Litcius/Paper detail

A Small Organic Molecular Catalyst with Efficient Electron Accumulation for Near‐unity CO<sub>2</sub> Photoreduction

Ting Liu, Li Yang, Youting Fang, Yukang Fu, Longxin Chen, Duobin Chao

2022Chemistry - An Asian Journal11 citationsDOI

Abstract

Abstract Molecular catalysis is of great interest to CO 2 photoreduction. Various transition metal complexes have been developed as efficient molecular catalysts. However, it remains a challenge to catalyze CO 2 reduction by a small organic molecular photocatalyst, as the accumulation of multiple electrons in a small organic molecule is normally difficult for CO 2 reduction. We report herein a small organic molecular catalyst can be used for selective reduction of CO 2 to CO under visible light irradiation. The turnover number (TON) of CO formation is found to be 400±26 with near 100% selectivity in DMF/H 2 O medium. UV‐Vis absorption spectroscopy, density functional theory (DFT) calculations, and spectroelectrochemical studies demonstrate that the organic molecular catalyst is capable of accumulating electrons through a 2e − reduced product which shows good stability and is responsible for interacting with CO 2 . These findings elucidate an accessible way to develop purely organic molecular catalysts for CO 2 reduction by strengthening the electron accumulation.

Topics & Concepts

CatalysisPhotochemistryChemistrySelectivityDensity functional theoryElectronSmall moleculeAbsorption (acoustics)PhotocatalysisMaterials scienceComputational chemistryOrganic chemistryComposite materialBiochemistryPhysicsQuantum mechanicsCO2 Reduction Techniques and CatalystsAdvanced Photocatalysis TechniquesCarbon dioxide utilization in catalysis