The Role of Cesium Cation in Controlling Interphasial Chemistry on Graphite Anode in Propylene Carbonate-Rich Electrolytes
Abstract
Despite the potential advantages it brings, such as wider liquid range and lower cost, propylene carbonate (PC) is seldom used in lithium-ion batteries because of its sustained cointercalation into the graphene structure and the eventual graphite exfoliation. Here, we report that cesium cation (Cs(+)) directs the formation of solid electrolyte interphase on graphite anode in PC-rich electrolytes through its preferential solvation by ethylene carbonate (EC) and the subsequent higher reduction potential of the complex cation. Effective suppression of PC-decomposition and graphite-exfoliation is achieved by adjusting the EC/PC ratio in electrolytes to allow a reductive decomposition of Cs(+)-(EC)m (1 ≤ m ≤ 2) complex preceding that of Li(+)-(PC)n (3 ≤ n ≤ 5). Such Cs(+)-directed interphase is stable, ultrathin, and compact, leading to significant improvement in battery performances. In a broader context, the accurate tailoring of interphasial chemistry by introducing a new solvation center represents a fundamental breakthrough in manipulating interfacial reactions that once were elusive to control.
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CsPF6 additive suppresses PC decomposition and graphite exfoliation by preferential solvation of Cs+ by EC and reductive decomposition of the Cs+-(EC)m complex preceding that of Li+-(PC)n.
“The PC decomposition and graphite exfoliation were effectively suppressed by adjusting the EC/PC ratio in electrolytes to achieve a reductive decomposition of Cs + -(EC) m (1 ⩽ m ⩽ 2) complex preceding that of Li + -(PC) n (3⩽ n ⩽ 5) (Fig. 17a).”
From Review on Low-Temperature Electrolytes for Lithium-Ion and Lithium Metal Batteries (2023) · cites this paper as [140]
The Cs+-containing interphase is stable, ultrathin, and compact, leading to significant improvement in battery performance.
“Such Cs + containing interphase is stable, ultrathin, and compact, leading to significant improvement in battery performance.”
From Review on Low-Temperature Electrolytes for Lithium-Ion and Lithium Metal Batteries (2023) · cites this paper as [140]
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Review on Low-Temperature Electrolytes for Lithium-Ion and Lithium Metal Batteries
Tan, S., Shadike, Z., Cai, X., Lin, R., Kludze, A., Borodin, O., Lucht, B. L., Wang, C., Hu, E., Xu, K., et al. (2023) · Electrochemical Energy Reviews · doi:10.1007/s41918-023-00199-1 · Cited by 118 · see citing works
“For example, Xu’s group reported using 0.04 M CsPF 6 as additive in 1 M LiPF 6 EC:PC:EMC (2:1:7, weight ratio) electrolyte [140] through the preferential solvation by EC of Cs + and the subsequent higher reduction potential of the complex cation.”
InfluentialSelf-citationGuo, R., & Han, W. (2022) · Materials Today Sustainability · doi:10.1016/j.mtsust.2022.100187 · Cited by 32 · see citing works
- Authors
- Xiang, H., Mei, D., Yan, P., Bhattacharya, P., Burton, S. D., von Wald Cresce, A., Cao, R., Engelhard, M. H., Bowden, M. E., Zhu, Z., Polzin, B. J., Wang, C.-M., Xu, K., Zhang, J.-G., & Xu, W.
- Affiliations
- Hefei University of Technology (CN)
- Argonne National Laboratory (US)
- Pacific Northwest National Laboratory (US)
- Sensor and Electron Devices Directorate, U.S. Army Research Laboratory, Adelphi, Maryland 20783, United States
- DEVCOM Army Research Laboratory (US)
- Corresponding author
- Xu, Wu
- ORCID
- Venue
- ACS Applied Materials & Interfaces
- Publisher
- American Chemical Society (ACS)
- Published
- 2015-09-10
- Volume
- 7
- Issue
- 37
- Pages
- 20687-20695
- ISSN
- 1944-8244 (ISSN-L)
- 1944-8252
- OpenAlex
- W2290675733
- Cited by
- 48
- References
- 0
- Citations by year
- 2026: 1 · 2025: 1 · 2024: 3 · 2023: 9 · 2022: 4 · 2021: 3 · 2020: 4 · 2019: 6 · 2018: 4 · 2017: 8 · 2016: 5
- FWCI
- 2.73
- Type
- journal article
- Language
- en
- Open access
- closed
- Locations
- ACS Applied Materials & Interfaces (publishedVersion)
- PubMed (publishedVersion)
- Funders
- Office of Energy Efficiency and Renewable Energy (DE-AC02-05CH11231)
- U.S. Department of Energy (DE-AC05-76RLO1830, DE-EE0006543)
- National Natural Science Foundation of China (21006033, 51372060)
- Ministry of Education of the People's Republic of China (2013HGCH0002)
- 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
- cesium cation, solid electrolyte interphase, graphite anode, propylene carbonate, ethylene carbonate, electrolyte solvation, co-intercalation, graphite exfoliation, electrolyte decomposition, lithium-ion batteries
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