Tandem amine scrubbing and CO2 electrolysis via direct piperazine carbamate reduction

Peng Li, Yu Mao, Heejong Shin, Qi Yang, Xuan Cheng, Yitong Li, Kangkang Li, Hai Yu, Roger Mulder, Wei Kong Pang, Huanyu Jin, Yong Zhao, Zhi Zheng, Emily Finch, Kyle Hearn, Baohua Jia, Geoffrey I. N. Waterhouse, Ziyun Wang () and Tianyi Ma ()
Additional contact information
Peng Li: RMIT University
Yu Mao: University of Auckland
Heejong Shin: Sogang University
Qi Yang: CSIRO Manufacturing
Xuan Cheng: CSIRO Manufacturing
Yitong Li: RMIT University
Kangkang Li: Peking University
Hai Yu: CSIRO Energy
Roger Mulder: CSIRO Manufacturing
Wei Kong Pang: University of Wollongong
Huanyu Jin: Chinese Academy of Sciences
Yong Zhao: CSIRO Energy
Zhi Zheng: CSIRO Energy
Emily Finch: Australian Synchrotron
Kyle Hearn: RMIT University
Baohua Jia: RMIT University
Geoffrey I. N. Waterhouse: University of Auckland
Ziyun Wang: University of Auckland
Tianyi Ma: RMIT University

Nature Energy, 2025, vol. 10, issue 10, 1262-1273

Abstract: Abstract Transforming CO2 into valuable products presents a promising route for reducing emissions across various industry sectors. However, conventional methods, including sequential CO2 electrolysis or reverse water–gas shift reaction, depend on energy-intensive CO2 purification; while emerging reactive CO2 capture strategies still face challenges in designing optimal system components that enable efficient electrochemical regeneration without compromising catalytic performance. Here we systematically screen a broad library of amine-based absorbents to establish a design rationale for tandem amine scrubbing and CO2 electrolysis. We identify piperazine as an optimal capture medium and show that its carbamate form can be directly reduced using a nickel single-atom catalyst. This charge-neutral intermediate facilitates spontaneous adsorption, rapid transport and efficient C–N bond cleavage, enabling stable carbon monoxide production alongside in situ amine regeneration. The process achieves an energy efficiency of ~48.8 GJ per tonne CO, offering a scalable and energy efficient pathway towards carbon-neutral chemical feedstocks.

Date: 2025
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DOI: 10.1038/s41560-025-01869-8

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