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To improve the atomic utilization of metals and reduce the cost of industrialization, the one-step total monoatomization of macroscopic bulk metals, as opposed to nanoscale metals, is effective. In this study, we used a thermal diffusion method to directly convert commercial centimeter-scale Ni foam to porous Ni single-atom-loaded carbon nanotubes (CNTs). As expected, owing to the coating of single-atom on porous, highly conductive CNT carriers, Ni single-atom electrocatalysts (Ni-SACs) exhibit extremely high activity and selectivity in CO2 electroreduction (CO2RR), yielding a current density of > 350 mA/cm 2, a selectivity for CO of > 91% under a flow cell configuration using a 1 M potassium chloride (KCl) electrolyte. Based on the superior activity of the Ni-SACs electrocatalyst, an integrated gas-phase electrochemical zero-gap reactor was introduced to generate a significant amount of CO current for potential practical applications. The overall current can be increased to 800 mA, while maintaining CO Faradaic efficiencies (FEs) at above 90% per unit cell. Our findings and insights on the active site transformation mechanism for macroscopic bulk Ni foam conversion into single atoms can inform the design of highly active single-atom catalysts used in industrial CO 2RR systems.

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Publication history

Received: 14 March 2022
Revised: 24 April 2022
Accepted: 25 April 2022
Published: 07 June 2022

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© Tsinghua University Press 2022

Acknowledgements

Acknowledgements

This work was supported by the Young Scientists Fund of the National Natural Science Foundation of China (No. 22101182), Guangdong Basic and Applied Basic Research Foundation (No. 2020A1515110499), Shenzhen Science and Technology Program (No. JCYJ20210324095202006), Shenzhen University Young Teacher Research Project (No. 000002110713), the Shccig-Qinling Program (No. 2021JLM-27), and the Jinchuan Group Co. Ltd. Chemical Environmental Protection Industry Joint Laboratory (No. 20-0837).

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Email: nanores@tup.tsinghua.edu.cn

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