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Electrified reversible surface mineralization of CO2 for direct air capture

Nature Energy (2026)Cite this article

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Abstract

Electrified CO2 capture and release from air offers net-negative emissions, but today’s liquid-carbonate-based systems have a high energy cost (6–10 GJ per ton of CO2), and organic sorbents are oxygen sensitive. Here we report electrified CO2 surface mineralization/demineralization capture/release, wherein an inorganic capture sorbent, MnO2, is electrochemically reduced/activated to generate Mn(III), which mineralizes CO2 to form MnOOCO2H (operando Raman); the process is reversed under oxidative potential. This approach is built upon Mn redox reaction that resides within the water-stable bracket, offering tunable driving force (kinetics/productivity) with applied potential (energy). After optimizing the electrochemical protocol, we capture from air (0.04% CO2 and 21% O2) at 4.1 GJ per ton of CO2, with capacity and kinetics comparable to prior sorbents, low sensitivity to oxygen/humidity, 80% single-pass CO2 capture ratio and release under a pure CO2 carrier gas stream and pressure drop <150 Pa. The system operates >1,000 h with >90% capacity retention and scales to 20 cm2 without loss; remaining challenges include material utilization, electrolyte, gas flow/pressure drop and CO2-purity management.

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Fig. 1: Electrified capture/release devices and chemical concepts, including eCO2-sMDCR.
Fig. 2: Proof-of-concept of the eCO2-sMDCR device and mechanistic study using operando Raman spectroscopy.
Fig. 3: Direct air capture performance of eCO2-sMDCR devices.
Fig. 4: Direct air capture durability evaluation of the eCO2-sMDCR device.

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The authors declare that all data supporting the major findings are available in the main text or the Supplementary Information. Source data are provided with this paper.

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Acknowledgements

This work made use of the Northwestern University Micro/Nano Fabrication Facility (NUFAB) facility of Northwestern University’s Atomic and Nanoscale Characterization Experimental Center (NUANCE), which has received support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (National Science Foundation, NSF ECCS-2025633), the International Institute for Nanotechnology (IIN) and Northwestern’s Materials Research Science and Engineering Center (MRSEC) programme (NSF DMR-2308691). W.A.G. thanks Department of Energy (DOE) (SC-0022230) for support. DFT calculations were also supported through computational resources and staff contributions provided for the Quest high-performance computing facility at Northwestern University, which is jointly supported by the Office of the Provost, the Office of Research and Northwestern University Information Technology. Funding: this work was financially supported by TotalEnergies SE.

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Author notes

  1. These authors contributed equally: Zeyan Liu, Huajie Ze, Bosi Peng.

Authors and Affiliations

  1. Department of Chemistry, Northwestern University, Evanston, IL, USA

    Zeyan Liu, Huajie Ze, Bosi Peng, Charles B. Musgrave III, Mohammad K. Shehab, Hyun Seung Jung, Hengzhou Liu, Kent O. Kirlikovali, Omar K. Farha, Ke Xie & Edward H. Sargent

  2. Department of Electrical and Computer Engineering, Northwestern University, Evanston, IL, USA

    Zeyan Liu, Huajie Ze, Bosi Peng, Charles B. Musgrave III, Hyun Seung Jung, Hengzhou Liu, Ke Xie & Edward H. Sargent

  3. Materials and Process Simulation Center, California Institute of Technology, Pasadena, CA, USA

    Charles B. Musgrave III & William A. Goddard III

  4. International Institute for Nanotechnology, Northwestern University, Evanston, IL, USA

    Mohammad K. Shehab, Kent O. Kirlikovali & Omar K. Farha

  5. Department of Chemical and Biological Engineering, Northwestern University, Evanston, IL, USA

    Omar K. Farha

  6. Paula M. Trienens Institute for Sustainability and Energy, Northwestern University, Evanston, IL, USA

    Omar K. Farha & Edward H. Sargent

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Contributions

Conceptualization: K.X., E.H.S., Z.L. and B.P. Materials synthesis, device development, testing methodology development and experimental validation: Z.L. and B.P. Materials structural characterization: B.P. Raman experiments design, measurement and interpretation: H.Z. Simulation studies: C.B.M. Adsorption isotherm characterization: M.K.S. Supplementary three-electrode investigations: Z.L., H.S.J. and H.L. Supervision: W.A.G., K.O.K., O.K.F., K.X. and E.H.S. Funding acquisition: O.K.F. and E.H.S. Writing–original draft: Z.L., B.P. and H.Z. Writing–reviewing and editing: Z.L., B.P., M.K.S., H.L., K.O.K, O.K.F., K.X. and E.H.S.

Corresponding authors

Correspondence to Ke Xie or Edward H. Sargent.

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Competing interests

Z.L., K.X. and E.H.S. are filling a patent based on this work. The remaining authors declare no competing interests.

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Nature Energy thanks the anonymous reviewers for their contribution to the peer review of this work.

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Supplementary Notes 1 and 2, Figs. 1–23 and Tables 1–3.

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Statistical source data for averaged results.

Source Data Fig. 4 (download XLSX )

Statistical source data for averaged results.

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Liu, Z., Ze, H., Peng, B. et al. Electrified reversible surface mineralization of CO2 for direct air capture. Nat Energy (2026). https://doi.org/10.1038/s41560-026-01989-9

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