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

Si Ma; Tianqi Deng; Ziping Li; Zhenwei Zhang; Ji Jia; Gang Wu; Hong Xia; Shuo-Wang Yang; Xiaoming Liu

doi:10.1002/anie.202208919

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

Angew Chem Int Ed Engl. 2022 Oct 17;61(42):e202208919. doi: 10.1002/anie.202208919. Epub 2022 Sep 12.

Authors

Si Ma¹, Tianqi Deng^{2

3}, Ziping Li¹, Zhenwei Zhang¹, Ji Jia^{1

4}, Gang Wu⁵, Hong Xia⁶, Shuo-Wang Yang⁵, Xiaoming Liu¹

Affiliations

¹ College of Chemistry, Jilin University, Changchun, 130012, P.R. China.
² Institute of Advanced Semiconductors & Zhejiang Provincial Key Laboratory of Power Semiconductor Materials and Devices, ZJU-Hangzhou Global Scientific and Technological Innovation Center, Hangzhou, 311200, P.R. China.
³ State Key Laboratory of Silicon Materials & School of Materials Science and Engineering, Zhejiang University, Hangzhou, 310027, P.R. China.
⁴ Department of Biomedical Engineering, Southern University of Science and Technology, Shenzhen, 518055, P.R. China.
⁵ Institute of High Performance Computing, Agency for Science, Technology and Research, 1 Fusionopolis Way, #16-16 Connexis, Singapore, 138632, Singapore.
⁶ State Key Laboratory on Integrated Optoelectronics, College of Electronic Science and Technology, Jilin University, Changchun, 130012, P.R. China.

PMID: 36028615
DOI: 10.1002/anie.202208919

Abstract

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 sp² -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 μmol g^-1 h^-1 for water splitting under visible-light illumination (λ>420 nm). Experimental and theoretical studies corroborate that the cyano-vinylene segments in COF-JLU100 extend the π-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.

Keywords: Covalent Organic Frameworks; Gradient Heating; Hydrogen Evolution; Photocatalysis; sp2 Carbon Linkage.

Abstract

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