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Nano Research 2024, 17(4): 2410-2419 https://doi.org/10.1007/s12274-023-6083-2
Research Article | Issue | Published: 14 September 2023

Hydroxylated metal–organic-layer nanocages anchoring single atomic cobalt sites for robust photocatalytic CO2 reduction

Show Author's Information Weiyi Pan1,2,  Zhihe Wei1,2,  Yanhui Su1,2,  Yuebin Lian3,  Zhangyi Zheng1,2,  Huihong Yuan1,2,  Yongze Qin1,2,  Xulan Xie1,2,  Qianqian Bai1,2,  Zhenyang Jiao1,2,  Wei Hua1,2,  Jinzhou Chen1,2,  Wenjun Yang1,2,  Zhao Deng1,2( ),  Yang Peng1,2,4( )
Soochow Institute for Energy and Materials Innovations, College of Energy, Soochow University, Suzhou 215006, China
Key Laboratory of Advanced Carbon Materials and Wearable Energy Technologies of Jiangsu Province, Soochow University, Suzhou 215006, China
School of Photoelectric Engineering, Changzhou institute of technology, Changzhou 213032, China
Jiangsu Key Laboratory for Advanced Negative Carbon Technologies, Soochow University, Suzhou 215123, China
Keywords:
single-atom catalyst, photocatalytic CO2 reduction, co-catalyst, nanocage, metal–organic layer
Topics:
Photocatalysis
Cite this article:
Pan W, Wei Z, Su Y, et al. Hydroxylated metal–organic-layer nanocages anchoring single atomic cobalt sites for robust photocatalytic CO2 reduction. Nano Research, 2024, 17(4): 2410-2419. https://doi.org/10.1007/s12274-023-6083-2
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Abstract Full text Electronic supplementary material About this article

Assembly of two-dimensional (2D) metal–organic layers (MOLs) based on the hard and soft acid–base theorem represents an exquisite strategy for the construction of photocatalytic platforms in virtue of the highly exposed active sites, much improved mass transport, and greatly elevated stability. Herein, nanocages composed of MOLs are produced for the first time through a cosolvent approach utilizing zirconium-based UiO-66-(OH)2 as the structural precursor. To endow the catalytic activity for CO2 conversion, single atomic Co2+ sites are appended to the Zr-oxo nodes of the MOL cages, demonstrating a remarkable CO yield of 7.74 mmol·g−1·h−1 and operational stability of 97.1% product retention after five repeated cycles. Such an outstanding photocatalytic performance is mainly attributed to the unique nanocage morphology comprising enormous 2D nanosheets for augmented Co2+ exposure and the abundant surface hydroxyl groups for local CO2 enrichment. This work underlines the tailoring of both metal–organic framework (MOF) morphology and functionality to boost the turnover rate of photocatalytic CO2 reduction reaction (CO2RR).


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Electronic supplementary material
About this article

Hydroxylated metal–organic-layer nanocages anchoring single atomic cobalt sites for robust photocatalytic CO2 reduction

Show Author's information Weiyi Pan1,2, Zhihe Wei1,2, Yanhui Su1,2, Yuebin Lian3, Zhangyi Zheng1,2, Huihong Yuan1,2, Yongze Qin1,2, Xulan Xie1,2, Qianqian Bai1,2, Zhenyang Jiao1,2, Wei Hua1,2, Jinzhou Chen1,2, Wenjun Yang1,2, Zhao Deng1,2( ), Yang Peng1,2,4( )
Soochow Institute for Energy and Materials Innovations, College of Energy, Soochow University, Suzhou 215006, China
Key Laboratory of Advanced Carbon Materials and Wearable Energy Technologies of Jiangsu Province, Soochow University, Suzhou 215006, China
School of Photoelectric Engineering, Changzhou institute of technology, Changzhou 213032, China
Jiangsu Key Laboratory for Advanced Negative Carbon Technologies, Soochow University, Suzhou 215123, China

Abstract

Assembly of two-dimensional (2D) metal–organic layers (MOLs) based on the hard and soft acid–base theorem represents an exquisite strategy for the construction of photocatalytic platforms in virtue of the highly exposed active sites, much improved mass transport, and greatly elevated stability. Herein, nanocages composed of MOLs are produced for the first time through a cosolvent approach utilizing zirconium-based UiO-66-(OH)2 as the structural precursor. To endow the catalytic activity for CO2 conversion, single atomic Co2+ sites are appended to the Zr-oxo nodes of the MOL cages, demonstrating a remarkable CO yield of 7.74 mmol·g−1·h−1 and operational stability of 97.1% product retention after five repeated cycles. Such an outstanding photocatalytic performance is mainly attributed to the unique nanocage morphology comprising enormous 2D nanosheets for augmented Co2+ exposure and the abundant surface hydroxyl groups for local CO2 enrichment. This work underlines the tailoring of both metal–organic framework (MOF) morphology and functionality to boost the turnover rate of photocatalytic CO2 reduction reaction (CO2RR).

Keywords: single-atom catalyst, photocatalytic CO2 reduction, co-catalyst, nanocage, metal–organic layer

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Publication history
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Acknowledgements

Publication history

Received: 15 June 2023
Revised: 02 August 2023
Accepted: 10 August 2023
Published: 14 September 2023
Issue date: April 2024

Copyright

© Tsinghua University Press 2023

Acknowledgements

Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (Nos. 22075193 and 22072101), the Natural Science Foundation of Jiangsu Province (Nos. BK20221239, BK20211306, and BK20220027), the Six Talent Peaks Project in Jiangsu Province (No. TD-XCL-006), and the Priority Academic Program Development (PAPD) of Jiangsu Higher Education Institutions. Besides, we also acknowledge the support from Soochow Municipal Laboratory for low carbon technologies and industries.

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