期刊
ACS APPLIED MATERIALS & INTERFACES
卷 14, 期 4, 页码 5194-5202出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.1c18889
关键词
near-infrared; photothermal catalysis; polyoxometalate; carbon dioxide fixation; mild condition
资金
- National Natural Science Foundation of China [91961117]
- Program for JLU Science and Technology Innovative Research Team [2017TD-10]
- Ministry of Science and Higher Education of the Russian Federation [AAAA-A21-121011390008-4]
This study proposes a strategy of incorporating near-infrared photothermal properties into multicomponent catalysts for enhanced conversion of carbon dioxide for cycloaddition reactions. The composite catalysts prepared by electrostatic adsorption of polyoxometalate clusters on polyethyleneimine show excellent catalytic activity and photothermal stability.
Enhanced conversion of carbon dioxide (CO2) for cycloaddition with epoxide derivatives is highly desired in organic synthesis and green chemistry, yet it is still a challenge to obtain satisfactory activity under mild reaction conditions of temperature and pressure. For this purpose, an unexploited strategy is proposed here by incorporating near-infrared (NIR) photothermal properties into multicomponent catalysts. Through the electrostatic adsorption of Co- or Ce-substituted polyoxometalate (POM) clusters on the surface of graphene oxide (GO) with covalently grafted polyethyleneimine (PEI), a series of composite catalysts POMs@ GO-PEI are prepared. The structural and property characterizations demonstrate the synergistic advantages of the catalysts bearing Lewis acids and bases and local NIR photothermal heating from the GO matrix for dramatically enhanced CO2 cycloaddition. Noticeably, while the turnover frequency increases up to 2718 h(-1), the heterogeneous catalysts exhibit photothermal stability and recyclability. With this method, the onsite NIR photothermal transformation becomes extendable to more green reaction processes.
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