材料科学
光催化
共价键
联苯
共价有机骨架
带隙
纳米技术
吸收(声学)
可见光谱
光化学
化学工程
多孔性
光电子学
复合材料
催化作用
有机化学
化学
工程类
作者
Qihan Lin,Yusran Yusran,Jiabin Xing,Yongsheng Li,Jiangshan Zhang,Tianhui Su,Lingyi Yang,Jinquan Suo,Liming Zhang,Qiaowei Li,Hui Wang,Qianrong Fang,Zhan‐Ting Li,Dan‐Wei Zhang
标识
DOI:10.1021/acsami.3c16724
摘要
Structural conjugation greatly affects the optical and electronic properties of the COF photocatalyst. Herein, we show that 2D hydrazone COFs with either π-extended biphenyl (BPh-COF) or acetylene (AC-COF) frameworks demonstrated distinct charge transfer and photocatalytic performances. The two COFs show good crystallinity and decent porosity as their frameworks are enforced by intra/interlayers hydrogen bonding. However, computational and experimental data reveal that AC-COF managed broader visible-light absorption and narrower optical bandgaps and performed efficient photoinduced charge separation and transfer in comparison with BPh-COF, meaning that the ethynyl skeleton with enhanced planarity better improves the π-conjugation of the whole structure. As a result, AC-COF exhibited an ideal bandgap for rapid oxidative coupling of amines under visible-light irradiation. Furthermore, taking advantage of its better charge transfer properties, AC-COF demonstrated considerable enhanced product conversion and notable functional tolerance for metallaphotocatalytic C-O cross-coupling of a wide range of both aryl bromides and chlorides with alcohols. More importantly, besides being recoverable, AC-COF showcased the previously inaccessible etherification of dihaloarene. This report shows a facile approach for manipulating the structure-activity relationship and paves the way for the development of a COF photocatalyst for solar-to-chemical energy conversion.
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