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Citation: Weikang Wang,  Yadong Wu,  Jianjun Zhang,  Kai Meng,  Jinhe Li,  Lele Wang,  Qinqin Liu. 三聚氰胺泡沫支撑的S型硫铟锌镉/硫掺杂氮化碳异质结的绿色H2O2合成：协同界面电荷转移调控与局域光热效应[J]. Acta Physico-Chimica Sinica, ;2025, 41(8): 100093. doi: 10.1016/j.actphy.2025.100093 shu

三聚氰胺泡沫支撑的S型硫铟锌镉/硫掺杂氮化碳异质结的绿色H2O2合成：协同界面电荷转移调控与局域光热效应

  • 1.

    School of Materials Science and Engineering, Jiangsu University, Zhenjiang 212013, Jiangsu Province, China;

  • 2.

    Laboratory of Solar Fuel, Faculty of Materials Science and Chemistry, China University of Geosciences, Wuhan 430078, Hubei Province, China;

  • 3.

    State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan 430070, Hubei Province, China

  • Received Date: 13 March 2025
    Revised Date: 1 April 2025
    Accepted Date: 10 April 2025

    Fund Project: This work was supported by the Natural Science Foundation of China (22472069, 22102064, 22302080) and Anhui Key Laboratory of Nanomaterials and Nanotechnology, the Major Science and Technology Projects in Anhui Province (202305a12020006).

  • 绿色光催化合成过氧化氢(H2O2)是替代高能耗蒽醌工艺的理想途径，但其在无牺牲剂体系中受限于快速载流子复合与氧化还原能力不足。本研究报道了一种原位化学浴-水热法制备的三聚氰胺泡沫(MF)负载的硫掺杂氮化碳(SCN)/硫空位修饰硫铟锌镉(CZIS)S型异质结(CZIS/SCN/MF)，用于无牺牲剂H2O2光合成。通过原位辐照X射线光电子能谱(XPS)、自由基捕获电子顺磁共振(EPR)、飞秒瞬态吸收光谱(fs-TA)及理论计算，证实了其S型电荷转移机制。具体而言，硫掺杂可调控氮化碳骨架的局域电荷分布，强化SCN/CZIS异质结界面内建电场；同时，CZIS中煅烧引入的硫空位作为光电子陷阱促进电荷分离，并保留光生空穴用于H2O氧化，从而实现无牺牲剂H2O2合成。结合MF三维多孔框架的光热效应，优化S掺杂浓度和SCN用量的CZIS/SCN/MF催化剂在纯水中H2O2产率达3.46 mmol·g-1·h-1，显著优于多数无牺牲剂体系。该研究为无牺牲剂光催化体系中的界面电荷协同调控与能量转换强化提供了新策略。
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