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ACS Appl Mater Interfaces. 2018 Apr 25;10(16):13462-13469. doi: 10.1021/acsami.8b00350. Epub 2018 Apr 12.

Dual-Excitation Polyoxometalate-Based Frameworks for One-Pot Light-Driven Hydrogen Evolution and Oxidative Dehydrogenation.

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Chemical School of Zhang Dayu State Key Laboratory of Fine Chemicals , Dalian University of Technology , Dalian 116024 , China.
Collaborative Innovation Center of Chemical Science and Engineering , Tianjin 300071 , China.


Dehydrogenation of the tetrahydroisoquinoline derivatives coupled with hydrogen production is important for hydrogen storage applications. Herein, we formulated a new system that embedded Dawson-type polyoxometalates as efficient photosensitizers into the pores of redox-active coordination polymers for the light-driven photocatalytic oxidative Mannich reaction and hydrogen evolution. In the designed Co-POM polymer, UV light excitation gives the excited state of the Dawson-type polyoxometalate first to oxidize electron donors or substrates; the reduced form (i.e., heteropolyblue) adsorbs visible light to achieve a new excited state, which reduced the cobalt redox sites and facilitates hydrogen evolution reaction. The photosensitizer recovered to the ground state, completing the catalytic cycle. Under the optimized conditions, Co-POM enabled the hydrogen evolution and dehydrogenation of tetrahydroisoquinoline without the presence of any other additives. The high catalytic efficiency and robustness indicated the advantages of the combining functional polyoxometalate-based catalysts and porous characters of the coordination polymers for the development of highly active heterogeneous catalysts.


dehydrogenation; electron transfer; hydrogen evolution; metal−organic framework; photocatalysis; polyoxometalate


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