Citation: Aonan Wang, Jingwen Dai, Yiming Guo, Fanghua Ning, Xiaoyu Liu, Sidra Subhan, Jiaqian Qin, Shigang Lu, Jin Yi. Imidazolium bromide based dual-functional redox mediator for the construction of dendrite-free Li-CO₂ batteries[J]. Chinese Chemical Letters, ;2025, 36(7): 110186. doi: 10.1016/j.cclet.2024.110186 shu

Imidazolium bromide based dual-functional redox mediator for the construction of dendrite-free Li-CO₂ batteries

Aonan Wang ^a ,
Jingwen Dai ^a ,
Yiming Guo ^a ,
Fanghua Ning ^a ,
Xiaoyu Liu ^{a, b} ,
Sidra Subhan ^c ,
Jiaqian Qin ^d ,
Shigang Lu ^a ,
Jin Yi ^{a, *,}

a.
Institute for Sustainable Energy/College of Sciences, Shanghai University, Shanghai 200444, China
b.
Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), Nankai University, Tianjin 300071, China
c.
Department of Chemistry, Bacha Khan University Charsadda, KPK 24420, Pakistan
d.
Center of Excellence on Advanced Materials for Energy Storage, Metallurgy and Materials Science Research Institute, Chulalongkorn University, Bangkok 10330, Thailand

jin.yi@shu.edu.cn

Received Date: 7 May 2024
Revised Date: 9 June 2024
Accepted Date: 27 June 2024
Available Online: 27 June 2024

Figures(5)

Rechargeable lithium-carbon dioxide (Li-CO₂) batteries have emerged as a highly promising approach to simultaneously address energy shortages and the greenhouse effect. However, certain limitations exist in Li-CO₂ batteries like high charge overpotential and unstable Li metal interface, which adversely affect the energy efficiency and cycling life. The incorporation of soluble redox mediators (RMs) has proven effective in enhancing the charge transfer between lithium carbonate (Li₂CO₃) and cathode, thereby substantially reducing the charge overpotential. Nevertheless, the severe shuttle effect of RMs results in the reactions with Li anode, not only exacerbating the corrosion of Li anode but also leading to the depletion of RMs and electrical energy efficiency. In this work, an organic compound containing large cation group, 1-ethyl-3-methylimidazole bromide (EMIBr) is proposed as the defense donor RM for Li anode in Li-CO₂ batteries to address the above problems simultaneously. During charging, Li₂CO₃ oxidation kinetics can be accelerated by bromide anion pair (Br₃⁻/Br⁻). Meanwhile, the cations (EMI⁺) are preferentially adsorbed around the protruding tips of Li anode through electrostatic interaction driven by surface free energy, forming protective layers that effectively inhibit further Li deposition at these tips, which is verified by DFT calculations. Additionally, Li dendrites growth is inhibited by the electrostatic repulsion of polar groups in EMIBr, resulting in uniform Li deposition. Consequently, a lower overpotential (~1.17 V) and a longer cycle life (~200 cycles) have been obtained for Li-CO₂ battery incorporating EMIBr.
- Li-CO₂ battery,
- Electrolyte additive,
- Redox mediator,
- Ionic liquid,
- Electrostatic shielding,
- Overpotential
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通讯作者: 陈斌, bchen63@163.com

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沈阳化工大学材料科学与工程学院沈阳 110142

Imidazolium bromide based dual-functional redox mediator for the construction of dendrite-free Li-CO2 batteries

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通讯作者: 陈斌, bchen63@163.com

Imidazolium bromide based dual-functional redox mediator for the construction of dendrite-free Li-CO₂ batteries