Abstract

One strategy for addressing the climate crisis caused by CO2 emissions is to efficiently convert CO2 to advanced materials suited for green and clean energy technology applications. Porous carbon is widely used as an advanced energy storage material because of its enhanced energy storage capabilities as an anode. Herein, we report electrochemical CO2 upcycling to solid carbon with a controlled microstructure and porosity in a ternary molten carbonate melt at 450 °C. Controlling the electrochemical parameters (voltage, temperature, cathode material) enabled the conversion of CO2 to porous carbon with a tunable morphology and porosity for the first time at such a low temperature. Additionally, a well-controlled morphology and porosity are beneficial for reversible energy storage. In fact, these carbon materials delivered high specific capacity, stable cycling performances, and exceptional rate capability even under extremely fast charging conditions when integrated as an anode in lithium-ion batteries (LIBs). The present approach not only demonstrated efficient upcycling of CO2 into porous carbon suitable for enhanced energy storage but can also contribute to a clean and green energy technology that can reduce carbon emissions to achieve sustainable energy goals.

Original languageEnglish
Pages (from-to)2251-2262
Number of pages12
JournalACS Applied Materials and Interfaces
Volume16
Issue number2
DOIs
StatePublished - Jan 17 2024

Funding

This research was 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 the 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 the Argonne National Laboratory under contract no. DE-AC02-06CH11357. This manuscript has been authored by UT-Battelle, LLC, under contract number DE-AC05-00OR22725, with the US Department of Energy (DOE). The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a nonexclusive, 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 ). Acknowledgments

Keywords

  • electrochemical CO upcycling
  • eutectic ternary melts
  • lithium-ion batteries (LIBs)
  • mesopores
  • micropores
  • porous carbon anode

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