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Proximity-independent acid–base synergy in a solid ZrOxHy catalyst for amine regeneration in post-combustion CO2 capture

Nature Catalysis volume 8, pages 270–281 (2025)Cite this article

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Abstract

Post-combustion CO2 capture with amines offers an almost ready-to-use capture technology to assist in the transition towards net-zero carbon emission. However, the technology suffers from a high regeneration cost due to the high process temperatures involved. Utilization of catalysts in the regeneration process was reported to be an elegant solution to lower process temperatures while maintaining high reaction kinetics. Earlier studies were performed under batch conditions and therefore lack practical validation, and a deeper mechanistic understanding of the catalysis is also missing. This study introduces a practical-to-synthesize, highly efficient, stable and recyclable ZrOxHy solid catalyst, showing high catalytic CO2 desorption rates for most common aqueous amine solutions. Kinetic and ex situ/in situ spectroscopic data reveal a proximity-independent acid–base synergistic mechanism between two catalytic cycles. The approach was validated in a fixed-bed continuous reactor, demonstrating sensible contact time shortening (up to 85%), suggesting considerable potential savings in regeneration energy, reactor construction and amine solvent cost.

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Fig. 1: Catalytic performance of ZrOxHy.
Fig. 2: Catalyst characterization.
Fig. 3: Structure–activity relationship and the proposed catalytic route.
Fig. 4: Operando ATR-FTIR spectroscopy to determine the acid–base synergistic mechanism.
Fig. 5: A first industrial application perspective.

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Data availability

The data supporting findings of this study are available within the paper and its Supplementary Information, or from the authors on reasonable request.

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Acknowledgements

We thank W. Vermandel and L. Utiu for kind technical support. Y.L. thanks the National Natural Science Foundation of China (52176213), C.Z. thanks the Chinese Scholarship Council (201906310137) for financial support, M.D. acknowledges FWO infrastructure projects (AKUL13/19 and I000920N) and B.F.S. acknowledges TotalEnergies for financial support.

Author information

Authors and Affiliations

  1. Center for Sustainable Catalysis and Engineering, KU Leuven, Heverlee, Belgium

    Cheng Zhou, Mostafa Torka Beydokhti, Fatima Rammal, Michiel Dusselier & Bert F. Sels

  2. TotalEnergies OneTech Belgium, Feluy, Belgium

    Parveen Kumar & Walter Vermeiren

  3. TotalEnergies Research & Technology Gonfreville, Harfleur, France

    Maxime Lacroix

  4. Guangzhou Institute of Energy Conversion, Chinese Academy of Sciences, Guangzhou, People’s Republic of China

    Yuhe Liao

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Contributions

C.Z., Y.L. and B.F.S. designed the experiments. C.Z., M.T.B. and F.R. performed the experiments. C.Z., M.T.B., Y.L. and B.F.S. analysed the data. C.Z. wrote the paper with guidance from B.F.S., Y.L., P.K., M.L., W.V. and M.D. provided valuable input in data analysis and comments on the paper.

Corresponding authors

Correspondence to Yuhe Liao or Bert F. Sels.

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This work is partly funded by TotalEnergies.

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Nature Catalysis thanks Maohong Fan and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary Methods, Figs. 1–22, Tables 1–4 and Refs. 1–5.

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Zhou, C., Beydokhti, M.T., Rammal, F. et al. Proximity-independent acid–base synergy in a solid ZrOxHy catalyst for amine regeneration in post-combustion CO2 capture. Nat Catal 8, 270–281 (2025). https://doi.org/10.1038/s41929-025-01307-8

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