Identifying the components of the solid–electrolyte interphase in Li-ion batteries
Abstract
The importance of the solid-electrolyte interphase (SEI) for reversible operation of Li-ion batteries has been well established, but the understanding of its chemistry remains incomplete. The current consensus on the identity of the major organic SEI component is that it consists of lithium ethylene di-carbonate (LEDC), which is thought to have high Li-ion conductivity, but low electronic conductivity (to protect the Li/C electrode). Here, we report on the synthesis and structural and spectroscopic characterizations of authentic LEDC and lithium ethylene mono-carbonate (LEMC). Direct comparisons of the SEI grown on graphite anodes suggest that LEMC, instead of LEDC, is likely to be the major SEI component. Single-crystal X-ray diffraction studies on LEMC and lithium methyl carbonate (LMC) reveal unusual layered structures and Li+ coordination environments. LEMC has Li+ conductivities of >1 × 10-6 S cm-1, while LEDC is almost an ionic insulator. The complex interconversions and equilibria of LMC, LEMC and LEDC in dimethyl sulfoxide solutions are also investigated.
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LEMC, instead of LEDC, becomes the major organic component in the SEI on graphite anodes in LiPF6-EC/DMC electrolytes after prolonged cycling.
“Their results show that lithium ethylene mono-carbonate (LEMC), instead of lithium ethylene di-carbonate (LEDC), becomes the major organic components in the SEI on graphite anodes in LiPF 6 -EC/DMC electrolytes, after prolonged cycling.”
From Review on Low-Temperature Electrolytes for Lithium-Ion and Lithium Metal Batteries (2023) · cites this paper as [30]
Section 1.5 describes analyzing the SEI on graphite after three cycles in LiPF6/EC/DMC, using LEMC and LEDC as reference materials. Supplementary Figure 26 reports that LEMC was more persistent than LEDC in separate reaction tests, but those tests do not establish which compound dominates the graphite SEI. The available passages do not support the claim that LEMC becomes its major organic component after prolonged cycling. (LLM, conf=0.78)
Experimental — accuracy not yet measuredPropylene carbonate cannot be used in graphite-anode-containing battery systems as the major or single solvent due to solvent co-intercalation and exfoliation of graphite anodes.
“However, it could not be used in graphite anode contained battery systems as the major/single solvent due to the solvent co-intercalation and exfoliation of the graphite anodes [30,31].”
From Review on Low-Temperature Electrolytes for Lithium-Ion and Lithium Metal Batteries (2023) · cites this paper as [30]
Section 1.4 describes graphite-electrode tests using DMC and EC electrolytes, but does not address propylene carbonate. Searches for propylene carbonate, co-intercalation, and exfoliation found no passage supporting the claimed restriction or its cause. Page numbers were not available in the indexed passages. (LLM, conf=0.74)
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Self-citation
- Authors
- Wang, L., Menakath, A., Han, F., Wang, Y., Zavalij, P. Y., Gaskell, K. J., Borodin, O., Iuga, D., Brown, S. P., Wang, C., Xu, K., & Eichhorn, B. W.
- Affiliations
- University of Maryland, College Park (US)
- University of Warwick (GB)
- DEVCOM Army Research Laboratory (US)
- Corresponding author
- Wang, Chunsheng
- Xu, Kang
- Eichhorn, Bryan W.
- ORCID
- Venue
- Nature Chemistry
- Published
- 2019-08-19
- Volume
- 11
- Issue
- 9
- Pages
- 789-796
- ISSN
- 1755-4330 (ISSN-L)
- 1755-4349
- OpenAlex
- W2967719016
- Cited by
- 514
- References
- 0
- Citations by year
- 2026: 41 · 2025: 73 · 2024: 78 · 2023: 100 · 2022: 74 · 2021: 76 · 2020: 64 · 2019: 8
- FWCI
- 19.96
- Type
- journal article
- Language
- en
- Open access
- closed
- Locations
- Nature Chemistry (publishedVersion)
- PubMed (publishedVersion)
- Warwick Research Archive Portal (University of Warwick) (acceptedVersion)
- Topics
- Physical Sciences › Engineering › Electrical and Electronic Engineering › Advancements in Battery Materials
- Physical Sciences › Engineering › Electrical and Electronic Engineering › Advanced Battery Materials and Technologies
- Physical Sciences › Engineering › Automotive Engineering › Advanced Battery Technologies Research
- Keywords
- solid electrolyte interphase, lithium-ion batteries, graphite anode, lithium ion conductivity, ionic insulators, layered structure, lithium coordination, SEI composition, electrolyte decomposition
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