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作者:

Kong, Xiang-Jing (Kong, Xiang-Jing.) | He, Tao (He, Tao.) | Zhou, Jian (Zhou, Jian.) | Zhao, Chen (Zhao, Chen.) | Li, Tong-Chuan (Li, Tong-Chuan.) | Wu, Xue-Qian (Wu, Xue-Qian.) | Wang, Kecheng (Wang, Kecheng.) | Li, Jian-Rong (Li, Jian-Rong.) (学者:李坚)

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摘要:

Despite numerous inherent merits of metal-organic frameworks (MOFs), structural fragility has imposed great restrictions on their wider involvement in many applications, such as in catalysis. Herein, a strategy for enhancing stability and enabling functionality in a labile Zr(IV)-MOF has been proposed by in situ porphyrin substitution. A size- and geometry-matched robust linear porphyrin ligand 4,4 '-(porphyrin-5,15-diyl)dibenzolate (DCPP2-) is selected to replace the 4,4 '-(1,3,6,8-tetraoxobenzo[lmn][3,8]phenanthroline-2,7(1H,3H,6H,8H)-diyl)dibenzoate (NDIDB2-) ligand in the synthesis of BUT-109(Zr), affording BUT-110 with varied porphyrin contents. Compared to BUT-109(Zr), the chemical stability of BUT-110 series is greatly improved. Metalloporphyrin incorporation endows BUT-110 MOFs with high catalytic activity in the photoreduction of CO2, in the absence of photosensitizers. By tuning the metal species and porphyrin contents in BUT-110, the resulting BUT-110-50%-Co is demonstrated to be a good photocatalyst for selective CO2-to-CO reduction, via balancing the chemical stability, photocatalytic efficiency, and synthetic cost. This work highlights the advantages of in situ ligand substitution for MOF modification, by which uniform distribution and high content of the incoming ligand are accessible in the resulting MOFs. More importantly, it provides a promising approach to convert unstable MOFs, which mainly constitute the vast MOF database but have always been neglected, into robust functional materials.

关键词:

photocatalytic CO in situ ligand substitution organic frameworks metal&#8211 porphyrin ligands (2) reduction stability enhancement

作者机构:

  • [ 1 ] [Kong, Xiang-Jing]Beijing Univ Technol, Beijing Key Lab Green Catalysis & Separat, Beijing 100124, Peoples R China
  • [ 2 ] [He, Tao]Beijing Univ Technol, Beijing Key Lab Green Catalysis & Separat, Beijing 100124, Peoples R China
  • [ 3 ] [Zhou, Jian]Beijing Univ Technol, Beijing Key Lab Green Catalysis & Separat, Beijing 100124, Peoples R China
  • [ 4 ] [Zhao, Chen]Beijing Univ Technol, Beijing Key Lab Green Catalysis & Separat, Beijing 100124, Peoples R China
  • [ 5 ] [Li, Tong-Chuan]Beijing Univ Technol, Beijing Key Lab Green Catalysis & Separat, Beijing 100124, Peoples R China
  • [ 6 ] [Wu, Xue-Qian]Beijing Univ Technol, Beijing Key Lab Green Catalysis & Separat, Beijing 100124, Peoples R China
  • [ 7 ] [Wang, Kecheng]Beijing Univ Technol, Beijing Key Lab Green Catalysis & Separat, Beijing 100124, Peoples R China
  • [ 8 ] [Li, Jian-Rong]Beijing Univ Technol, Beijing Key Lab Green Catalysis & Separat, Beijing 100124, Peoples R China
  • [ 9 ] [Kong, Xiang-Jing]Beijing Univ Technol, Dept Environm Chem Engn, Beijing 100124, Peoples R China
  • [ 10 ] [He, Tao]Beijing Univ Technol, Dept Environm Chem Engn, Beijing 100124, Peoples R China
  • [ 11 ] [Zhou, Jian]Beijing Univ Technol, Dept Environm Chem Engn, Beijing 100124, Peoples R China
  • [ 12 ] [Zhao, Chen]Beijing Univ Technol, Dept Environm Chem Engn, Beijing 100124, Peoples R China
  • [ 13 ] [Li, Tong-Chuan]Beijing Univ Technol, Dept Environm Chem Engn, Beijing 100124, Peoples R China
  • [ 14 ] [Wu, Xue-Qian]Beijing Univ Technol, Dept Environm Chem Engn, Beijing 100124, Peoples R China
  • [ 15 ] [Wang, Kecheng]Beijing Univ Technol, Dept Environm Chem Engn, Beijing 100124, Peoples R China
  • [ 16 ] [Li, Jian-Rong]Beijing Univ Technol, Dept Environm Chem Engn, Beijing 100124, Peoples R China

通讯作者信息:

  • 李坚

    [Li, Jian-Rong]Beijing Univ Technol, Beijing Key Lab Green Catalysis & Separat, Beijing 100124, Peoples R China;;[Li, Jian-Rong]Beijing Univ Technol, Dept Environm Chem Engn, Beijing 100124, Peoples R China

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来源 :

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ISSN: 1613-6810

年份: 2021

期: 22

卷: 17

1 3 . 3 0 0

JCR@2022

ESI学科: MATERIALS SCIENCE;

ESI高被引阀值:116

JCR分区:1

被引次数:

WoS核心集被引频次: 12

SCOPUS被引频次: 127

ESI高被引论文在榜: 0 展开所有

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