Zhao Wei, Yan Peiyao, Li Boyu, Bahri Mounib, Liu Lunjie, Zhou Xiang, Clowes Rob, Browning Nigel D, Wu Yue, Ward John W, Cooper Andrew I
Materials Innovation Factory and Department of Chemistry, University of Liverpool, Liverpool L69 7ZD, United Kingdom.
Leverhulme Research Centre for Functional Materials Design, Materials Innovation Factory and Department of Chemistry, University of Liverpool, Liverpool L69 7ZD, United Kingdom.
J Am Chem Soc. 2022 Jun 8;144(22):9902-9909. doi: 10.1021/jacs.2c02666. Epub 2022 May 30.
A high-throughput sonochemical synthesis and testing strategy was developed to discover covalent organic frameworks (COFs) for photocatalysis. In total, 76 conjugated polymers were synthesized, including 60 crystalline COFs of which 18 were previously unreported. These COFs were then screened for photocatalytic hydrogen peroxide (HO) production using water and oxygen. One of these COFs, sonoCOF-F2, was found to be an excellent photocatalyst for photocatalytic HO production even in the absence of sacrificial donors. However, after long-term photocatalytic tests (96 h), the imine sonoCOF-F2 transformed into an amide-linked COF with reduced crystallinity and loss of electronic conjugation, decreasing the photocatalytic activity. When benzyl alcohol was introduced to form a two-phase catalytic system, the photostability of sonoCOF-F2 was greatly enhanced, leading to stable HO production for at least 1 week.
开发了一种高通量声化学合成与测试策略,以发现用于光催化的共价有机框架(COF)。总共合成了76种共轭聚合物,包括60种结晶COF,其中18种是以前未报道过的。然后使用水和氧气对这些COF进行光催化过氧化氢(HO)生成的筛选。其中一种COF,声致COF-F2,即使在没有牺牲供体的情况下,也被发现是用于光催化HO生成的优异光催化剂。然而,经过长期光催化测试(96小时)后,亚胺声致COF-F2转变为结晶度降低且电子共轭丧失的酰胺连接COF,从而降低了光催化活性。当引入苯甲醇形成两相催化体系时,声致COF-F2的光稳定性大大提高,导致至少1周内HO的稳定生成。