化工进展2024,Vol.43Issue(1) :292-301.DOI:10.16085/j.issn.1000-6613.2023-1463

D-A共轭聚合强化光电性能及光催化CO2转化

Enhanced photoelectric properties and photocatalytic CO2 conversion by D-A conjugated polymerization

于笑笑 巢艳红 刘海燕 朱文帅 刘植昌
化工进展2024,Vol.43Issue(1) :292-301.DOI:10.16085/j.issn.1000-6613.2023-1463

D-A共轭聚合强化光电性能及光催化CO2转化

Enhanced photoelectric properties and photocatalytic CO2 conversion by D-A conjugated polymerization

于笑笑 1巢艳红 1刘海燕 1朱文帅 2刘植昌3
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作者信息

  • 1. 中国石油大学(北京)理学院,北京 102249
  • 2. 中国石油大学(北京)化学工程与环境学院,北京 102249;江苏大学化学化工学院, 江苏 镇江 212013
  • 3. 中国石油大学(北京)化学工程与环境学院,北京 102249
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摘要

2,6-二溴蒽醌(2,6-dibromoanthraquinone,AQ)分别与三(4-乙炔苯基)胺(tris(4-ethynylphenyl)amine,TEA)和1,3,5-三乙炔基苯(1,3,5-triethynylbenzene,TEB),通过Sonogashira偶联反应制备得到两种蒽醌功能化的给体-受体(D-A)共轭聚合物催化剂(AQ-TEA和AQ-TEB).采用FTIR、XPS、XRD和TEM 对其化学结构和形貌进行了表征.通过固体紫外/可见漫反射光谱、稳态荧光光谱、时间分辨荧光光谱和电化学表征探究了两种催化材料的光学和电学性能.结果表明,三(4-乙炔苯基)胺与2,6-二溴蒽醌构筑的AQ-TEA表现出更强的可见光吸收和电荷转移性能.研究了两种光催化剂在H2O环境下光还原CO2的催化性能.特别是AQ-TEA表现出更好的光催化性能,其CO的生成速率为392μmol/(g·h),是AQ-TEB的1.8倍.基于实验和理论计算的结果,推测共轭聚合物中强的分子内电荷转移(intramolecular charge transfer,ICT)可促进其光吸收、光电转换和光催化效率的提升.本研究为设计和制备高效的光催化活性共轭聚合物催化剂提供了新的思路.

Abstract

Herein,two anthraquinone-functionalized donor-acceptor(D-A)conjugated polymeric catalysts(AQ-TEA and AQ-TEB),were prepared via Sonogashira cross-coupling of 2,6-dibromoanthraquinone(AQ)with tris(4-ethynylphenyl)amine(TEA)and 1,3,5-triethynylbenzene(TEB),respectively.The chemical structures and morphologies of the catalysts were characterized by FTIR,XPS,XRD and TEM.The optical and electronic properties of two catalysts were investigated by solid UV/Vis diffuse reflectance spectroscopy,steady-state fluorescence spectroscopy,time-resolved fluorescence spectroscopy,and electrochemical characterization.The results indicated that AQ-TEA derived from 2,6-dibromoanthraquinone and tris(4-ethynylphenyl)amine exhibited stronger visible-light absorption and charge-transfer performance.The catalytic performance of two photocatalysts for the photoreduction of CO2 in the presence of H2O was studied.AQ-TEA showed better performance,with a CO production rate of 392μmol/(g·h),which was 1.8 times that of AQ-TEB.Based on the results of experiments and theoretical calculations,we deduced that the strong intramolecular charge transfer(ICT)in the conjugated polymers could promote their light absorption,photoelectric conversion and photocatalytic performance.This work provides a new insight into design and fabrication of active conjugated polymeric catalysts with high photocatalytic efficiency for solar-energy conversion.

关键词

聚合物/催化剂/光化学/二氧化碳

Key words

polymers/catalyst/photochemistry/carbon dioxide

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基金项目

国家自然科学基金(22178154)

中国石油大学(北京)科学基金(2462023QNXZ009)

重质油全国重点实验室自主研究项目(2023-12)

海南省水环境污染治理与资源化重点实验室(SHJKFKT202306)

出版年

2024
化工进展
中国化工学会,化学工业出版社

化工进展

CSTPCD北大核心
影响因子:1.062
ISSN:1000-6613
参考文献量3
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