Unravelling asynchronous oxidation of carbon and lithium carbonate during charging in lithium-carbon dioxide battery

IF 8.1 2区 工程技术 Q1 CHEMISTRY, PHYSICAL
Wanzhen Li , Wentao Wang , Ningxuan Zhu , Chuan Tan , Xiangwen Gao , Yuhui Chen
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Abstract

Lithium carbonate (Li2CO3) and carbon (C) play crucial roles as primary discharge products in lithium-carbon dioxide (Li-CO2) batteries. Understanding the reversible formation and oxidation of Li2CO3 and C during charge-discharge cycles is essential for the cyclic performance of Li-CO2 batteries. However, the role of the decomposition mechanisms of Li2CO3 and the C substrate remains debated, especially under real operating conditions. Here, we find that the discharge product C undergoes oxidation during charging, displaying non-synchronous oxidation compared to Li2CO3. Oxidation primarily involves C and the electrolyte in the early charging stages, producing CO2 and CO. In the later stages, the decomposition of Li2CO3 predominates, producing highly reactive CO3·- intermediates. Interestingly, after prolonged ball milling of lithium carbonate and carbon, the C elements can be exchanged through Li2CO3•C composite materials. By forming Li2CO3•C composites, C can be oxidized synchronously during the charging. Therefore, designing a catalyst to promote the reversible formation/decomposition of Li2CO3•C could be vital to achieving reversible cycling in Li-CO2 batteries.

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来源期刊
Journal of Power Sources
Journal of Power Sources 工程技术-电化学
CiteScore
16.40
自引率
6.50%
发文量
1249
审稿时长
36 days
期刊介绍: The Journal of Power Sources is a publication catering to researchers and technologists interested in various aspects of the science, technology, and applications of electrochemical power sources. It covers original research and reviews on primary and secondary batteries, fuel cells, supercapacitors, and photo-electrochemical cells. Topics considered include the research, development and applications of nanomaterials and novel componentry for these devices. Examples of applications of these electrochemical power sources include: • Portable electronics • Electric and Hybrid Electric Vehicles • Uninterruptible Power Supply (UPS) systems • Storage of renewable energy • Satellites and deep space probes • Boats and ships, drones and aircrafts • Wearable energy storage systems
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