Cu–O/N single sites incorporated 2D covalent organic framework ultrathin nanobelts for highly selective visible-light-driven CO₂ reduction to CO
Developing heterogeneous catalysts with identifiable catalytic sites provides opportunities to explore their structure–activity relationship. Covalent organic framework (COF) represents an emerging class of porous materials that have exhibited great potential in various applications. Herein, a singl...
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sg-ntu-dr.10356-1731802024-01-19T15:31:59Z Cu–O/N single sites incorporated 2D covalent organic framework ultrathin nanobelts for highly selective visible-light-driven CO₂ reduction to CO Tu, Wenguang Yang, Yanqin Chen, Chunping Zhou, Tianhua Li, Tianhao Wang, Haojing Wu, Shuyang Zhou, Yong O’Hare, Dermot Zou, Zhigang Xu, Rong School of Chemistry, Chemical Engineering and Biotechnology C4T CREATE Science::Chemistry Reduction Reactions Ultrathin Nanobelts Developing heterogeneous catalysts with identifiable catalytic sites provides opportunities to explore their structure–activity relationship. Covalent organic framework (COF) represents an emerging class of porous materials that have exhibited great potential in various applications. Herein, a single-site heterogeneous photocatalyst consisting of 2D COF ultrathin nanobelts coordinated with single Cu–O/N sites (defined as Cu–COF) is synthesized and investigated for visible-light-driven CO2 reduction. The relatively weak N and O binding sites from the imine and methoxy groups of the organic linkers result in active Cu–O/N sites for charge transfer and CO2 reduction. The resultant Cu–COF with 0.2 wt% Cu only serves as a bifunctional photocatalyst for visible-light-driven CO2 reduction in the absence of a photosensitizer with triethanolamine as the sacrificial reagent. A high CO selectivity of 94% is obtained. This study further demonstrates the great potential of COFs in heterogeneous catalysis with the abundant choices of functional groups in the organic linkers. Nanyang Technological University National Research Foundation (NRF) Published version This work is supported by Nanyang Technological University and the National Research Foundation (NRF), Singapore, under its Campus for Research Excellence and Technological Enterprise (CREATE) program through the Carbon Reduction in Chemical Technology (C4T) program. Dr. W.T. and Prof. Z.Z. gratefully acknowledge the support by the Program from Guangdong Introducing Innovative and Entrepreneurial Teams (2019ZT08L101 and RCTDPT-2020-001), the University Development Fund (UDF01001159), the Shenzhen Key Laboratory of Eco-materials and Renewable Energy (ZDSYS20200922160400001), the Young Scientists Fund of the National Natural Science Foundation of China (Grant No. 52202306), and the Shenzhen Natural Science Foundation (GXWD20201231105722002-20200824163747001). 2024-01-16T06:49:50Z 2024-01-16T06:49:50Z 2023 Journal Article Tu, W., Yang, Y., Chen, C., Zhou, T., Li, T., Wang, H., Wu, S., Zhou, Y., O’Hare, D., Zou, Z. & Xu, R. (2023). Cu–O/N single sites incorporated 2D covalent organic framework ultrathin nanobelts for highly selective visible-light-driven CO₂ reduction to CO. Small Structures, 4(6), 2200233-. https://dx.doi.org/10.1002/sstr.202200233 2688-4062 https://hdl.handle.net/10356/173180 10.1002/sstr.202200233 2-s2.0-85174870457 6 4 2200233 en Small Structures © 2022 The Authors. Small Structures published by Wiley-VCH GmbH. This is an open access article under the terms of the Creative Commons Attribution License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited. application/pdf |
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Science::Chemistry Reduction Reactions Ultrathin Nanobelts Tu, Wenguang Yang, Yanqin Chen, Chunping Zhou, Tianhua Li, Tianhao Wang, Haojing Wu, Shuyang Zhou, Yong O’Hare, Dermot Zou, Zhigang Xu, Rong Cu–O/N single sites incorporated 2D covalent organic framework ultrathin nanobelts for highly selective visible-light-driven CO₂ reduction to CO |
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Developing heterogeneous catalysts with identifiable catalytic sites provides opportunities to explore their structure–activity relationship. Covalent organic framework (COF) represents an emerging class of porous materials that have exhibited great potential in various applications. Herein, a single-site heterogeneous photocatalyst consisting of 2D COF ultrathin nanobelts coordinated with single Cu–O/N sites (defined as Cu–COF) is synthesized and investigated for visible-light-driven CO2 reduction. The relatively weak N and O binding sites from the imine and methoxy groups of the organic linkers result in active Cu–O/N sites for charge transfer and CO2 reduction. The resultant Cu–COF with 0.2 wt% Cu only serves as a bifunctional photocatalyst for visible-light-driven CO2 reduction in the absence of a photosensitizer with triethanolamine as the sacrificial reagent. A high CO selectivity of 94% is obtained. This study further demonstrates the great potential of COFs in heterogeneous catalysis with the abundant choices of functional groups in the organic linkers. |
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School of Chemistry, Chemical Engineering and Biotechnology |
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School of Chemistry, Chemical Engineering and Biotechnology Tu, Wenguang Yang, Yanqin Chen, Chunping Zhou, Tianhua Li, Tianhao Wang, Haojing Wu, Shuyang Zhou, Yong O’Hare, Dermot Zou, Zhigang Xu, Rong |
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Article |
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Tu, Wenguang Yang, Yanqin Chen, Chunping Zhou, Tianhua Li, Tianhao Wang, Haojing Wu, Shuyang Zhou, Yong O’Hare, Dermot Zou, Zhigang Xu, Rong |
author_sort |
Tu, Wenguang |
title |
Cu–O/N single sites incorporated 2D covalent organic framework ultrathin nanobelts for highly selective visible-light-driven CO₂ reduction to CO |
title_short |
Cu–O/N single sites incorporated 2D covalent organic framework ultrathin nanobelts for highly selective visible-light-driven CO₂ reduction to CO |
title_full |
Cu–O/N single sites incorporated 2D covalent organic framework ultrathin nanobelts for highly selective visible-light-driven CO₂ reduction to CO |
title_fullStr |
Cu–O/N single sites incorporated 2D covalent organic framework ultrathin nanobelts for highly selective visible-light-driven CO₂ reduction to CO |
title_full_unstemmed |
Cu–O/N single sites incorporated 2D covalent organic framework ultrathin nanobelts for highly selective visible-light-driven CO₂ reduction to CO |
title_sort |
cu–o/n single sites incorporated 2d covalent organic framework ultrathin nanobelts for highly selective visible-light-driven co₂ reduction to co |
publishDate |
2024 |
url |
https://hdl.handle.net/10356/173180 |
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1789483223581982720 |