Zhang Jin, Chen Jinwei, Wan Yingfei, Liu Hongwei, Chen Wang, Wang Gang, Wang Ruilin
College of Materials Science and Engineering, Sichuan University, Chengdu 610065, China.
ACS Appl Mater Interfaces. 2020 Mar 25;12(12):13805-13812. doi: 10.1021/acsami.9b21115. Epub 2020 Mar 13.
Defect modulation usually has a great influence on the electronic structures and activities of photocatalysts. Here, atomically layered g-CN modified via defect engineering with nitrogen vacancy and cyanogen groups is obtained through two facile steps of thermal treatment (denoted as A-V-g-CN). Detailed analysis reveals that the atomic-layered graphitic carbon nitride (2.3 nm) with defect engineering modifying provides more active sites and decreases the electron/hole transferring distances. More importantly, the defects that contain nitrogen vacancies and cyanogen groups extend the responsive wavelength to 650 nm, which effectively suppresses the quantum size effect of atomic-layered g-CN. Therefore, the as-obtained A-V-g-CN exhibited a photocatalytic H evolution rate and apparent quantum yield of 3.7 mmol·g·h and 14.98% (λ > 420 nm), respectively. This work is expected to provide guidance for the rational design of atomic-layered g-CN.
缺陷调控通常对光催化剂的电子结构和活性有很大影响。在此，通过两步简便的热处理步骤获得了经氮空位和氰基缺陷工程修饰的原子层状g-CN（表示为A-V-g-CN）。详细分析表明，经缺陷工程修饰的原子层状石墨相氮化碳（2.3纳米）提供了更多活性位点并缩短了电子/空穴转移距离。更重要的是，含有氮空位和氰基的缺陷将响应波长扩展至650纳米，这有效地抑制了原子层状g-CN的量子尺寸效应。因此，所制备的A-V-g-CN的光催化析氢速率和表观量子产率分别为3.7 mmol·g·h和14.98%（λ>420纳米）。这项工作有望为原子层状g-CN的合理设计提供指导。
