China
    2 School of Materials Science and Engineering, Yancheng Institute of Technology, Yancheng 224051, Jiangsu Province, China
    3 Eco-Materials and Renewable Energy Research Centre (ERERC), Nanjing University, Nanjing 210093, Jiangsu Province, China
  • Received:2025-06-29 Revised:2025-08-04 Accepted:2025-08-07 Published:2025-11-01
  • Contact:

RichHTML

18

PDF

211

赞

摘要：

利用太阳能制氢(H2)技术是实现碳中和目标的关键策略，但是设计最优异质结构光催化剂仍面临重大挑战。本研究首次在溶剂热过程中成功实现了高度分散的黑色NiO团簇与ZIS微球的自组装。所构建的NiO/ZIS S型异质结构复合材料可提供更多活性位点用于可见光驱动光催化产氢(PHE)反应。最优样品2-NiO/ZIS表现出2474.0 μmol g−1 h−1的最佳产氢速率、36.67%的最高表观量子产率(AQY)以及优异的结构稳定性。此外，NiO/ZIS复合材料在天然海水中也展现出高产氢活性。通过原位X射线光电子能谱(XPS)、水相时间分辨光致发光光谱(TRPL)和瞬态吸收光谱(TAS)等先进表征技术，系统评估了催化剂的电荷分离行为。实验分析与理论计算结果共同阐明了NiO/ZIS的S型电荷转移机制。提升的PHE活性源于黑色NiO团簇与ZIS之间的协同效应，包括增强光捕获能力、加速载流子传输与分离、保持高氧化还原能力以及改善表面反应动力学。本研究为构建具有光热效应的S型异质结构复合材料提供了新思路。

关键词: S型异质结, NiO团簇, ZnIn2S4, 光热效应, 产氢

Abstract:

Hydrogen (H2) production technology utilizing solar energy is an essential strategy for questing carbon-neutral, but designing the optimal heterostructured photocatalysts is one of the great challenges. To date, the self-integration of highly-dispersed black NiO clusters with ZIS microspheres was successfully achieved during the solvothermal process. These constructed NiO/ZIS S-scheme heterostructured composites could provide more active for photocatalytic H2 evolution (PHE) under visible light. The optimal 2-NiO/ZIS showed the best PHE rate of 2474.0 μmol g−1 h−1, highest apparent quantum yield (AQY) value of 36.67% and excellent structural stability. Furthermore, NiO/ZIS composites also exhibited the high PHE rates in natural seawater. The charge separation behaviors of the catalyst were systematically evaluated using advanced spectroscopic characterization techniques, specifically in situ XPS, time-resolved photoluminescence (TRPL) tested in water and transient absorption spectroscopy (TAS). The experimental analysis and theoretical calculation results elucidated the S-scheme charge transfer mechanism for NiO/ZIS. The promoted PHE activity was ascribed to the combined effect between black NiO clusters and ZIS, which enhanced light harvesting ability, accelerated charge carrier transportation and separation, remained high redox ability, and improved surface reaction kinetics. This study offers the insights into constructing S-scheme heterostructured composites with photothermal effect.

Key words: S-scheme heterojunction, NiO clusters, ZnIn2S4, Photothermal effect, Hydrogen evolution