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Tandem amine scrubbing and CO2 electrolysis via direct piperazine carbamate reduction

Nature Energy (2025)Cite this article

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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.

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Fig. 1: Feedstock-producing route comparison and tandem amine scrubbing and CO2 electrolysis.
Fig. 2: Amine absorbents structures and the screening rationale.
Fig. 3: Reaction equations and speciation conditions of PZ upon bubbling CO2.
Fig. 4: Diffusion properties of amine and KHCO3 solutions.
Fig. 5: Catalyst investigation and mechanistic studies.
Fig. 6: Performance in scale-up electrolyser and system-level energy analysis.

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The authors declare that all data supporting the findings of this study are available within the paper, Supplementary Information and Source data files. Source data are provided with this paper.

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Acknowledgements

We would like to thank the financial support from the Australian Research Council (ARC) through Future Fellowship (FT210100298, FT210100806), DECRA (DE230101068), Discovery Project (DP220100603), Linkage Project (LP220100088, LP210200504, LP210200345, LP210100467, LP230200897), Industrial Transformation Training Centre (IC180100005) and Industrial Transformation Research Hub (IH240100009) schemes, the Australian Government through the Cooperative Research Centres Projects (CRCPXIII000077) and the Australian Renewable Energy Agency (ARENA) as part of ARENA’s Transformative Research Accelerating Commercialization Program (TM021) and European Commission’s Australia-Spain Network for Innovation and Research Excellence (AuSpire). P.L. would like to thank Australian Nuclear Science and Technology Organisation (ANSTO) for providing beamline access and technical support to complete X-ray absorption spectroscopy (XAS) tests at the Australian Synchrotron via the Medium Energy X-ray (MEX) beamline (beamtime: M20409/M21349). We acknowledge the use of the instruments and scientific and technical assistance at RMIT Microscopy and Microanalysis Facility (RMMF) and the Monash Centre for Electron Microscopy, a Node of Microscopy Australia (ARC LE0454166). The computational study is supported by the Marsden Fund Council from Government funding (21–UOA–237) and Catalyst: Seeding General Grant (22–UOA–031–CGS), managed by Royal Society Te Apārangi. Z.W. and Y.M. acknowledge the use of New Zealand eScience Infrastructure (NeSI) high-performance computing facilities, consulting support and/or training services as part of this research. G.I.N.W. and Y.M. acknowledge funding support from the MacDiarmid Institute for Advanced Materials and Nanotechnology, the Energy Education Trust of New Zealand and the Royal Society Te Apārangi.

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  1. These authors contributed equally: Peng Li, Yu Mao, Heejong Shin.

Authors and Affiliations

  1. School of Science, RMIT University, Melbourne, Victoria, Australia

    Peng Li, Yitong Li, Kyle Hearn, Baohua Jia & Tianyi Ma

  2. School of Chemical Sciences, University of Auckland, Auckland, New Zealand

    Yu Mao, Geoffrey I. N. Waterhouse & Ziyun Wang

  3. Department of Chemical and Biomolecular Engineering, Institute of Emergent Materials, Sogang University, Seoul, Republic of Korea

    Heejong Shin

  4. CSIRO Manufacturing, Clayton, Victoria, Australia

    Qi Yang, Xuan Cheng & Roger Mulder

  5. Department of Energy and Resources Engineering, College of Engineering, Peking University, Beijing, China

    Kangkang Li

  6. CSIRO Energy, Mayfield West, New South Wales, Australia

    Hai Yu, Yong Zhao & Zhi Zheng

  7. Institute for Superconducting & Electronic Materials, Australian Institute for Innovative Materials, University of Wollongong, Wollongong, New South Wales, Australia

    Wei Kong Pang

  8. Institute of Technology for Carbon Neutrality, Shenzhen Institutes of Advanced Technology, Chinese Academy of Sciences, Shenzhen, China

    Huanyu Jin

  9. Australian Synchrotron, Clayton, Victoria, Australia

    Emily Finch

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Contributions

P.L. and T.M. conceived the idea, designed the study, prepared the catalysts and conducted catalyst characterizations and electrochemical tests. H.S. and P.L. conducted full-cell electrolyser tests. Y.M. and Z.W. conducted the DFT calculations and Gaussian simulations. X.C. did the electron microscopy characterizations. H.J. H.Y. and W.K.P. collected the FTIR spectra data. Q.Y., K.L. and K.H. conducted the 13C NMR test. R.M. contributed to the diffusion tests. Z.Z., Y.Z. and E.F. did the XAS test. Y.L., B.J. and G.I.N.W. discussed the electrochemical data.

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Correspondence to Ziyun Wang or Tianyi Ma.

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P.L. and T.M. are listed as inventors on a patent application filed by RMIT University that pertains to this work (PCT/AU2025/050293). The other authors declare no competing interests.

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Li, P., Mao, Y., Shin, H. et al. Tandem amine scrubbing and CO2 electrolysis via direct piperazine carbamate reduction. Nat Energy (2025). https://doi.org/10.1038/s41560-025-01869-8

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