Lowering Charge Transfer Barrier of LiMn2O4 via Nickel Surface Doping To Enhance Li+ Intercalation Kinetics at Subzero Temperatures
Open accessAbstract
Sluggish interfacial kinetics leading to considerable loss of energy and power capabilities at subzero temperatures is still a big challenge to overcome for Li-ion batteries operating under extreme environmental conditions. Herein, using LiMn 2 O 4 as the model system, we demonstrated that nickel surface doping to construct a new interface owning lower charge transfer energy barrier, could effectively facilitate the interfacial process and inhibit the capacity loss with decreased temperature. Detailed investigations on the charge transfer process via electrochemical impedance spectroscopy and density functional theory calculation, indicate that the interfacial chemistry tuning could effectively lower the activation energy of charge transfer process by nearly 20%, endowing the cells with ∼75.4% capacity at −30 °C, far surpassing the hardly discharged unmodified counterpart. This control of surface chemistry to tune interfacial dynamics proposes insights and design ideas for batteries to well survive under thermal extremes.
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To compensate for low Li-ion conductivity and sluggish interfacial charge transfer kinetics, the cathode should have a small particle size and a structure with high ionic and electronic conductivity.
“In order to compensate for low Li-ion conductivity and sluggish interfacial charge transfer kinetics, the cathode should have a small particle size and a structure with high ionic and electronic conductivity6,7.”
From High-performance Na3V2(PO4)3/C cathode for efficient low-temperature lithium-ion batteries (2025) · cites this paper as [6]
In the Supporting Information Placeholder section (page not given), the paper identifies slow Li diffusion and sluggish charge transfer as low-temperature limitations and says nanostructures can shorten Li-ion diffusion paths. It does not recommend a cathode structure with high ionic and electronic conductivity; for interfacial charge transfer, it instead proposes lowering the energy barrier through nickel surface doping. (LLM, conf=0.86)
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Cited by
Sorted by citations
High-performance Na3V2(PO4)3/C cathode for efficient low-temperature lithium-ion batteries
Mukushev, I., Tyan, Y., Kalimuldina, G., Mukanova, A., Jakupova, Z., Kim, S.-S., Bakenov, Z., & Nurpeissova, A. (2025) · NPG Asia Materials · doi:10.1038/s41427-025-00591-x · Cited by 11 · see citing works
“The coin cells (CR2032) were assembled in an argon-fi lled glove box (Mbraun, Labmaster Pro DP) with lithium metal as anode and counter electrode, Whatman GF/D glass micro fi ber fi lter as separator and 1 M LiPF 6 in a mixture of ethyl carbonate (EC), dimethyl carbonate (DEC) and dimethyl carbonate (EMC) (1:1:1 in v/v)…”
- Authors
- Zhang, W., Sun, X., Tang, Y., Xia, H., Zeng, Y., Qiao, L., Zhu, Z., Lv, Z., Zhang, Y., Ge, X., Xi, S., Wang, Z., Du, Y., & Chen, X.
- Affiliations
- Nanyang Technological University (SG)
- University of Electronic Science and Technology of China (CN)
- Institute of Chemical and Engineering Sciences (SG)
- Corresponding author
- Du, Yonghua
- Chen, Xiaodong
- ORCID
- Venue
- Journal of the American Chemical Society
- Publisher
- American Chemical Society (ACS)
- Published
- 2019-08-25
- Volume
- 141
- Issue
- 36
- Pages
- 14038-14042
- ISSN
- 0002-7863 (ISSN-L)
- 1520-5126
- OpenAlex
- W2969579263
- Cited by
- 201
- References
- 4
- Citations by year
- 2026: 10 · 2025: 39 · 2024: 32 · 2023: 29 · 2022: 33 · 2021: 27 · 2020: 26 · 2019: 5
- FWCI
- 8.18
- Type
- journal article
- Language
- en
- Open access
- green
- hdl.handle.net
- Licence
- Locations
- Journal of the American Chemical Society (publishedVersion)
- PubMed (publishedVersion)
- DR-NTU (Nanyang Technological University) (submittedVersion)
- Funders
- National Research Foundation Singapore (NRF2015EWT-EIRP002-008)
- 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
- LiMn2O4, charge transfer barrier, subzero temperatures, low-temperature cycling, interfacial chemistry, capacity retention, activation energy, cathode materials, lithium-ion batteries
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