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Title: Photosensitizer‐Anchored 2D MOF Nanosheets as Highly Stable and Accessible Catalysts toward Artemisinin Production

Abstract

2D metal–organic frameworks (2D-MOFs) have recently emerged as promising materials for gas separations, sensing, conduction, and catalysis. However, the stability of these 2D-MOF catalysts and the tunability over catalytic environments are limited. Herein, it is demonstrated that 2D-MOFs can act as stable and highly accessible catalyst supports by introducing more firmly anchored photosensitizers as bridging ligands. An ultrathin MOF nanosheet-based material, Zr-BTB (BTB = 1,3,5-tris(4-carboxyphenyl)benzene), is initially constructed by connecting Zr 6-clusters with the tritopic carboxylate linker. Surface modification of the Zr-BTB structure was realized through the attachment of porphyrin-based carboxylate ligands on the coordinatively unsaturated Zr metal sites in the MOF through strong Zr-carboxylate bond formation. The functionalized MOF nanosheet, namely PCN-134-2D, acts as an efficient photocatalyst for 1O 2 generation and artemisinin production. Compared to the 3D analogue (PCN-134-3D), PCN-134-2D allows for fast reaction kinetics due to the enhanced accessibility of the catalytic sites within the structure and facile substrate diffusion. Additionally, PCN-134(Ni)-2D exhibits an exceptional yield of artemisinin, surpassing all reported homo- or heterogeneous photocatalysts for the artemisinin production.

Authors:
 [1];  [2];  [2];  [2];  [2];  [2];  [3];  [2];  [4];  [2];  [2];  [5];  [4]; ORCiD logo [2];  [6]
  1. College of ChemistryTianjin Normal University Tianjin 300387 China, Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education)Nankai University Tianjin 300071 China
  2. Department of ChemistryTexas A&,M University College Station TX 77843 USA
  3. College of ChemistryTianjin Normal University Tianjin 300387 China
  4. Institute of New Energy Materials &, Low Carbon TechnologySchool of Material Science &, EngineeringTianjin University of Technology Tianjin 300384 China
  5. College of Chemistry and Materials ScienceNanjing Normal University Nanjing 210023 China
  6. Department of ChemistryTexas A&,M University College Station TX 77843 USA, Department of Materials Science and EngineeringTexas A&,M University College Station TX 77842 USA
Publication Date:
Research Org.:
Texas A & M Univ., College Station, TX (United States); Univ. of California, Oakland, CA (United States)
Sponsoring Org.:
USDOE Office of Fossil Energy (FE)
OSTI Identifier:
1506130
Alternate Identifier(s):
OSTI ID: 1506131; OSTI ID: 1614285
Grant/Contract Number:  
FE0026472; SC0001015
Resource Type:
Journal Article: Published Article
Journal Name:
Advanced Science
Additional Journal Information:
Journal Name: Advanced Science; Journal ID: ISSN 2198-3844
Publisher:
Wiley
Country of Publication:
Germany
Language:
English
Subject:
36 MATERIALS SCIENCE; Chemistry; Science & Technology; Materials Science

Citation Formats

Wang, Ying, Feng, Liang, Pang, Jiandong, Li, Jialuo, Huang, Ning, Day, Gregory S., Cheng, Lin, Drake, Hannah F., Wang, Ye, Lollar, Christina, Qin, Junsheng, Gu, Zhiyuan, Lu, Tongbu, Yuan, Shuai, and Zhou, Hong‐Cai. Photosensitizer‐Anchored 2D MOF Nanosheets as Highly Stable and Accessible Catalysts toward Artemisinin Production. Germany: N. p., 2019. Web. doi:10.1002/advs.201802059.
Wang, Ying, Feng, Liang, Pang, Jiandong, Li, Jialuo, Huang, Ning, Day, Gregory S., Cheng, Lin, Drake, Hannah F., Wang, Ye, Lollar, Christina, Qin, Junsheng, Gu, Zhiyuan, Lu, Tongbu, Yuan, Shuai, & Zhou, Hong‐Cai. Photosensitizer‐Anchored 2D MOF Nanosheets as Highly Stable and Accessible Catalysts toward Artemisinin Production. Germany. https://doi.org/10.1002/advs.201802059
Wang, Ying, Feng, Liang, Pang, Jiandong, Li, Jialuo, Huang, Ning, Day, Gregory S., Cheng, Lin, Drake, Hannah F., Wang, Ye, Lollar, Christina, Qin, Junsheng, Gu, Zhiyuan, Lu, Tongbu, Yuan, Shuai, and Zhou, Hong‐Cai. Tue . "Photosensitizer‐Anchored 2D MOF Nanosheets as Highly Stable and Accessible Catalysts toward Artemisinin Production". Germany. https://doi.org/10.1002/advs.201802059.
@article{osti_1506130,
title = {Photosensitizer‐Anchored 2D MOF Nanosheets as Highly Stable and Accessible Catalysts toward Artemisinin Production},
author = {Wang, Ying and Feng, Liang and Pang, Jiandong and Li, Jialuo and Huang, Ning and Day, Gregory S. and Cheng, Lin and Drake, Hannah F. and Wang, Ye and Lollar, Christina and Qin, Junsheng and Gu, Zhiyuan and Lu, Tongbu and Yuan, Shuai and Zhou, Hong‐Cai},
abstractNote = {2D metal–organic frameworks (2D-MOFs) have recently emerged as promising materials for gas separations, sensing, conduction, and catalysis. However, the stability of these 2D-MOF catalysts and the tunability over catalytic environments are limited. Herein, it is demonstrated that 2D-MOFs can act as stable and highly accessible catalyst supports by introducing more firmly anchored photosensitizers as bridging ligands. An ultrathin MOF nanosheet-based material, Zr-BTB (BTB = 1,3,5-tris(4-carboxyphenyl)benzene), is initially constructed by connecting Zr6-clusters with the tritopic carboxylate linker. Surface modification of the Zr-BTB structure was realized through the attachment of porphyrin-based carboxylate ligands on the coordinatively unsaturated Zr metal sites in the MOF through strong Zr-carboxylate bond formation. The functionalized MOF nanosheet, namely PCN-134-2D, acts as an efficient photocatalyst for 1O2 generation and artemisinin production. Compared to the 3D analogue (PCN-134-3D), PCN-134-2D allows for fast reaction kinetics due to the enhanced accessibility of the catalytic sites within the structure and facile substrate diffusion. Additionally, PCN-134(Ni)-2D exhibits an exceptional yield of artemisinin, surpassing all reported homo- or heterogeneous photocatalysts for the artemisinin production.},
doi = {10.1002/advs.201802059},
url = {https://www.osti.gov/biblio/1506130}, journal = {Advanced Science},
issn = {2198-3844},
number = ,
volume = ,
place = {Germany},
year = {2019},
month = {4}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record at https://doi.org/10.1002/advs.201802059

Citation Metrics:
Cited by: 14 works
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