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Electroreduction of carbon dioxide into value-added fuels or chemicals using renewable energy helps to effectively reduce carbon dioxide emission and alleviate the greenhouse effect while storing intermittent energies. Due to the existing infrastructure of global natural gas utilization and distribution, methane produced in such a green route attracts wide interests. However, limited success has been witnessed in the practical application of catalysts imparting satisfactory methane activity and selectivity. Herein, we report the fabrication of an atomically dispersed Co-Cu alloy through the reconstruction of trace-Co doped Cu metal-organic framework. This catalyst exhibits a methane Faradaic efficiency of 60% ± 1% with the corresponding partial current density of 303 ± 5 mA·cm−2. Operando X-ray adsorption spectroscopy and attenuated-total-reflection surface enhanced infrared spectroscopy unravel that the introduction of atomically dispersed Co in Cu favors *CO protonation via enhancing surface water activation, and suppresses C−C coupling by reducing *CO coverage, thereby leading to high methane selectivity.


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Atomically dispersed Co-Cu alloy reconstructed from metal-organic framework to promote electrochemical CO2 methanation

Show Author's information Hao Sun1,2Ling Lin1,3Wei Hua1,3Xulan Xie1,3Qiaoqiao Mu1,3Kun Feng4Jun Zhong4Fenglei Lyu1,2Zhao Deng1,3Yang Peng1,2,5( )
Soochow Institute for Energy and Materials Innovations, College of Energy, Soochow University, Suzhou 215006, China
Jiangsu Key Laboratory of Advanced Negative Carbon Technologies, Soochow University, Suzhou 215006, China
Key Laboratory of Advanced Carbon Materials and Wearable Energy Technologies of Jiangsu Province, Soochow University, Suzhou 215006, China
Institute of Functional Nano & Soft Materials, Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Soochow University, Suzhou 215123, China
Soochow Municipal laboratory for low carbon technologies and industries, Soochow University, Suzhou 215006, China

Abstract

Electroreduction of carbon dioxide into value-added fuels or chemicals using renewable energy helps to effectively reduce carbon dioxide emission and alleviate the greenhouse effect while storing intermittent energies. Due to the existing infrastructure of global natural gas utilization and distribution, methane produced in such a green route attracts wide interests. However, limited success has been witnessed in the practical application of catalysts imparting satisfactory methane activity and selectivity. Herein, we report the fabrication of an atomically dispersed Co-Cu alloy through the reconstruction of trace-Co doped Cu metal-organic framework. This catalyst exhibits a methane Faradaic efficiency of 60% ± 1% with the corresponding partial current density of 303 ± 5 mA·cm−2. Operando X-ray adsorption spectroscopy and attenuated-total-reflection surface enhanced infrared spectroscopy unravel that the introduction of atomically dispersed Co in Cu favors *CO protonation via enhancing surface water activation, and suppresses C−C coupling by reducing *CO coverage, thereby leading to high methane selectivity.

Keywords: alloy, metal-organic framework, methane, electrochemical carbon dioxide reduction, catalyst reconstruction

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Publication history
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Acknowledgements

Publication history

Received: 28 May 2022
Revised: 29 June 2022
Accepted: 30 June 2022
Published: 01 August 2022
Issue date: March 2023

Copyright

© Tsinghua University Press 2022

Acknowledgements

Acknowledgements

This work was supported by the National Natural Science Foundation of China (Nos. 22072101 and 22075193), the Natural Science Foundation of Jiangsu Province (No. BK20211306), Six Talent Peaks Project in Jiangsu Province (No. TD-XCL-006), and the Priority Academic Program Development (PAPD) of Jiangsu Higher Education Institutions.

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