Chemical Origin of in Situ Carbon Dioxide Outgassing from a Cation-Disordered Rock Salt Cathode

© 2024 The Authors. Published by American Chemical Society.

Bibliographische Detailangaben
Veröffentlicht in:Chemistry of materials : a publication of the American Chemical Society. - 1998. - 36(2024), 13 vom: 09. Juli, Seite 6535-6546
1. Verfasser: Huang, Tzu-Yang (VerfasserIn)
Weitere Verfasser: Cai, Zijian, Crafton, Matthew J, Giovine, Raynald, Patterson, Ashlea, Hau, Han-Ming, Rastinejad, Justin, Rinkel, Bernardine L D, Clément, Raphaële J, Ceder, Gerbrand, McCloskey, Bryan D
Format: Online-Aufsatz
Sprache:English
Veröffentlicht: 2024
Zugriff auf das übergeordnete Werk:Chemistry of materials : a publication of the American Chemical Society
Schlagworte:Journal Article
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520 |a In situ carbon dioxide (CO2) outgassing is a common phenomenon in lithium-ion batteries (LiBs), primarily due to parasitic side reactions at the cathode-electrolyte interface. However, little is known about the chemical origins of the in situ CO2 released from emerging Li-excess cation-disordered rock salt (DRX) cathodes. In this study, we selectively labeled various carbon sources with 13C in cathodes containing a representative DRX material, Li1.2Mn0.4Ti0.4O2 (LMTO), and performed differential electrochemical mass spectrometry (DEMS) during galvanostatic cycling in a carbonate-based electrolyte. When charging LMTO cathodes, electrolyte solvent (EC) decomposition is the dominant source of the CO2 outgassing. The amount of EC-originated CO2 is strongly correlated with the total surface area of carbon black in the electrode, revealing the critical role of electron-conducting carbon additives in the electrolyte degradation mechanisms. In addition, unusual bimodal CO2 evolution during the first cycle is found to originate from carbon black oxidation. Overall, the underlying chemical origin of in situ CO2 release during battery cycling is highly voltage- and cycle-dependent. This work further provides insights into improving the stability of DRX cathodes in LiBs and is envisioned to help guide future relevant material design to mitigate parasitic reactions in DRX-based batteries 
650 4 |a Journal Article 
700 1 |a Cai, Zijian  |e verfasserin  |4 aut 
700 1 |a Crafton, Matthew J  |e verfasserin  |4 aut 
700 1 |a Giovine, Raynald  |e verfasserin  |4 aut 
700 1 |a Patterson, Ashlea  |e verfasserin  |4 aut 
700 1 |a Hau, Han-Ming  |e verfasserin  |4 aut 
700 1 |a Rastinejad, Justin  |e verfasserin  |4 aut 
700 1 |a Rinkel, Bernardine L D  |e verfasserin  |4 aut 
700 1 |a Clément, Raphaële J  |e verfasserin  |4 aut 
700 1 |a Ceder, Gerbrand  |e verfasserin  |4 aut 
700 1 |a McCloskey, Bryan D  |e verfasserin  |4 aut 
773 0 8 |i Enthalten in  |t Chemistry of materials : a publication of the American Chemical Society  |d 1998  |g 36(2024), 13 vom: 09. Juli, Seite 6535-6546  |w (DE-627)NLM098194763  |x 0897-4756  |7 nnns 
773 1 8 |g volume:36  |g year:2024  |g number:13  |g day:09  |g month:07  |g pages:6535-6546 
856 4 0 |u http://dx.doi.org/10.1021/acs.chemmater.4c00756  |3 Volltext 
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