材料科学
光催化
光诱导电荷分离
光降解
共价键
三嗪
降级(电信)
化学工程
光化学
纳米技术
催化作用
化学
有机化学
工程类
高分子化学
人工光合作用
电信
计算机科学
作者
J. Chen,G. Li,Na Lü,Hua‐Tay Lin,Shouyong Zhou,Fu Liu
标识
DOI:10.1016/j.mtchem.2022.100832
摘要
Covalent triazine frameworks (CTFs) show great potential in photocatalytic fields, while their practical efficiency is still limited due to rapid charge recombination. Here we report a nanospatial separation strategy for photoinduced electron-hole pairs of CTF-1 nanosheets via single-atom Co using facile pyrolysis and phosphorization to form stable Co–N3 (≈1.60 Å) architecture. HAADF-STEM image demonstrates Co atoms are uniformly dispersed onto ultrathin CTF-1. The local structure surrounding and chemical valent state of Co are systematically investigated by Fourier-transformed EXAFS and K-edge XANES, respectively. Co single atoms as oxidation centers can capture holes transferred from CTF-1, thus resulting in narrow bandgap and improved photo-exciton dissociation in the two-dimensional (2D) direction. The obtained Co/CTF-1 exhibits excellent efficiency of 99.9% for pollutant photodegradation, far outperforming that of pristine CTF-1 (68.8%). Nanospatial separation endows Co/CTF-1 with various micropollution removal capabilities, outstanding cyclic stability, and a widely effective pH range (1.0–11.0) under visible light. Furthermore, active oxidating radicals of h+ and •O2− are dominant in photocatalytic degradation for various organic contaminants. This study motivates the atomic design and fabrication of 2D photocatalysts with excellent charge nanospatial separation.
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