Ma Si, Deng Tianqi, Li Ziping, Zhang Zhenwei, Jia Ji, Wu Gang, Xia Hong, Yang Shuo-Wang, Liu Xiaoming
College of Chemistry, Jilin University, Changchun, 130012, P.R. China.
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.
Angew Chem Int Ed Engl. 2022 Oct 17;61(42):e202208919. doi: 10.1002/anie.202208919. Epub 2022 Sep 12.
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 -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 h 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.
二维共价有机框架（2D-COFs）已成为太阳能到化学能转换的有吸引力的平台。在本研究中，我们实施了一种梯度加热策略来合成一种sp-碳连接的三嗪基COF，即COF-JLU100，它具有高结晶度、大表面积、良好的耐久性和载流子迁移率，可用于太阳能驱动的光催化析氢。在可见光照射（λ>420 nm）下，Pt掺杂的COF-JLU100对水分解表现出超过100000 μmol g⁻¹ h⁻¹的高析氢速率。实验和理论研究证实，COF-JLU100中的氰基乙烯片段扩展了π离域，实现了快速的电荷转移和分离速率以及在水中的良好分散性。此外，COF-JLU100可以由低成本且易于获得的单体制备，并且具有出色的稳定性，这对于实际的太阳能驱动制氢是理想的。
