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二维sp~2碳共价有机框架及高效光催化制氢（英文）

Fully conjugated two-dimensional sp~2-carbon covalent organic frameworks for efficient photocatalytic hydrogen generation

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【作者】 刘辉； 王丹博； 于泽芳； 陈雅静； 李旭兵； 张瑞玲； 陈雄； 吴骊珠； 丁乃秀； 王元成； 赵英杰；

【Author】 Hui Liu;Danbo Wang;Zefang Yu;Yajing Chen;Xubing Li;Ruiling Zhang;Xiong Chen;Lizhu Wu;Naixiu Ding;Yuancheng Wang;Yingjie Zhao;College of Polymer Science and Engineering, Qingdao University of Science and Technology;Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry, Chinese Academy of Sciences;Institute of Molecular Sciences and Engineering, Institute of Frontier and Interdisciplinary Science, Shandong University;Key Laboratory of Molecule Synthesis and Function Discovery(Fujian Province University), State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University;

【通讯作者】 丁乃秀;王元成;赵英杰;

【机构】 College of Polymer Science and Engineering, Qingdao University of Science and Technology； Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry, Chinese Academy of Sciences； Institute of Molecular Sciences and Engineering, Institute of Frontier and Interdisciplinary Science, Shandong University； Key Laboratory of Molecule Synthesis and Function Discovery(Fujian Province University), State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University；

【摘要】 本文设计合成了两种具有不同连接方式(亚胺键和sp~2-C-CN键)的三嗪基共价有机框架(COFs)材料.连接单元的微小变化导致可见光驱动制氢性能的巨大差异.具有sp~2碳连接方式的全π共轭二维COFs在450 nm波长处表现出13.48%的外量子效率,优于已报道的COFs光催化剂.而亚胺键的二维COFs几乎没有光活性.借助光电化学研究和量子化学计算进一步研究了二维COFs的催化机理,为太阳能转化高性能有机光催化剂的制备提供了新的见解.

【Abstract】 In this paper,two types of conjugated,triazinebased covalent organic frameworks(COFs) with different connected linkages(imine bond and sp~2-carbon-CN bond) are presented.The insignificant difference in the linkages creates a remarkable difference in their performance in visible-lightdriven hydrogen generation.The fully π-conjugated two-dimensional(2D) COF with sp~2-carbon-CN linkages showed an external quantum efficiency of 13.48% at 450 nm,which is an unprecedented result for COF photocatalysts.In contrast,the imine-linked 2D COF displayed almost no photoactivity.Further photoelectrochemical and quantum chemical studies provide an in-depth understanding of the catalytic mechanism.This finding provides new insight into preparing highperformance organic photocatalysts for solar energy conversion.

【关键词】 covalent organic frameworks； photocatalytic hydrogen generation； π-conjugated system； triazine；
【Key words】 covalent organic frameworks； photocatalytic hydrogen generation； π-conjugated system； triazine；
【基金】 financially supported by the National Natural Science Foundation of China (31202117 and 51972185);the Natural Science Foundation of Shandong Province (ZR2020ZD38)
  • 【文献出处】 Science China(Materials) ,中国科学:材料科学(英文版) , 编辑部邮箱 ,2023年06期
  • 【分类号】TQ116.2;O643.36;O644.1
  • 【下载频次】71
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