Amide-Engineered Metal–Organic Porous Liquids Toward Enhanced CO2 Photoreduction Performance

Yangrui Xu; Yewei Ren; Guosheng Zhou; Sheng Feng; Zhenzhen Yang; Sheng Dai; Ziyang Lu; Tianhua Zhou

doi:10.1002/adfm.202313695

Amide-Engineered Metal–Organic Porous Liquids Toward Enhanced CO₂ Photoreduction Performance

Yangrui Xu, Yewei Ren, Guosheng Zhou, Sheng Feng, Zhenzhen Yang, Sheng Dai, Ziyang Lu, Tianhua Zhou

Research output: Contribution to journal › Article › peer-review

44 Scopus citations

Abstract

The development of alternative catalytic systems toward high-performance CO₂ photoreduction is considered to be a promising approach to address the future energy demand and reduce the CO₂ emissions. However, CO₂ molecules are thermodynamically stable in nature, and thus the adsorption and activation of CO₂ on the surface of catalysts are the key factors to determine the conversion efficiency. Herein, a porous liquid (NH₂-UIO-66 PL) is demonstrated for efficiently facilitating the adsorption and activation of CO₂ by modification of metal–organic framework (NH₂-UIO-66) with ionic liquid via amide bonds. CdS/NH₂-UIO-66 PL exhibits high-performance CO₂-to-CO photoreduction with CO yield of 71.37 µmol g⁻¹ h⁻¹ and selectivity of 100%. Experiments and theoretical calculations show that the introduced amide moieties not only enriched the electron density at Zr⁴⁺ active sites but also stabilize ^*COOH intermediate. The achievements provide an effective strategy for the development of metal–organic frameworks for energy catalysis.

Original language	English
Article number	2313695
Journal	Advanced Functional Materials
Volume	34
Issue number	19
DOIs	https://doi.org/10.1002/adfm.202313695
State	Published - May 10 2024

Funding

Y.X. and Y.R. contributed equally to this work. This work was supported by the National Natural Science Foundation of China (22278190 and 22279143), the China Postdoctoral Science Foundation (2022M711382), the Zhenjiang Carbon Emissions Peak/Carbon Neutrality Science and the Technology Innovation Special Fund Project (CQ2022009), Qing Lan Project of Jiangsu Province (2023), the Jiangsu Collaborative Innovation Center of Technology and Material of Water Treatment, the Open Project of State Key Laboratory of Structural Chemistry (20230022), the Project of Research on Educational Reform and Talent Development, the School of Emergency Management, Jiangsu University (JG-03-11), the Special Scientific Research Project of School of Emergency Management, Jiangsu University (KY-C-12), and the Young Scientific and Technological Talents Support Project of Jiangsu Association for Science and Technology ((2021)091). Z.Y. and S.D. were supported by the Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences, US Department of Energy. Y.X. and Y.R. contributed equally to this work. This work was supported by the National Natural Science Foundation of China (22278190 and 22279143), the China Postdoctoral Science Foundation (2022M711382), the Zhenjiang Carbon Emissions Peak/Carbon Neutrality Science and the Technology Innovation Special Fund Project (CQ2022009), Qing Lan Project of Jiangsu Province (2023), the Jiangsu Collaborative Innovation Center of Technology and Material of Water Treatment, the Open Project of State Key Laboratory of Structural Chemistry (20230022), the Project of Research on Educational Reform and Talent Development, the School of Emergency Management, Jiangsu University (JG\u201003\u201011), the Special Scientific Research Project of School of Emergency Management, Jiangsu University (KY\u2010C\u201012), and the Young Scientific and Technological Talents Support Project of Jiangsu Association for Science and Technology ((2021)091). Z.Y. and S.D. were supported by the Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences, US Department of Energy.

Keywords

CO adsorption
CO photoreduction
metal–organic framework
photocatalysis
porous liquid

Access to Document

10.1002/adfm.202313695

Cite this

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title = "Amide-Engineered Metal–Organic Porous Liquids Toward Enhanced CO2 Photoreduction Performance",

abstract = "The development of alternative catalytic systems toward high-performance CO2 photoreduction is considered to be a promising approach to address the future energy demand and reduce the CO2 emissions. However, CO2 molecules are thermodynamically stable in nature, and thus the adsorption and activation of CO2 on the surface of catalysts are the key factors to determine the conversion efficiency. Herein, a porous liquid (NH2-UIO-66 PL) is demonstrated for efficiently facilitating the adsorption and activation of CO2 by modification of metal–organic framework (NH2-UIO-66) with ionic liquid via amide bonds. CdS/NH2-UIO-66 PL exhibits high-performance CO2-to-CO photoreduction with CO yield of 71.37 µmol g−1 h−1 and selectivity of 100%. Experiments and theoretical calculations show that the introduced amide moieties not only enriched the electron density at Zr4+ active sites but also stabilize *COOH intermediate. The achievements provide an effective strategy for the development of metal–organic frameworks for energy catalysis.",

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author = "Yangrui Xu and Yewei Ren and Guosheng Zhou and Sheng Feng and Zhenzhen Yang and Sheng Dai and Ziyang Lu and Tianhua Zhou",

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AU - Dai, Sheng

AU - Lu, Ziyang

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N2 - The development of alternative catalytic systems toward high-performance CO2 photoreduction is considered to be a promising approach to address the future energy demand and reduce the CO2 emissions. However, CO2 molecules are thermodynamically stable in nature, and thus the adsorption and activation of CO2 on the surface of catalysts are the key factors to determine the conversion efficiency. Herein, a porous liquid (NH2-UIO-66 PL) is demonstrated for efficiently facilitating the adsorption and activation of CO2 by modification of metal–organic framework (NH2-UIO-66) with ionic liquid via amide bonds. CdS/NH2-UIO-66 PL exhibits high-performance CO2-to-CO photoreduction with CO yield of 71.37 µmol g−1 h−1 and selectivity of 100%. Experiments and theoretical calculations show that the introduced amide moieties not only enriched the electron density at Zr4+ active sites but also stabilize *COOH intermediate. The achievements provide an effective strategy for the development of metal–organic frameworks for energy catalysis.

AB - The development of alternative catalytic systems toward high-performance CO2 photoreduction is considered to be a promising approach to address the future energy demand and reduce the CO2 emissions. However, CO2 molecules are thermodynamically stable in nature, and thus the adsorption and activation of CO2 on the surface of catalysts are the key factors to determine the conversion efficiency. Herein, a porous liquid (NH2-UIO-66 PL) is demonstrated for efficiently facilitating the adsorption and activation of CO2 by modification of metal–organic framework (NH2-UIO-66) with ionic liquid via amide bonds. CdS/NH2-UIO-66 PL exhibits high-performance CO2-to-CO photoreduction with CO yield of 71.37 µmol g−1 h−1 and selectivity of 100%. Experiments and theoretical calculations show that the introduced amide moieties not only enriched the electron density at Zr4+ active sites but also stabilize *COOH intermediate. The achievements provide an effective strategy for the development of metal–organic frameworks for energy catalysis.

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