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

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. 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.

Authors:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [2]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [4]; ORCiD logo [1]
  1. Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division
  2. Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
  3. Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
  4. Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division; University of Tennessee, Knoxville, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC); USDOE Laboratory Directed Research and Development (LDRD) Program
OSTI Identifier:
1985387
Alternate Identifier(s):
OSTI ID: 2000211
Grant/Contract Number:  
AC05-00OR22725; AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Carbon
Additional Journal Information:
Journal Volume: 212; Journal Issue: N/A; Journal ID: ISSN 0008-6223
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; electrochemical conversion of CO2; graphite; eutectic carbonate melts; high-rate anode; lithium-ion batteries; LIBs

Citation Formats

Thapaliya, Bishnu Prasad, Ivanov, Alexander S., Chao, Hsin-Yun, Lamm, Meghan, Chi, Miaofang, Meyer III, Harry M., Sun, Xiao-Guang, Aytug, Tolga, Dai, Sheng, and Mahurin, Shannon M. Molten salt electrochemical upcycling of CO2 to graphite for high performance battery anodes. United States: N. p., 2023. Web. doi:10.1016/j.carbon.2023.118151.
Thapaliya, Bishnu Prasad, Ivanov, Alexander S., Chao, Hsin-Yun, Lamm, Meghan, Chi, Miaofang, Meyer III, Harry M., Sun, Xiao-Guang, Aytug, Tolga, Dai, Sheng, & Mahurin, Shannon M. Molten salt electrochemical upcycling of CO2 to graphite for high performance battery anodes. United States. https://doi.org/10.1016/j.carbon.2023.118151
Thapaliya, Bishnu Prasad, Ivanov, Alexander S., Chao, Hsin-Yun, Lamm, Meghan, Chi, Miaofang, Meyer III, Harry M., Sun, Xiao-Guang, Aytug, Tolga, Dai, Sheng, and Mahurin, Shannon M. Sat . "Molten salt electrochemical upcycling of CO2 to graphite for high performance battery anodes". United States. https://doi.org/10.1016/j.carbon.2023.118151.
@article{osti_1985387,
title = {Molten salt electrochemical upcycling of CO2 to graphite for high performance battery anodes},
author = {Thapaliya, Bishnu Prasad and Ivanov, Alexander S. and Chao, Hsin-Yun and Lamm, Meghan and Chi, Miaofang and Meyer III, Harry M. and Sun, Xiao-Guang and Aytug, Tolga and Dai, Sheng and Mahurin, Shannon M.},
abstractNote = {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. 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.},
doi = {10.1016/j.carbon.2023.118151},
journal = {Carbon},
number = N/A,
volume = 212,
place = {United States},
year = {Sat May 20 00:00:00 EDT 2023},
month = {Sat May 20 00:00:00 EDT 2023}
}

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