Anthraquinone-Based Conjugated Organic Polymers Containing Dual Oxidation Centers for Photocatalytic H2O2 Production from H2O and O2 under Visible-Light Irradiation

被引:17
|
作者
Xu, Xiahong [1 ,2 ]
Sui, Yan [2 ]
Chen, Wentong [2 ]
Zhou, Gangyong [2 ]
Li, Yuntong [2 ]
Zhong, Hong [2 ]
Wen, He-Rui [1 ]
机构
[1] Jiangxi Univ Sci & Technol, Sch Chem & Chem Engn, Jiangxi Prov Key Lab Funct Mol Mat Chem, Ganzhou 341000, Jiangxi Provinc, Peoples R China
[2] Jinggangshan Univ, Key Lab Coordinat Chem Jiangxi Prov, Sch Chem & Chem Engn, Jian 343009, Jiangxi Provinc, Peoples R China
基金
中国国家自然科学基金;
关键词
conjugated organic polymers; dual oxidation centers; photocatalysis; H2O2; visible light; HYDROGEN-PEROXIDE PRODUCTION; MOLECULAR-OXYGEN; REDOX CENTERS; WATER; FRAMEWORK; GENERATION; RICH;
D O I
10.1021/acsapm.3c01455
中图分类号
T [工业技术];
学科分类号
08 ;
摘要
Photocatalytic H2O2 productionfrom H2O and O-2 under visible-light irradiationis a promisingmethod for the green chemical industry and the conversion of solarenergy to fuel. However, the efficiencies remain relatively low dueto the rapid photogenerated charge recombination caused by the inefficientH(2)O oxidation. Herein, we present an anthraquinone-basedconjugated organic polymer (AQTT-COP) containing alkynyl and triazinyldual oxidation centers by the Sonogashira cross-coupling reactionof 2,6-dibromoanthraquinone (AQ) and 2,4,6-tris(4-ethynylphenyl)-1,3,5-triazine(TT). The dual H2O-oxidation centers of triazinyl and alkynylmoieties are conducive to the consumption of photogenerated holesand inhibit electron-hole pair recombination by efficient H2O-oxidation reactions. Meanwhile, the anthraquinone moietiescould serve as O-2 reduction centers to accept photogeneratedelectrons and transfer them to the O-2 molecules for thesubsequent production of H2O2, thereby boostingthe overall reaction kinetics, which in turn improves non-sacrificialH(2)O(2) production. The rational design of AQTT-COPwith spatially separated O-2 reduction centers and dualH(2)O-oxidation centers enables maximizing photogeneratedelectron utilization and exhibits efficient photocatalytic H2O2 production with an initial rate of 3221 & mu;molg(-1) h(-1) under visible-light (& lambda;& GE; 400 nm) irradiation without any additives. This work providesa protocol for the unification of task-specific catalytically activecomponents for photocatalytic H2O2 production.
引用
收藏
页码:7571 / 7580
页数:10
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