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CO2 fixation into carbon nanofibres using electrochemical–thermochemical tandem catalysis

Nature Catalysis volume 7, pages 98–109 (2024)Cite this article

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Abstract

Carbon dioxide (CO2) fixation into value-added solid carbon such as carbon nanofibres (CNF) for longer-term storage represents a promising avenue for achieving net-negative carbon emissions. However, directly converting CO2 to CNF via thermocatalytic approaches faces thermodynamic constraints, while electrocatalytic methods typically lead to amorphous carbon with limited yields or require energy-intensive conditions (>720 °C). Here, we present an electrocatalytic–thermocatalytic tandem strategy for CNF production, which circumvents the aforementioned thermodynamic limitations by integrating the co-electrolysis of CO2 and water into syngas (CO and H2) with a subsequent thermochemical process at relatively mild conditions (370–450 °C, 1 atm), yielding CNF at a high production rate (average 2.5 gcarbon gmetals−1 h−1). The optimal coordinated actions of FeCo alloy and extra metallic Co were ascertained to enhance the dissociative activation of syngas and favour the carbon–carbon bond formation to produce CNF. This tandem strategy opens a door to leverage renewable energy for decarbonizing CO2 into valuable solid carbon products while producing renewable H2.

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Fig. 1: Feasibility and demonstration of CNF formation from the CO and H2 reaction.
Fig. 2: In situ structural characterizations of CeO2-supported FeCo-based catalysts.
Fig. 3: Theoretical studies on the stability and reactivity of iron–cobalt catalysts.
Fig. 4: Electrochemical–thermochemical tandem process for producing CNFs and renewable H2.

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The source data that support the findings of this study are available from the corresponding authors on reasonable request. Source data are provided with this paper.

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Acknowledgements

This work was financially supported by the Division of Chemical Sciences, Geosciences and Biosciences, Office of Basic Energy Sciences (grant numbers DE-SC0012704 and DE-FG02-13ER16381). This research used resources of the Center for Functional Nanomaterials (CFN) and beamlines 7-BM (QAS) and 8-ID (ISS) of the National Synchrotron Light Source II (NSLS-II) at Brookhaven National Laboratory (contract nos DE-SC0012704 and DE-SC0012653), US DOE Office of Science User Facilities. Beamline operations were supported in part by the Synchrotron Catalysis Consortium (US DOE, Office of Basic Energy Sciences, grant no. DE-SC0012335). We acknowledge the assistance of Z. Lin, A. Ooi and D. Huang in performing Raman and ICP measurements. The DFT calculations were performed using computational resources at the Center for Functional Nanomaterials, a user facility at Brookhaven National Laboratory and at the National Energy Research Scientific Computing Center (NERSC), which is supported by the Office of Science of the US DOE under contract no. DE-AC02-05CH11231. S.G. acknowledges the National Science Foundation Graduate Research Fellowship Program (DGE-2036197).

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  1. These authors contributed equally: Zhenhua Xie, Erwei Huang.

Authors and Affiliations

  1. Department of Chemical Engineering, Columbia University, New York, NY, USA

    Zhenhua Xie, Samay Garg & Jingguang G. Chen

  2. Chemistry Division, Brookhaven National Laboratory, Upton, NY, USA

    Zhenhua Xie, Erwei Huang, Ping Liu & Jingguang G. Chen

  3. Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton, NY, USA

    Sooyeon Hwang

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Contributions

Z.X., S.G. and J.G.C. conceived the idea and designed the research; Z.X. carried out catalyst synthesis, reactions, in situ synchrotron measurements, product separation, energy cost and CO2 emission assessments, and analysis of all the experimental data; Z.X. and S.H. performed the electron microscopy imaging; S.G. contributed to the discussion, conducted Raman and ICP measurements, and assisted with the materials preparation and electrochemical experiments. E.H. conducted all the DFT calculations and theoretical data analysis under the supervision of P.L. and J.G.C.; Z.X. and E.H. prepared the initial draft; Z.X., E.H., S.G., P.L. and J.G.C. reviewed and revised the manuscript; and J.G.C. and P.L. supervised the whole project.

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Correspondence to Ping Liu or Jingguang G. Chen.

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Supplementary information

Supplementary Information

Supplementary Methods, Discussion, Figs. 1–57 and Tables 1–16.

Supplementary Data 1

DFT-optimized atomic coordinates information.

Source data

Source Data Fig. 1

Feasibility and demonstration of CNF formation.

Source Data Fig. 2

In situ structural characterizations.

Source Data Fig. 3

Theoretical studies on catalyst stability and reactivity.

Source Data Fig. 4

Electrochemical–thermochemical tandem-reactor experimental results.

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Xie, Z., Huang, E., Garg, S. et al. CO2 fixation into carbon nanofibres using electrochemical–thermochemical tandem catalysis. Nat Catal 7, 98–109 (2024). https://doi.org/10.1038/s41929-023-01085-1

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