Molten salt electrochemical upcycling of CO2 to graphite for high performance battery anodes

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Abstract

The efficient transformation of CO2 into a value-added material is a potential strategy to help mitigate climate effects caused by CO2 emissions. One potential CO2 conversion product is graphite which is an important and versatile material extensively used in many applications including as an anode for lithium-ion batteries (LIBs). Commercial graphite, however, is traditionally synthesized via the energy intensive Acheson process (>3000 °C) and the performance of such graphite can be limited under fast charging conditions which is important for vehicle electrification. Herein, we report the electrochemical transformation of CO2 to highly crystalline nano-graphite with a controlled microstructure in a carbonate molten salt at 780 °C. The use of a nickel foam electrode and controlled electrochemical parameters during the molten salt conversion process yielded pure graphite at a lower temperature compared to the Acheson process. Moreover, when investigated as an anode material for LIBs, the CO2-converted graphite exhibited high reversible capacity, long cycle life, and excellent rate capability even under fast charging conditions. This process provides a way to potentially reduce carbon emissions through the utilization of waste CO2 by converting it into value-added graphite suitable for fast charging, high-energy-density batteries for vehicle electrification.

Original languageEnglish
Article number118151
JournalCarbon
Volume212
DOIs
StatePublished - Aug 2023

Funding

This manuscript has been authored in part by UT-Battelle, LLC, under contract DE-AC05-00OR22725 with the US Department of Energy (DOE) and supported by the DOE Office of Fossil Energy. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a non-exclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. The DOE will provide public access to these results of federally sponsored research under the DOE Public Access Plan ( http://energy.gov/downloads/doe-public-access-plan ). Research sponsored by the Laboratory Directed Research and Development Program of Oak Ridge National Laboratory , managed by UT-Battelle, LLC, for the U. S. Department of Energy . The microscopy work was supported by an Early Career project supported by DOE Office of Science FWP #ERKCZ55–KC040304. All microscopy technique development was performed and supported by Oak Ridge National Laboratory's (ORNL) Center for Nanophase Materials Sciences (CNMS) , which is a DOE Office of Science User Facility. This research used resources of the Advanced Photon Source, a DOE User Facility, operated for the DOE Office of Science by Argonne National Laboratory under contract no. DE-AC02-06CH11357. Research sponsored by the Laboratory Directed Research and Development Program of Oak Ridge National Laboratory, managed by UT-Battelle, LLC, for the U. S. Department of Energy. The microscopy work was supported by an Early Career project supported by DOE Office of Science FWP #ERKCZ55–KC040304. All microscopy technique development was performed and supported by Oak Ridge National Laboratory's (ORNL) Center for Nanophase Materials Sciences (CNMS), which is a DOE Office of Science User Facility. This research used resources of the Advanced Photon Source, a DOE User Facility, operated for the DOE Office of Science by Argonne National Laboratory under contract no. DE-AC02-06CH11357.☆ This manuscript has been authored in part by UT-Battelle, LLC, under contract DE-AC05-00OR22725 with the US Department of Energy (DOE) and supported by the DOE Office of Fossil Energy. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a non-exclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. The DOE will provide public access to these results of federally sponsored research under the DOE Public Access Plan (http://energy.gov/downloads/doe-public-access-plan).

FundersFunder number
Center for Nanophase Materials Sciences
DOE Public Access Plan
United States Government
U.S. Department of Energy
Office of Fossil Energy
Office of ScienceFWP #ERKCZ55–KC040304
Argonne National LaboratoryDE-AC05-00OR22725, DE-AC02-06CH11357
Oak Ridge National Laboratory

    Keywords

    • Electrochemical conversion of CO
    • Eutectic carbonate melts
    • Graphite
    • High-rate anode
    • Lithium-ion batteries (LIBs)

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