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

61 Citations (Scopus)

118 Downloads (CityUHK Scholars)

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.

UN SDGs

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

SDG 13 Climate Action

Research Keywords

asymmetric covalent triazine framework
efficient selectivity
photocatalytic CO2 reduction

Publisher's Copyright Statement

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

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

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.",

keywords = "asymmetric covalent triazine framework, efficient selectivity, photocatalytic CO2 reduction",

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

year = "2024",

month = jul,

day = "24",

doi = "10.1002/advs.202402645",

language = "English",

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journal = "Advanced Science",

issn = "2198-3844",

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T1 - Constructing an Asymmetric Covalent Triazine Framework to Boost the Efficiency and Selectivity of Visible-Light-Driven CO2 Photoreduction

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

KW - photocatalytic CO2 reduction

UR - https://www.scopus.com/pages/publications/85192824184

UR - https://www.scopus.com/pages/publications/85192824184#tab=impact

U2 - 10.1002/advs.202402645

DO - 10.1002/advs.202402645

M3 - RGC 21 - Publication in refereed journal

C2 - 38738739

SN - 2198-3844

VL - 11

JO - Advanced Science

JF - Advanced Science

IS - 28

M1 - 2402645

ER -

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

Abstract

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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

Abstract

Funding

UN SDGs

Research Keywords

Publisher's Copyright Statement

ESI Highly Cited Papers

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Projects

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

Cite this

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