Designing Heteroatom‐Codoped Iron Metal–Organic Framework for Promotional Photoreduction of Carbon Dioxide to Ethylene

Rational engineering active sites and vantage defects of catalysts are promising but grand challenging task to enhance photoreduction CO2 to high value‐added C2 products. In this study, we designed an N,S‐codoped Fe‐based MIL‐88B catalyst with well‐defined bipyramidal hexagonal prism morphology via...

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Veröffentlicht in:	Angewandte Chemie (International ed.) Jg. 62; H. 14; S. e202216232 - n/a
Hauptverfasser:	Guo, Fan, Li, Rui‐Xia, Yang, Sizhuo, Zhang, Xiao‐Yu, Yu, Hongjian, Urban, Jeffrey J., Sun, Wei‐Yin
Format:	Journal Article
Sprache:	Englisch
Veröffentlicht:	Germany Wiley Subscription Services, Inc 27.03.2023 Wiley
Ausgabe:	International ed. in English
Schlagworte:	Acetic acid C2H4 Carbon dioxide Catalysts CO2 Reduction Defects Dimerization Doping Electron density INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY Intermediates Iron Irradiation Metal-organic frameworks Photocatalysis Photoreduction Radiation Solar radiation Synergistic effect Metal-Organic Frameworks C2H4 Photocatalysis CO2 Reduction Doping
ISSN:	1433-7851, 1521-3773, 1521-3773
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Abstract	Rational engineering active sites and vantage defects of catalysts are promising but grand challenging task to enhance photoreduction CO2 to high value‐added C2 products. In this study, we designed an N,S‐codoped Fe‐based MIL‐88B catalyst with well‐defined bipyramidal hexagonal prism morphology via a facile and effective process, which was synthesized by addition of appropriate 1,2‐benzisothiazolin‐3‐one (BIT) and acetic acid to the reaction solution. Under simulated solar irradiation, the designed catalyst exhibits high C2H4 evolution yield of 17.7 μmol g−1⋅h, which has been rarely achieved in photocatalytic CO2 reduction process. The synergistic effect of Fe‐N coordinated sites and reasonable defects in the N,S‐codoped photocatalyst can accelerate the migration of photogenerated carriers, resulting in high electron density, and this in turn helps to facilitate the formation and dimerization of C−C coupling intermediates for C2H4 effectively. The integration of new active sites with beneficial defects in Fe‐MOF MIL‐88B catalysts gives enhanced photoreduction of CO2 to C2H4 under visible light. The modified structure promotes the migration and separation of the photoelectrons to produce the pivotal C−C coupling intermediate for the generation of C2H4, a result supported by in situ FT‐IR analysis.
AbstractList	Rational engineering active sites and vantage defects of catalysts are promising but grand challenging task to enhance photoreduction CO2 to high value‐added C2 products. In this study, we designed an N,S‐codoped Fe‐based MIL‐88B catalyst with well‐defined bipyramidal hexagonal prism morphology via a facile and effective process, which was synthesized by addition of appropriate 1,2‐benzisothiazolin‐3‐one (BIT) and acetic acid to the reaction solution. Under simulated solar irradiation, the designed catalyst exhibits high C2H4 evolution yield of 17.7 μmol g−1⋅h, which has been rarely achieved in photocatalytic CO2 reduction process. The synergistic effect of Fe‐N coordinated sites and reasonable defects in the N,S‐codoped photocatalyst can accelerate the migration of photogenerated carriers, resulting in high electron density, and this in turn helps to facilitate the formation and dimerization of C−C coupling intermediates for C2H4 effectively. Rational engineering active sites and vantage defects of catalysts are promising but grand challenging task to enhance photoreduction CO2 to high value-added C2 products. In this study, we designed an N,S-codoped Fe-based MIL-88B catalyst with well-defined bipyramidal hexagonal prism morphology via a facile and effective process, which was synthesized by addition of appropriate 1,2-benzisothiazolin-3-one (BIT) and acetic acid to the reaction solution. Under