Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 142, Issue 10, Pages 4862-4871Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.0c00054
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Funding
- Singapore Agency for Science, Technology and Research (A*STAR) AME IRG grant [A1783c0007]
- Singapore National Research Foundation Investigatorship [NRF-NRFI2018-03]
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Covalent organic frameworks (COFs) are excellent platforms with tailored functionalities in photocatalysis. There are still challenges in increasing the photochemical performance of COFs. Therefore, we designed and prepared a series of COFs for photocatalytic hydrogen generation. Varying different ratios of beta-ketoenamine to imine moieties in the linkages could differ the ordered structure, visible light harvesting, and bandgap. Overall, beta-ketoenamine-linked COFs exhibited much better photocatalytic activity than those COFs having both beta-ketoenamine and imine moieties on account of a nonquenched excited state and more favorable HOMO level in the photoinduced oxidation reaction from the former. Specifically, after in situ growth of beta-ketoenamine-linked COFs onto NH2-Ti3C2Tx MXene via covalent connection, the heterohybrid showed an obvious improvement in photocatalytic H-2 evolution because of strong covalent coupling, electrical conductivity, and efficient charge transfer. This integrated linkage evolution and covalent hybridization approach advances the development of COF-based photocatalysts.
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