氧化还原
人工光合作用
催化作用
光化学
光催化
化学
光合作用
电子转移
反应机理
选择性
析氧
材料科学
作者
Xiaoxin Li,Lei Zhang,Yuan Lin,Tong Wang,Long‐Zhang Dong,Kai Huang,Jiang Liu,Ya‐Qian Lan
标识
DOI:10.1016/j.cej.2022.136157
摘要
Artificial photosynthesis, coupling CO2 photoreduction and water photooxidation reactions, is an important and green means to convert CO2. Compared with traditional multiphasic heterojunctions, monophasic photocatalysts for artificial photosynthesis are still very rare. Here we construct a crystalline overall reaction catalyst, RO-4, by connecting reductive {CuI8} and oxidative {PMo8V6O42} clusters with bridging oxygen atoms, which allow the photogenerated electrons to transfer easily between the redox clusters. Under light irradiation, RO-4 can achieve efficient artificial photosynthesis with a high CO production activity of 20.06 μmol g-1h−1 (>99.5% selectivity) along with O2 release. Furthermore, in situ DRIFTS and DFT calculations uncover the related reaction intermediates and CO2 photoreduction mechanism. This work validates a feasible strategy to engineer monophasic crystalline RO photocatalysts for efficient artificial photosynthetic overall reaction.
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