simulated solar irradiation, the designed catalyst exhibits high C2 H4 evolution yield of 17.7 μmol g-1 ∙h, which has been rarely achieved in photocatalytic CO2 reduction process. The synergistic effect of Fe-N coordinated sites and reasonable defects in the N,S-codoped photocatalyst can accelerate the migration of photogenerated carriers, resulting in high electron density, and this in turn helps to facilitate the formation and dimerization of C-C coupling intermediates for C2 H4 effectively. Rational engineering active sites and vantage defects of catalysts are promising but grand challenging task to enhance photoreduction CO2 to high value‐added C2 products. In this study, we designed an N,S‐codoped Fe‐based MIL‐88B catalyst with well‐defined bipyramidal hexagonal prism morphology via a facile and effective process, which was synthesized by addition of appropriate 1,2‐benzisothiazolin‐3‐one (BIT) and acetic acid to the reaction solution. Under simulated solar irradiation, the designed catalyst exhibits high C2H4 evolution yield of 17.7 μmol g−1⋅h, which has been rarely achieved in photocatalytic CO2 reduction process. The synergistic effect of Fe‐N coordinated sites and reasonable defects in the N,S‐codoped photocatalyst can accelerate the migration of photogenerated carriers, resulting in high electron density, and this in turn helps to facilitate the formation and dimerization of C−C coupling intermediates for C2H4 effectively. The integration of new active sites with beneficial defects in Fe‐MOF MIL‐88B catalysts gives enhanced photoreduction of CO2 to C2H4 under visible light. The modified structure promotes the migration and separation of the photoelectrons to produce the pivotal C−C coupling intermediate for the generation of C2H4, a result supported by in situ FT‐IR analysis. Rational engineering active sites and vantage defects of catalysts are promising but grand challenging task to enhance photoreduction CO2 to high value-added C2 products. In this study, we designed an N,S-codoped Fe-based MIL-88B catalyst with well-defined bipyramidal hexagonal prism morphology via a facile and effective process, which was synthesized by addition of appropriate 1,2-benzisothiazolin-3-one (BIT) and acetic acid to the reaction solution. Under simulated solar irradiation, the designed catalyst exhibits high C2 H4 evolution yield of 17.7 μmol g-1 ⋅h, which has been rarely achieved in photocatalytic CO2 reduction process. The synergistic effect of Fe-N coordinated sites and reasonable defects in the N,S-codoped photocatalyst can accelerate the migration of photogenerated carriers, resulting in high electron density, and this in turn helps to facilitate the formation and dimerization of C-C coupling intermediates for C2 H4 effectively.Rational engineering active sites and vantage defects of catalysts are promising but grand challenging task to enhance photoreduction CO2 to high value-added C2 products. In this study, we designed an N,S-codoped Fe-based MIL-88B catalyst with well-defined bipyramidal hexagonal prism morphology via a facile and effective process, which was synthesized by addition of appropriate 1,2-benzisothiazolin-3-one (BIT) and acetic acid to the reaction solution. Under simulated solar irradiation, the designed catalyst exhibits high C2 H4 evolution yield of 17.7 μmol g-1 ⋅h, which has been rarely achieved in photocatalytic CO2 reduction process. The synergistic effect of Fe-N coordinated sites and reasonable defects in the N,S-codoped photocatalyst can accelerate the migration of photogenerated carriers, resulting in high electron density, and this in turn helps to facilitate the formation and dimerization of C-C coupling intermediates for C2 H4 effectively. Rational engineering active sites and vantage defects of catalysts are promising but grand challenging task to enhance photoreduction CO 2 to high value‐added C2 products. In this study, we designed an N,S‐codoped Fe‐based MIL‐88B catalyst with well‐defined bipyramidal hexagonal prism morphology via a