光催化
还原(数学)
共价键
共价有机骨架
化学
金属有机骨架
电荷(物理)
化学工程
光化学
材料科学
催化作用
有机化学
吸附
物理
工程类
几何学
数学
量子力学
作者
Shouxin Zhang,Yuemeng Liu,Hangshuai Li,Guoyi Bai,Xingwang Lan
标识
DOI:10.1016/j.cej.2024.151479
摘要
Covalent organic frameworks (COFs) engineered by single-atom sites have attracted significant attention for CO2 photoreduction. However, precisely manipulating the chemical environment of active sites on the COFs is a grand challenge. Herein, we synthesized a series of isostructural COFs for photocatalytic CO2 reduction, where the strong coordination conformation guides atomically dispersed metal sites to chelate spontaneously in the predesigned imine-pyridine position of COFs. Experimental and theoretical results revealed the crucial influence of the single-Ni site engineering and electronic structures of COF configuration on improving extended π-conjugation, exciton dissociation, charge separation efficiency, and charge carrier migration. Benefiting from the synergistic effect, the optimal Ni-TAPT-COF exhibited a record-high CO production rate of 25.5 mmol g−1h−1 and a selectivity of 98.8 %, even natural-sunlight-driven diluted CO2 (10 %). This work paves the way for the rational design of high-performance COF-based photocatalysts at the molecular level, highlighting their practical potential for CO2 photoreduction.
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