Volume 9 Issue 9
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Article Navigation >  Green Energy&Environment  > 2024  >  9(9): 1407-1418
Sheng-Yan Yin, Ziyi Li, Yingcai Hu, Xiao Luo, Jishan Li. A novel metal-free porous covalent organic polymer for efficient room-temperature photocatalytic CO2 reduction via dry-reforming of methane. Green Energy&Environment, 2024, 9(9): 1407-1418. doi: 10.1016/j.gee.2023.03.003
Citation: Sheng-Yan Yin, Ziyi Li, Yingcai Hu, Xiao Luo, Jishan Li. A novel metal-free porous covalent organic polymer for efficient room-temperature photocatalytic CO2 reduction via dry-reforming of methane. Green Energy&Environment, 2024, 9(9): 1407-1418. doi: 10.1016/j.gee.2023.03.003
shu

A novel metal-free porous covalent organic polymer for efficient room-temperature photocatalytic CO2 reduction via dry-reforming of methane

doi: 10.1016/j.gee.2023.03.003

  • a. College of Chemistry and Chemical Engineering, Hunan University, Changsha, 410082, China;

  • b. Institute of Basic Medicine and Cancer (IBMC), Chinese Academy of Sciences, Hangzhou, Zhejiang, 310022, China

Funds:

This work was supported by National Natural Science Foundation of China (Nos. 22274039 and 22178089) and Hunan Provincial Innovation Foundation for Postgraduate (No.CX20220392) was acknowledged. The testing platform (https://www.shiyanjia.com/) was gratefully acknowledged to carry out characterizations.

  • Received date 08 January 2023, Accepted date 16 March 2023, RevRecd date 21 February 2023, Publish date 21 March 2023,
    Abstract
  • 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.

     

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