facile and effective process, which was synthesized by addition of appropriate 1,2‐benzisothiazolin‐3‐one (BIT) and acetic acid to the reaction solution. Under simulated solar irradiation, the designed catalyst exhibits high C 2 H 4 evolution yield of 17.7 μmol g −1 ⋅h, which has been rarely achieved in photocatalytic CO 2 reduction process. The synergistic effect of Fe‐N coordinated sites and reasonable defects in the N,S‐codoped photocatalyst can accelerate the migration of photogenerated carriers, resulting in high electron density, and this in turn helps to facilitate the formation and dimerization of C−C coupling intermediates for C 2 H 4 effectively. Rational engineering active sites and vantage defects of catalysts are promising but grand challenging task to enhance photoreduction CO to high value-added C2 products. In this study, we designed an N,S-codoped Fe-based MIL-88B catalyst with well-defined bipyramidal hexagonal prism morphology via a facile and effective process, which was synthesized by addition of appropriate 1,2-benzisothiazolin-3-one (BIT) and acetic acid to the reaction solution. Under simulated solar irradiation, the designed catalyst exhibits high C H evolution yield of 17.7 μmol g ⋅h, which has been rarely achieved in photocatalytic CO reduction process. The synergistic effect of Fe-N coordinated sites and reasonable defects in the N,S-codoped photocatalyst can accelerate the migration of photogenerated carriers, resulting in high electron density, and this in turn helps to facilitate the formation and dimerization of C-C coupling intermediates for C H effectively.
Author	Sun, Wei‐Yin Urban, Jeffrey J. Li, Rui‐Xia Guo, Fan Yang, Sizhuo Yu, Hongjian Zhang, Xiao‐Yu
Author_xml	– sequence: 1 givenname: Fan surname: Guo fullname: Guo, Fan email: guofan@yzu.edu.cn organization: Nanjing University – sequence: 2 givenname: Rui‐Xia surname: Li fullname: Li, Rui‐Xia organization: Yangzhou University – sequence: 3 givenname: Sizhuo surname: Yang fullname: Yang, Sizhuo organization: Lawrence Berkeley National Laboratory – sequence: 4 givenname: Xiao‐Yu surname: Zhang fullname: Zhang, Xiao‐Yu organization: Nanjing University – sequence: 5 givenname: Hongjian surname: Yu fullname: Yu, Hongjian organization: Yangzhou University – sequence: 6 givenname: Jeffrey J. surname: Urban fullname: Urban, Jeffrey J. organization: Lawrence Berkeley National Laboratory – sequence: 7 givenname: Wei‐Yin orcidid: 0000-0001-8966-9728 surname: Sun fullname: Sun, Wei‐Yin email: sunwy@nju.edu.cn organization: Nanjing University
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Snippet	Rational engineering active sites and vantage defects of catalysts are promising but grand challenging task to enhance photoreduction CO2 to high value‐added... Rational engineering active sites and vantage defects of catalysts are promising but grand challenging task to enhance photoreduction CO 2 to high value‐added... Rational engineering active sites and vantage defects of catalysts are promising but grand challenging task to enhance photoreduction CO to high value-added C2... Rational engineering active sites and vantage defects of catalysts are promising but grand challenging task to enhance photoreduction CO2 to high value-added...
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SubjectTerms	Acetic acid C2H4 Carbon dioxide Catalysts CO2 Reduction Defects Dimerization Doping Electron density INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY Intermediates Iron Irradiation Metal-organic frameworks Photocatalysis Photoreduction Radiation Solar radiation Synergistic effect
Title	Designing Heteroatom‐Codoped Iron Metal–Organic Framework for Promotional Photoreduction of Carbon Dioxide to Ethylene
URI	https://onlinelibrary.wiley.com/doi/abs/10.1002%2Fanie.202216232 https://www.ncbi.nlm.nih.gov/pubmed/36748922 https://www.proquest.com/docview/2788348639 https://www.proquest.com/docview/2774268687 https://www.osti.gov/servlets/purl/1963674
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