Constructing an Asymmetric Covalent Triazine Framework to Boost the Efficiency and Selectivity of Visible-Light-Driven CO2 Photoreduction

Guang-Dong Qi; Dan Ba; Yu-Jie Zhang; Xue-Qing Jiang; Zihao Chen; Miao-Miao Yang; Jia-Min Cao; Wen-Wen Dong; Jun Zhao; Dong-Sheng Li; Qichun Zhang

doi:10.1002/advs.202402645

Constructing an Asymmetric Covalent Triazine Framework to Boost the Efficiency and Selectivity of Visible-Light-Driven CO₂ Photoreduction

Guang-Dong Qi, Dan Ba, Yu-Jie Zhang, Xue-Qing Jiang, Zihao Chen, Miao-Miao Yang, Jia-Min Cao, Wen-Wen Dong^*, Jun Zhao^*, Dong-Sheng Li^*, Qichun Zhang^*

^*Corresponding author for this work

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

30 Citations (Scopus)

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Abstract

The photocatalytic reduction of CO₂ represents an environmentally friendly and sustainable approach for generating valuable chemicals. In this study, a thiophene-modified highly conjugated asymmetric covalent triazine framework (As-CTF-S) is developed for this purpose. Significantly, single-component intramolecular energy transfer can enhance the photogenerated charge separation, leading to the efficient conversion of CO₂ to CO during photocatalysis. As a result, without the need for additional photosensitizers or organic sacrificial agents, As-CTF-S demonstrates the highest photocatalytic ability of 353.2 µmol g⁻¹ and achieves a selectivity of ≈99.95% within a 4 h period under visible light irradiation. This study provides molecular insights into the rational control of charge transfer pathways for high-efficiency CO₂ photoreduction using single-component organic semiconductor catalysts. © 2024 The Authors. Advanced Science published by Wiley-VCH GmbH.

Original language	English
Article number	2402645
Journal	Advanced Science
Volume	11
Issue number	28
Online published	13 May 2024
DOIs	https://doi.org/10.1002/advs.202402645
Publication status	Published - 24 Jul 2024

Funding

G.-D.Q. and D.B. contributed equally to this work. This work was financially supported by the National Natural Science Foundation of China (Grants 21671119 and 21971143), the Distinguished Youth Foundation of Hubei province (2020CFA092), the 111 Project (DT20015), the Research Program for Natural Science of Yichang (A23-2-022 and A22-3-014), the Program for Innovative Teams of Outstanding Young and Middle-aged Researchers in the Higher Education Institutions of Hubei Province (T201904), and the opening fund of Hubei Three Gorges Laboratory (SC232013 and 213004). Q.Z. acknowledges the funding support from the City University of Hong Kong (9380117 and 7020089) Hong Kong, P. R. China. Q.Z. thanks the funding support from the Innovation and Technology Fund (ITF, ITS/322/22) and the funding support from State Key Laboratory of Supramolecular Structure and Materials, Jilin University (sklssm2024039), P. R. China.

Research Keywords

asymmetric covalent triazine framework
efficient selectivity
photocatalytic CO2 reduction

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This full text is made available under CC-BY 4.0. https://creativecommons.org/licenses/by/4.0/

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This output contributes to the following UN Sustainable Development Goals (SDGs)

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abstract = "The photocatalytic reduction of CO2 represents an environmentally friendly and sustainable approach for generating valuable chemicals. In this study, a thiophene-modified highly conjugated asymmetric covalent triazine framework (As-CTF-S) is developed for this purpose. Significantly, single-component intramolecular energy transfer can enhance the photogenerated charge separation, leading to the efficient conversion of CO2 to CO during photocatalysis. As a result, without the need for additional photosensitizers or organic sacrificial agents, As-CTF-S demonstrates the highest photocatalytic ability of 353.2 µmol g−1 and achieves a selectivity of ≈99.95% within a 4 h period under visible light irradiation. This study provides molecular insights into the rational control of charge transfer pathways for high-efficiency CO2 photoreduction using single-component organic semiconductor catalysts. {\textcopyright} 2024 The Authors. Advanced Science published by Wiley-VCH GmbH.",

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AU - Qi, Guang-Dong

AU - Ba, Dan

AU - Zhang, Yu-Jie

AU - Jiang, Xue-Qing

AU - Chen, Zihao

AU - Yang, Miao-Miao

AU - Cao, Jia-Min

AU - Dong, Wen-Wen

AU - Zhao, Jun

AU - Li, Dong-Sheng

AU - Zhang, Qichun

PY - 2024/7/24

Y1 - 2024/7/24

N2 - The photocatalytic reduction of CO2 represents an environmentally friendly and sustainable approach for generating valuable chemicals. In this study, a thiophene-modified highly conjugated asymmetric covalent triazine framework (As-CTF-S) is developed for this purpose. Significantly, single-component intramolecular energy transfer can enhance the photogenerated charge separation, leading to the efficient conversion of CO2 to CO during photocatalysis. As a result, without the need for additional photosensitizers or organic sacrificial agents, As-CTF-S demonstrates the highest photocatalytic ability of 353.2 µmol g−1 and achieves a selectivity of ≈99.95% within a 4 h period under visible light irradiation. This study provides molecular insights into the rational control of charge transfer pathways for high-efficiency CO2 photoreduction using single-component organic semiconductor catalysts. © 2024 The Authors. Advanced Science published by Wiley-VCH GmbH.

AB - The photocatalytic reduction of CO2 represents an environmentally friendly and sustainable approach for generating valuable chemicals. In this study, a thiophene-modified highly conjugated asymmetric covalent triazine framework (As-CTF-S) is developed for this purpose. Significantly, single-component intramolecular energy transfer can enhance the photogenerated charge separation, leading to the efficient conversion of CO2 to CO during photocatalysis. As a result, without the need for additional photosensitizers or organic sacrificial agents, As-CTF-S demonstrates the highest photocatalytic ability of 353.2 µmol g−1 and achieves a selectivity of ≈99.95% within a 4 h period under visible light irradiation. This study provides molecular insights into the rational control of charge transfer pathways for high-efficiency CO2 photoreduction using single-component organic semiconductor catalysts. © 2024 The Authors. Advanced Science published by Wiley-VCH GmbH.

KW - asymmetric covalent triazine framework

KW - efficient selectivity

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Constructing an Asymmetric Covalent Triazine Framework to Boost the Efficiency and Selectivity of Visible-Light-Driven CO₂ Photoreduction

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ITF: High Performance All-organic Rechargeable Sodium-ion Batteries Based on Covalent Organic Frameworks

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Constructing an Asymmetric Covalent Triazine Framework to Boost the Efficiency and Selectivity of Visible-Light-Driven CO2 Photoreduction

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ITF: High Performance All-organic Rechargeable Sodium-ion Batteries Based on Covalent Organic Frameworks

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Constructing an Asymmetric Covalent Triazine Framework to Boost the Efficiency and Selectivity of Visible-Light-Driven CO₂ Photoreduction