Wang Tianyu, Pan Xuanlin, He Minyi, Kang Lei, Ma Wangjing
Technical Institute of Physics and Chemistry, Chinese Academy of Sciences, Zhongguancun East Road, Haidian District, Beijing, 100190, China.
University of Chinese Academy of Sciences, Zhongguancun East Road, Haidian District, Beijing, 100049, China.
Adv Sci (Weinh). 2024 Sep;11(33):e2403771. doi: 10.1002/advs.202403771. Epub 2024 Jul 3.
The rational design of visible-light-responsive catalysts is crucial for converting solar energy into hydrogen energy to promote sustainable energy development. In this work, a C─S─C bond is introduced into g-CN (CN) through S doping. With the help of the flexible C─S─C bond under specific stimuli, a hollow coral-like porous structure of S-doped g-CN (S-CN) is synthesized for the first time. And an S-doped g-CN/ZnInS (S-CN/ZIS) heterojunction catalyst is in situ synthesized based on S-CN. S-CN/ZIS exhibits excellent photocatalytic hydrogen evolution (PHE) efficiency (19.25 mmol g h), which is 2.7 times higher than that of the g-CN/ZnInS (CN/ZIS) catalyst (8.46 mmol g h), with a high surface quantum efficiency (AQE) of 34.43% at 420 nm. Experiments and theoretical calculations demonstrate that the excellent photocatalytic performance is attributed to the larger specific surface area and porosity, enhanced interfacial electric field (IEF) effect, and appropriate hydrogen adsorption Gibbs free energy (ΔG). The synergistic effect of S doping and S-scheme heterojunction contributes to the above advancement. This study provides new insights and theoretical basis for the design of CN-based photocatalysts.
可见光响应型催化剂的合理设计对于将太阳能转化为氢能以促进可持续能源发展至关重要。在这项工作中，通过硫掺杂将C─S─C键引入到石墨相氮化碳（g-CN）中。在特定刺激下借助柔性C─S─C键，首次合成了硫掺杂g-CN（S-CN）的中空珊瑚状多孔结构。并基于S-CN原位合成了硫掺杂g-CN/锌铟硫化物（S-CN/ZIS）异质结催化剂。S-CN/ZIS表现出优异的光催化析氢（PHE）效率（19.25 mmol g⁻¹ h⁻¹），比g-CN/锌铟硫化物（CN/ZIS）催化剂（8.46 mmol g⁻¹ h⁻¹）高2.7倍，在420 nm处具有34.43%的高表面量子效率（AQE）。实验和理论计算表明，优异的光催化性能归因于更大的比表面积和孔隙率、增强的界面电场（IEF）效应以及合适的氢吸附吉布斯自由能（ΔG）。硫掺杂和S型异质结的协同效应促成了上述进展。该研究为基于g-CN的光催化剂设计提供了新的见解和理论依据。
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