Journal
CHEMICAL ENGINEERING JOURNAL
Volume 442, Issue -, Pages -Publisher
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2022.136157
Keywords
Reduction-oxidation cluster -based compounds; Copper (I) photocatalyst; Polyoxometalate; Artificial photosynthesis; Photocatalytic reaction
Categories
Funding
- NSFC [92061101, 21871141, 21871142, 22071109, 51778142]
- China Civil Aviation Science and Technology Innovation Fund [MHRD20140215]
- Excellent Youth Foundation and Distinguished Youth Foundation of Jiangsu Province Natural Science Foundation [BK20211593]
- GuangDong Basic and Applied Basic Research Foundation [2021A1515110429]
- Priority Academic Program Development of Jiangsu Higher Education Institutions
- Foundation of Jiangsu Collaborative Innovation Center of Biomedical Functional Materials
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In this study, a crystalline overall reaction catalyst, RO-4, is constructed to achieve efficient artificial photosynthesis for CO2 conversion. The catalyst allows easy transfer of photogenerated electrons between redox clusters, leading to high CO production activity and O2 release. The research uncovers the related reaction intermediates and CO2 photoreduction mechanism.
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 {PMo(8)V6O42} 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 mu mol g (-1)h(-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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