Jin Lin, Wei Yajuan, Feng Lanlan, Wang Yuwen, Liu Shuang, Zhang Junwei, Ma Ruoxuan, Shao Xueying, Zhang Xuan, Kong Demeng, Zhao Zibo, Zhang Wei, Liu Jia, Zhang Jingbo
Key Laboratory of Inorganic-Organic Hybrid Functional Material Chemistry, Ministry of Education, Tianjin Key Laboratory of Structure and Performance for Functional Molecules, College of Chemistry, Tianjin Normal University, Tianjin 300387, China.
Key Laboratory of Inorganic-Organic Hybrid Functional Material Chemistry, Ministry of Education, Tianjin Key Laboratory of Structure and Performance for Functional Molecules, College of Chemistry, Tianjin Normal University, Tianjin 300387, China.
J Colloid Interface Sci. 2025 Jan 15;678(Pt C):742-753. doi: 10.1016/j.jcis.2024.09.153. Epub 2024 Sep 16.
The construction of ultra-close 2D atomic-thickness Van der Waals heterojunctions with high-speed charge transfer still faces challenges. Here, we synthesized single-layer ZnInS and g-CN, and introduced silver single atoms to regulate Van der Waals heterojunctions at the atomic level to optimize charge transfer and catalytic activity. At the atomic scale, the impact of detailed structural differences between the two characteristic surfaces of ZnInS ([Zn-S] and [In-S]) on catalytic performance has been first proposed. Experiments combined with the DFT study demonstrate that single atom Ag not only acts as a charge transfer bridge but also regulates the energy band and intrinsic catalytic activity. Benefiting from the enhanced electron delocalization, the synthesized catalyst ZIS/Ag@CN exhibits excellent photocatalytic performance, with a hydrogen production rate of 5.50 mmol·g·h, which is much higher than the reported Ag-based single-atom catalysts so far. This work provides a new understanding of atomic-level heterojunction interface regulation and modification.
构建具有高速电荷转移能力的超紧密二维原子厚度范德华异质结仍面临挑战。在此，我们合成了单层ZnInS和g-CN，并引入银单原子在原子水平上调控范德华异质结，以优化电荷转移和催化活性。在原子尺度上，首次提出了ZnInS两个特征表面（[Zn-S]和[In-S]）之间详细结构差异对催化性能的影响。实验结合DFT研究表明，单原子Ag不仅充当电荷转移桥，还调节能带和本征催化活性。受益于增强的电子离域，合成的催化剂ZIS/Ag@CN表现出优异的光催化性能，产氢速率为5.50 mmol·g·h，远高于迄今为止报道的银基单原子催化剂。这项工作为原子级异质结界面调控和修饰提供了新的认识。
