Tailoring Low-Temperature Performance of a Lithium-Ion Battery via Rational Designing Interphase on an Anode
Abstract
Performances of lithium-ion batteries at subambient temperatures are extremely restricted by the resistive interphases originated from electrolyte decomposition, especially on the anode surface. This work reports a novel strategy that an anode interphase of low impedance is constructed by applying an electrolyte additive dimethyl sulfite (DMS). Electrochemical measurements indicate that the as-constructed interphase provides graphite/LiNi 0.5 Co 0.2 Mn 0.3 O 2 pouch cells with excellent low-temperature performance, outperforming the interphase constructed by 1,3,2-dioxathiolane 2,2-dioxide (DTD), a common commercially used electrolyte additive. Spectral characterizations in combination with theoretical calculations demonstrate that the improved performance is attributed to the unique molecular structure of DMS, which presents appropriate reduction activity and constructs the more stable and ionically conductive anode interphase due to the weaker combination of its reduction product with lithium ions than DTD. This rational design of interphases via an additive structure has been proven to be a low cost but rather an effective approach to tailor the performances of lithium-ion batteries.
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The DTD system had lower resistance than baseline at room temperature, but at low temperature its charge transfer resistance increased significantly and was higher than baseline, implying sluggish charge transfer of DTD-formed SEIs at low temperatures.
“The DTD system also had lower resistance compared to baseline at RT, while the charge transfer resistance of the DTD system at LT increased significantly and was even higher than the baseline electrolyte, implying sluggish charge transfer of DTD formed SEIs at LTs.”
From Review on Low-Temperature Electrolytes for Lithium-Ion and Lithium Metal Batteries (2023) · cites this paper as [130]
There are competing arguments in the literature that improved battery performance at low temperatures was obtained by decreasing inorganic species including LiF in SEIs.
“there are competing arguments regarding the effects of inorganic components of SEIs in the literature claiming that improved battery performance was obtained at LTs by decreasing inorganic species including LiF in SEIs.”
From Review on Low-Temperature Electrolytes for Lithium-Ion and Lithium Metal Batteries (2023) · cites this paper as [130]
The DMS reduction product CH3OSO has lower binding energy with Li+ than DTD (OCH2CH2SO3), suggesting faster ionic migration through such SEI.
“DMS reduction products (CH 3 OSO) has lower binding energy with Li + compared that of DTD (OCH 2 CH 2 SO 3 ), suggesting a faster ionic migration through such SEI.”
From Review on Low-Temperature Electrolytes for Lithium-Ion and Lithium Metal Batteries (2023) · cites this paper as [130]
Cells using DMS electrolytes delivered 74.28% of RT capacity at -20 °C and C/2, followed by DTD-based cells (68.64%) and electrolyte without additive (66.44%).
“The cells using DMS electrolytes showed the best results (Fig. 15d), which delivered 74.28% of RT capacity, followed by the DTD-based cell (68.64%) and the electrolyte without additive (66.44%).”
From Review on Low-Temperature Electrolytes for Lithium-Ion and Lithium Metal Batteries (2023) · cites this paper as [130]
The DMS-based electrolyte system had the lowest Rsei and Rct at both room and low temperatures, indicating more ionically conductive SEIs formed by DMS.
“According to EIS results, the DMSbased electrolyte system had the lowest R sei and R ct at both RT and LT, indicating more ionic conductive SEIs formed by DMS.”
From Review on Low-Temperature Electrolytes for Lithium-Ion and Lithium Metal Batteries (2023) · cites this paper as [130]
Lower amounts of LiF and Li2CO3 were generated in DMS-presence, indicating a more protective nature of the as-formed SEI from DMS.
“Based on the XPS results (Fig. 15c), lower amounts of LiF and Li 2 CO 3 were generated by decomposition of carbonate electrolytes and LiPF 6 in DMS-presence, indicating more protective nature of as-formed SEI from DMS.”
From Review on Low-Temperature Electrolytes for Lithium-Ion and Lithium Metal Batteries (2023) · cites this paper as [130]
CH3OSO experienced less structural change after combining with Li+ compared to DTD, implying a stabler structure in this SEI.
“CH 3 OSO experienced less structural change after combining with Li + compared to DTD, implying a stabler structure in this SEI.”
From Review on Low-Temperature Electrolytes for Lithium-Ion and Lithium Metal Batteries (2023) · cites this paper as [130]
Cites
Electrolytes and Interphases in Li-Ion Batteries and Beyond
Xu, K. (2014) · Chemical Reviews · doi:10.1021/cr500003w · Cited by 5,566 · see citing works
Self-citationLiao, B., Li, H., Xu, M., Xing, L., Liao, Y., Ren, X., Fan, W., Yu, L., Xu, K., & Li, W. (2018) · Advanced Energy Materials · doi:10.1002/aenm.201800802 · Cited by 292 · see citing works
Self-citationYang, B., Zhang, H., Yu, L., Fan, W., & Huang, D. (2016) · Electrochimica Acta · doi:10.1016/j.electacta.2016.10.037 · Cited by 156 · see citing works
Self-citationYang, T., Fan, W., Wang, C., Lei, Q., Ma, Z., Yu, L., Zuo, X., & Nan, J. (2018) · ACS Applied Materials & Interfaces · doi:10.1021/acsami.8b04743 · Cited by 92 · see citing works
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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
“They compared the performance using DMS and DTD as additives in 1 M LiPF 6 in EC:EMC (1:2, weight ratio) [130].”
Self-citationGuo, R., & Han, W. (2022) · Materials Today Sustainability · doi:10.1016/j.mtsust.2022.100187 · Cited by 32 · see citing works
Self-citation
- Authors
- Guo, R., Che, Y., Lan, G., Lan, J., Li, J., Xing, L., Xu, K., Fan, W., Yu, L., & Li, W.
- Affiliations
- South China Normal University (CN)
- DEVCOM Army Research Laboratory (US)
- Guangzhou Tinci Material Technology Co., Ltd, Guangzhou 510760, China
- Corresponding author
- Xu, K.
- Li, Weishan
- Venue
- ACS Applied Materials & Interfaces
- Publisher
- American Chemical Society (ACS)
- Published
- 2019-09-25
- Volume
- 11
- Issue
- 41
- Pages
- 38285-38293
- ISSN
- 1944-8244 (ISSN-L)
- 1944-8252
- OpenAlex
- W2977201496
- Cited by
- 113
- References
- 4
- Citations by year
- 2026: 16 · 2025: 14 · 2024: 14 · 2023: 33 · 2022: 17 · 2021: 11 · 2020: 7 · 2019: 1
- FWCI
- 3.24
- Type
- journal article
- Language
- en
- Open access
- closed
- Licence
- Locations
- ACS Applied Materials & Interfaces (publishedVersion)
- PubMed (publishedVersion)
- Funders
- the National Key Research and Development Program of China (2018YFB0104000)
- the key project of Science and Technology in Guangdong Province (2017A010106006)
- Topics
- Physical Sciences › Engineering › Electrical and Electronic Engineering › Advancements in Battery Materials
- Physical Sciences › Engineering › Automotive Engineering › Advanced Battery Technologies Research
- Physical Sciences › Engineering › Electrical and Electronic Engineering › Advanced Battery Materials and Technologies
- Keywords
- lithium-ion batteries, low-temperature performance, electrolyte additives, dimethyl sulfite, graphite anode, NCM cathode, electrolyte decomposition, interfacial resistance, molecular structure design
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