Journal
JACS AU
Volume 1, Issue 8, Pages 1288-1295Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacsau.1c00186
Keywords
polyoxometalates; crystalline materials; RO cluster-based photocatalysts; CO2 reduction reaction; artificial photosynthesis
Categories
Funding
- NSFC [21622104, 92061101, 21871141, 21871142, 21901122]
- Natural Science Research of Jiangsu Higher Education Institutions of China [19KJB150011]
- China Postdoctoral Science Foundation [2018M630572, 2019M651873]
- Priority Academic Program Development of Jiangsu Higher Education Institutions
- Foundation of Jiangsu Collaborative Innovation Center of Biomedical Functional Materials
- East-West Cooperation Project of Ningxia Key RD Plan [2019BFH02014]
- Postgraduate Research & Practice Innovation Program of Jiangsu Province [KYCX20_1171]
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This study successfully designed and synthesized a novel cluster-based catalyst that can simultaneously photocatalyze CO2 reduction to CO and water oxidation to O2, showing good product selectivity and yield. Density functional theory calculations reveal that catalytically active sites for reduction and oxidation reactions, as well as effective electron transfer between sites, are key factors in achieving artificial photosynthesis.
Metal cluster-based compounds have difficulty finishing the photocatalytic carbon dioxide reduction reaction (CO2RR) and water oxidation reaction (WOR) simultaneously because of the big challenge in realizing the coexistence of independently and synergistically reductive and oxidative active sites in one compound. Herein, we elaborately designed and synthesized one kind of crystalline reduction-oxidation (RO) cluster-based catalysts connecting reductive {M3L8(H2O)(2)} (M = Zn, Co, and Ni for RO-1, 2, 3 respectively) cluster and oxidative {PMo9V7O44} cluster through a single oxygen atom bridge to achieve artificial photosynthesis successfully. These clusters can all photocatalyze CO2-to-CO and H2O-to-O-2 reactions simultaneously, of which the CO yield of RO-1 is 13.8 mu mol/g center dot h, and the selectivity is nearly 100%. Density functional theory calculations reveal that the concomitantly catalytically reductive and oxidative active sites (for CO2RR and WOR, respectively) and the effective electron transfer between the sites in these RO photocatalysts are the key factors to complete the overall photosynthesis.
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