Lithium–CO2 batteries are attractive energy‐storage systems for fulfilling the demand of future large‐scale applications such as electric vehicles due to their high specific energy density. However, a major challenge with Li–CO2 batteries is to attain reversible formation and decomposition of the Li2CO3 and carbon discharge products. A fully reversible Li–CO2 battery is developed with overall carbon neutrality using MoS2 nanoflakes as a cathode catalyst combined with an ionic liquid/dimethyl sulfoxide electrolyte. This combination of materials produces a multicomponent composite (Li2CO3/C) product. The battery shows a superior long cycle life of 500 for a fixed 500 mAh g−1 capacity per cycle, far exceeding the best cycling stability reported in Li–CO2 batteries. The long cycle life demonstrates that chemical transformations, making and breaking covalent C-O bonds can be used in energy‐storage systems. Theoretical calculations are used to deduce a mechanism for the reversible discharge/charge processes and explain how the carbon interface with Li2CO3 provides the electronic conduction needed for the oxidation of Li2CO3 and carbon to generate the CO2 on charge. This achievement paves the way for the use of CO2 in advanced energy‐storage systems.
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This content will become publicly available on October 1, 2024
Improved cycle performance of Li-CO2 batteries with nickel manganite supported carbon nanotube NiMn2O4 @CNT cathode
Rechargeable Li-CO2 batteries have emerged as promising candidates for next generation batteries due to their low cost, high theoretical capacity, and ability to capture the greenhouse gas CO2. However, these batteries still face challenges such as slow reaction kinetic and short cycle performance due to the accumulation of discharge products. To address this issue, it is necessary to design and develop high efficiency electrocatalysts that can improve CO2 reduction reaction. In this study, we report the use of NiMn2O4 electrocatalysts combined with multiwall carbon nanotubes as a cathode material in the Li-CO2 batteries. This combination proved effective in decomposing discharge products and enhancing cycle performance. The battery shows stable discharge–charge cycles for at least 30 cycles with a high limited capacity of 1000 mAh/g at current density of 100 mA/g. Furthermore, the battery with the NiMn2O4@CNT catalyst exhibits a reversible discharge capacity of 2636 mAh/g. To gain a better understanding of the reaction mechanism of Li-CO2 batteries, spectroscopies and microscopies were employed to identify the chemical composition of the discharge products. This work paves a pathway to increase cycle performance in metal-CO2 batteries, which could have significant implications for energy storage and the reduction of greenhouse gas emissions.
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- Award ID(s):
- 2119688
- NSF-PAR ID:
- 10433404
- Editor(s):
- Doron Aurbach
- Date Published:
- Journal Name:
- Journal of the Electrochemical Society
- ISSN:
- 0013-4651
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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