Xing Weinan, Shao Weifan, Li Yingfu, Lin Huage, Han Jiangang, Zou Luyi, Jia Ran, Wu Guangyu
College of Ecology and Environment, Co-Innovation Center for the Sustainable Forestry in Southern China, Nanjing Forestry University, Nanjing, 210037, P. R. China.
Department of Chemical and Biomolecular Engineering, National University of Singapore, Engineering Drive 4, Singapore, 117585, Singapore.
Small. 2025 Mar;21(10):e2412036. doi: 10.1002/smll.202412036. Epub 2025 Jan 23.
Constructing heterojunctions between phase interfaces represents a crucial strategy for achieving excellent photocatalytic performance, but the absence of sufficient interface driving force and limited charge transfer pathway leads to unsatisfactory charge separation processes. Herein, a doping-engineering strategy is introduced to construct a In─N bond-bridged InS nanocluster modified S doped carbon nitride (CN) nanosheets Z-Scheme van der Waals (VDW) heterojunctions (InS/CNS) photocatalyst, and the preparation process just by one-step pyrolysis using the pre-coordination confinement method. Specifically, S atoms doping enhances the bond strength of In─N and forms high-quality interfacial In─N linkage which serves as the atomic-level interfacial "highway" for improving the interfacial electrons migration, decreasing the charge recombination probability. The detailed characterization results, along with theoretical calculations, confirm that both S atom incorporation and the formation of Z-Scheme VDW heterojunctions synergistically improve the internal electric field. This, in turn, accelerates charge separation and simultaneously enhances light absorption capacity. Consequently, the optimal hydrogen evolution performance of In₂S₃/CNS2 is 160.8 times greater than that of In₂S₃, 8.2 times higher than that of CNS. This study emphasizes the crucial role of atomic-scale interface regulation and intrinsic electric fields in Z-Scheme VDW heterojunctions, contributing to ameliorative photocatalytic performance.
在相界面之间构建异质结是实现优异光催化性能的关键策略，但缺乏足够的界面驱动力和有限的电荷转移途径会导致电荷分离过程不尽人意。在此，引入一种掺杂工程策略来构建一种由In─N键桥接的InS纳米团簇修饰的S掺杂氮化碳（CN）纳米片Z型范德华（VDW）异质结（InS/CNS）光催化剂，其制备过程仅通过一步热解采用预配位限域法。具体而言，S原子掺杂增强了In─N的键强度并形成高质量的界面In─N键，该键作为原子级界面“高速公路”用于改善界面电子迁移，降低电荷复合概率。详细的表征结果以及理论计算证实，S原子掺入和Z型VDW异质结的形成协同改善了内部电场。这反过来加速了电荷分离并同时增强了光吸收能力。因此，In₂S₃/CNS2的最佳析氢性能比In₂S₃高160.8倍，比CNS高8.2倍。本研究强调了原子尺度界面调控和固有电场在Z型VDW异质结中的关键作用，有助于改善光催化性能。
