New Insight on the Role of Electrolyte Additives in Rechargeable Lithium Ion Batteries

Jun Ming, Zhen Cao, Yingqiang Wu, Wandi Wahyudi, Wenxi Wang, Xianrong Guo, Luigi Cavallo, Jang-Yeon Hwang, Atif Shamim, Lain-Jong Li, Yang-Kook Sun, Husam N. Alshareef

Research output: Contribution to journalArticlepeer-review

31 Scopus citations

Abstract

Solid electrolyte interphase (SEI)-forming agents such as vinylene carbonate, sulfone, and cyclic sulfate are commonly believed to be film-forming additives in lithium-ion batteries that help to enhance graphite anode stability. However, we find that the film-forming effect and the resultant SEI may not be the only reasons for the enhanced graphite stability. This is because the as-formed SEI cannot inhibit Li+–solvent co-intercalation once the additive is removed from the electrolyte. Instead, we show that the Li+ solvation structure, which is modified by these additives, plays a critical role in achieving reversible Li+ (de)intercalation within graphite. This discovery is confirmed in both carbonate and ether-based electrolytes. We show that the problem of graphite exfoliation caused by Li+–solvent co-intercalation can be mitigated by adding ethene sulfate to tune the Li+ coordination structure. This work brings new insight into the role of additives in electrolytes, expanding the prevailing thinking over the past 2 decades. In addition, this finding can guide the design of more versatile electrolytes for advanced rechargeable metal-ion batteries.
Original languageEnglish (US)
Pages (from-to)2613-2622
Number of pages10
JournalACS Energy Letters
Volume4
Issue number11
DOIs
StatePublished - Oct 11 2019

Fingerprint Dive into the research topics of 'New Insight on the Role of Electrolyte Additives in Rechargeable Lithium Ion Batteries'. Together they form a unique fingerprint.

Cite this