Photocatalytic C–C Coupling from Carbon Dioxide Reduction on Copper Oxide with Mixed-Valence Copper(I)/Copper(II)

光催化 化学 催化作用 咪唑酯 无机化学 氧化物 氧化铜 光化学 价(化学) 二氧化碳电化学还原 一氧化碳 有机化学
作者
Wei Wang,Chaoyuan Deng,Shijie Xie,Yangfan Li,Wanyi Zhang,Hua Sheng,Chuncheng Chen,Jincai Zhao
出处
期刊:Journal of the American Chemical Society [American Chemical Society]
卷期号:143 (7): 2984-2993 被引量:220
标识
DOI:10.1021/jacs.1c00206
摘要

To realize the evolution of C2+ hydrocarbons like C2H4 from CO2 reduction in photocatalytic systems remains a great challenge, owing to the gap between the relatively lower efficiency of multielectron transfer in photocatalysis and the sluggish kinetics of C–C coupling. Herein, with Cu-doped zeolitic imidazolate framework-8 (ZIF-8) as a precursor, a hybrid photocatalyst (CuOX@p-ZnO) with CuOX uniformly dispersed among polycrystalline ZnO was synthesized. Upon illumination, the catalyst exhibited the ability to reduce CO2 to C2H4 with a 32.9% selectivity, and the evolution rate was 2.7 μmol·g–1·h–1 with water as a hole scavenger and as high as 22.3 μmol·g–1·h–1 in the presence of triethylamine as a sacrificial agent, all of which have rarely been achieved in photocatalytic systems. The X-ray absorption fine structure spectra coupled with in situ FT-IR studies reveal that, in the original catalyst, Cu mainly existed in the form of CuO, while a unique Cu+ surface layer upon the CuO matrix was formed during the photocatalytic reaction, and this surface Cu+ site is the active site to anchor the in situ generated CO and further perform C–C coupling to form C2H4. The C–C coupling intermediate *OC–COH was experimentally identified by in situ FT-IR studies for the first time during photocatalytic CO2 reduction. Moreover, theoretical calculations further showed the critical role of such Cu+ sites in strengthening the binding of *CO and stabilizing the C–C coupling intermediate. This work uncovers a new paradigm to achieve the reduction of CO2 to C2+ hydrocarbons in a photocatalytic system.
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