4.8 Article

Photocatalytic Hydrogen Production on a sp2-Carbon-Linked Covalent Organic Framework

期刊

出版社

WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202208919

关键词

Covalent Organic Frameworks; Gradient Heating; Hydrogen Evolution; Photocatalysis; sp(2) Carbon Linkage

资金

  1. Natural Science Foundation of China [52073119, 62075081, 21774040]

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In this study, a gradient heating strategy was used to synthesize a sp(2)-carbon-linked triazine-based COF, COF-JLU100, which exhibits high crystallinity, large surface area, good stability, and carrier mobility for solar-driven photocatalytic hydrogen evolution. The Pt-doped COF-JLU100 demonstrates a high hydrogen evolution rate of over 100,000 μmol g(-1) h(-1) for water splitting under visible-light illumination (λ>420 nm). It can be prepared by low-cost and easily available monomers and has excellent stability, making it desirable for practical solar-driven hydrogen production.
Two-dimensional covalent organic frameworks (2D-COFs) have emerged as attractive platforms for solar-to-chemical energy conversion. In this study, we have implemented a gradient heating strategy to synthesize a sp(2)-carbon-linked triazine-based COF, COF-JLU100, exhibiting high crystallinity, large surface area, good durability and carrier mobility for solar-driven photocatalytic hydrogen evolution. The Pt-doped COF-JLU100 demonstrated a high hydrogen evolution rate of over 100 000 mu mol g(-1) h(-1) for water splitting under visible-light illumination (lambda>420 nm). Experimental and theoretical studies corroborate that the cyano-vinylene segments in COF-JLU100 extend the pi-delocalization and enable fast charge transfer and separation rates as well as good dispersion in water. Moreover, COF-JLU100 can be prepared by low-cost and easily available monomers and has excellent stability, which is desirable for practical solar-driven hydrogen production.

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