光催化
催化作用
二氧化碳电化学还原
光化学
化学
分子内力
氧化还原
铼
材料科学
一氧化碳
无机化学
有机化学
作者
Yuan‐Zhe Cheng,Wenyan Ji,Peng‐Yuan Hao,Xue‐Han Qi,Xianxin Wu,Xiaomeng Dou,Xin‐Yue Bian,Di Jiang,Fa‐tang Li,Xinfeng Liu,Donghui Yang,Xuesong Ding,Bao‐Hang Han
标识
DOI:10.1002/anie.202308523
摘要
Abstract Constructing a powerful photocatalytic system that can achieve the carbon dioxide (CO 2 ) reduction half‐reaction and the water (H 2 O) oxidation half‐reaction simultaneously is a very challenging but meaningful task. Herein, a porous material with a crystalline topological network, named viCOF‐bpy‐Re, was rationally synthesized by incorporating rhenium complexes as reductive sites and triazine ring structures as oxidative sites via robust −C=C− bond linkages. The charge‐separation ability of viCOF‐bpy‐Re is promoted by low polarized π‐bridges between rhenium complexes and triazine ring units, and the efficient charge‐separation enables the photogenerated electron–hole pairs, followed by an intramolecular charge‐transfer process, to form photogenerated electrons involved in CO 2 reduction and photogenerated holes that participate in H 2 O oxidation simultaneously. The viCOF‐bpy‐Re shows the highest catalytic photocatalytic carbon monoxide (CO) production rate (190.6 μmol g −1 h −1 with about 100 % selectivity) and oxygen (O 2 ) evolution (90.2 μmol g −1 h −1 ) among all the porous catalysts in CO 2 reduction with H 2 O as sacrificial agents. Therefore, a powerful photocatalytic system was successfully achieved, and this catalytic system exhibited excellent stability in the catalysis process for 50 hours. The structure–function relationship was confirmed by femtosecond transient absorption spectroscopy and density functional theory calculations.
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