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Boosting a practical Li-CO2 battery through dimerization reaction based on solid redox mediator.

Wei Li1, Menghang Zhang1, Xinyi Sun1

  • 1Center of Energy Storage Materials & Technology, College of Engineering and Applied Sciences, Jiangsu Key Laboratory of Artificial Functional Materials, National Laboratory of Solid-State Microstructures and Collaborative Innovation Center of Advanced Microstructures, Nanjing University, Nanjing, 210093, PR China.

Nature Communications
|January 27, 2024
PubMed
Summary
This summary is machine-generated.

This study introduces a novel solid redox mediator for lithium-carbon dioxide (Li-CO2) batteries, enhancing energy conversion efficiency. The new mediator facilitates efficient CO2 capture and promotes stable battery cycling for practical applications.

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Area of Science:

  • Electrochemistry
  • Materials Science
  • Energy Storage

Background:

  • Lithium-carbon dioxide (Li-CO2) batteries offer a pathway for CO2 utilization and electricity generation.
  • Direct electrocatalytic reduction of CO2 in Li-CO2 batteries often leads to Li2CO3 formation, reducing voltage and efficiency.
  • Soluble redox mediators face challenges like shuttle effects and sluggish kinetics.

Purpose of the Study:

  • To develop an effective solid redox mediator system for Li-CO2 batteries.
  • To overcome the limitations of direct CO2 reduction and soluble redox mediators.
  • To improve the voltage, efficiency, and cycling stability of Li-CO2 batteries.

Main Methods:

  • A solid redox mediator system was designed using a Cu(II) coordination compound of benzene-1,3,5-tricarboxylic acid affixed to the cathode.
  • Electrochemical reduction of the Cu(II) mediator to Cu(I) was performed.
  • The performance of the Li-CO2 battery with the solid redox mediator was evaluated through discharge/charge cycling and voltage measurements.

Main Results:

  • The Cu(I) solid redox mediator efficiently captured CO2, promoting Li2C2O4 formation via a dimeric oxalate intermediate.
  • The Li-CO2 battery achieved a higher discharge voltage (2.8 V) and lower charge potential (3.7 V).
  • Superior cycling performance exceeding 400 cycles was observed, alongside the development of a functional Li-CO2 pouch battery.

Conclusions:

  • Solid redox mediators, specifically the Cu(II) coordination compound, effectively enhance Li-CO2 battery performance by facilitating CO2 conversion.
  • This approach mitigates issues associated with direct CO2 reduction and soluble mediators, improving energy efficiency and stability.
  • The successful demonstration of a Li-CO2 pouch battery signifies progress towards the practical application of metal-CO2 batteries.