首页|A novel metal-free porous covalent organic polymer for efficient room-temperature photocatalytic CO2 reduction via dry-reforming of methane
A novel metal-free porous covalent organic polymer for efficient room-temperature photocatalytic CO2 reduction via dry-reforming of methane
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At room temperature,the conversion of greenhouse gases into valuable chemicals using metal-free catalysts for dry reforming of methane(DRM)is quite promising and challenging.Herein,we developed a novel covalent organic porous polymer(TPE-COP)with rapid charge separation of the electron-hole pairs for DRM driven by visible light at room temperature,which can efficiently generate syngas(CO and H2).Both electron donor(tris(4-aminophenyl)amine,TAPA)and acceptor(4,4',4",4('")-((1 E,1'E,1"E,1('")E)-(ethene-1,1,2,2-tetrayltetrakis(benzene-4,1-diyl))tetrakis(ethene-2,1-diyl))tetrakis(1-(4-formylbenzyl)quinolin-1-ium),TPE-CHO)were existed in TPE-COP,in which the push-pull effect between them promoted the separation of photogenerated electron-hole,thus greatly improving the photocatalytic activity.Density functional theory(DFT)simulation results show that TPE-COP can form charge-separating species under light irradiation,leading to electrons accumulation in TPE-CHO unit and holes in TAPA,and thus efficiently initiating DRM.After 20 h illumination,the photocatalytic results show that the yields reach 1123.6 and 30.8 μmol g-1 for CO and H2,respectively,which are significantly higher than those of TPE-CHO small molecules.This excellent result is mainly due to the increase of specific surface area,the enhancement of light absorption capacity,and the improvement of photoelectron-generating efficiency after the formation of COP.Overall,this work contributes to understanding the advantages of COP materials for photocatalysis and fundamentally pushes metal-free catalysts into the door of DRM field.
Metal-freePhotocatalytic CO2 reductionCovalent organic polymerDry-reforming of methaneElectron donor and acceptor
Sheng-Yan Yin、Ziyi Li、Yingcai Hu、Xiao Luo、Jishan Li
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College of Chemistry and Chemical Engineering,Hunan University,Changsha,410082,China
Institute of Basic Medicine and Cancer(IBMC),Chinese Academy of Sciences,Hangzhou,Zhejiang,310022,China
National Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaHunan Provincial Innovation Foundation for Postgraduate
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