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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Main Authors: Tu, Wenguang, Yang, Yanqin, Chen, Chunping, Zhou, Tianhua, Li, Tianhao, Wang, Haojing, Wu, Shuyang, Zhou, Yong, O’Hare, Dermot, Zou, Zhigang, Xu, Rong
Other Authors: School of Chemistry, Chemical Engineering and Biotechnology
Format: Article
Language:English
Published: 2024
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Online Access:https://hdl.handle.net/10356/173180
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Institution: Nanyang Technological University
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spelling 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
institution Nanyang Technological University
building NTU Library
continent Asia
country Singapore
Singapore
content_provider NTU Library
collection DR-NTU
language English
topic Science::Chemistry
Reduction Reactions
Ultrathin Nanobelts
spellingShingle 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
description 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.
author2 School of Chemistry, Chemical Engineering and Biotechnology
author_facet 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
format Article
author 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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