Detrimental Effects of Chemical Crossover from the Lithium Anode to Cathode in Rechargeable Lithium Metal Batteries
Abstract
Interfacial stability is one of the crucial factors for long-term cyclability of lithium (Li) metal batteries (LMBs). While cross-contamination phenomena have been well-studied in Li-ion batteries (LIBs), similar phenomena have rarely been reported in LMBs. Here, we investigated cathode failure triggered by chemical crossover from the anode in LMBs. In contrast to LIBs, the cathode in LMBs suffers more significant capacity fading, and its capacity cannot be fully recovered by replacing the Li anode. In-depth surface characterization reveals severe deterioration related to the accumulation of highly resistive polymeric components in the cathode–electrolyte interphase. The soluble byproducts generated by extensive electrolyte decomposition at the Li metal surface can diffuse toward the cathode side, resulting in severe deterioration of the cathode and separator surfaces. A selective Li-ion permeable separator with a polydopamine coating has been developed to mitigate the detrimental chemical crossover and enhance the cathode stability.
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Cycled NVP/C shows additional LiF (136.69 eV) and LixPOyFz (135.35 eV) peaks in the P 2p spectrum.
“Cycled NVP/C demonstrated additional LiF (136.69 eV) and LixPOyFz(135.35 eV) peaks, which also show the formation of the passivation layer46.”
From High-performance Na3V2(PO4)3/C cathode for efficient low-temperature lithium-ion batteries (2025) · cites this paper as [46]
The additional LiF and LixPOyFz peaks after cycling show the formation of the passivation layer.
“Cycled NVP/C demonstrated additional LiF (136.69 eV) and LixPOyFz(135.35 eV) peaks, which also show the formation of the passivation layer46.”
From High-performance Na3V2(PO4)3/C cathode for efficient low-temperature lithium-ion batteries (2025) · cites this paper as [46]
Cites
Ageing mechanisms in lithium-ion batteries
Vetter, J., Novák, P., Wagner, M. R., Veit, C., Möller, K.-C., Besenhard, J. O., Winter, M., Wohlfahrt-Mehrens, M., Vogler, C., & Hammouche, A. (2005) · Journal of Power Sources · doi:10.1016/j.jpowsour.2005.01.006 · Cited by 3,987 · see citing works
High rate and stable cycling of lithium metal anode
Qian, J., Henderson, W. A., Xu, W., Bhattacharya, P., Engelhard, M., Borodin, O., & Zhang, J.-G. (2015) · Nature Communications · doi:10.1038/ncomms7362 · Cited by 2,561 · see citing works
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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
“Cycled NVP/C demonstrated additional LiF (136.69 eV) and Li x PO y F z (135.35 eV) peaks, which also show the formation of the passivation layer 46 .”
Influential
- Authors
- Lee, H., Lim, H.-S., Ren, X., Yu, L., Engelhard, M. H., Han, K. S., Lee, J., Kim, H.-T., Xiao, J., Liu, J., Xu, W., & Zhang, J.-G.
- Affiliations
- Pacific Northwest National Laboratory (US)
- Energy & Environment Directorate, Pacific Northwest National Laboratory (PNNL), 902 Battelle Boulevard, Richland, Washington 99354, United States
- Department of Chemical & Biomolecular Engineering, Korea Advanced Institute of Science and Technology (KAIST), 291 Daehak-ro, Yuseong-gu, Daejeon 34141, Republic of Korea
- Korea Advanced Institute of Science and Technology (KR)
- Corresponding author
- Xu, Wu
- Zhang, Ji-Guang
- ORCID
- Venue
- ACS Energy Letters
- Publisher
- American Chemical Society (ACS)
- Published
- 2018-11-09
- Volume
- 3
- Issue
- 12
- Pages
- 2921-2930
- ISSN
- 2380-8195 (ISSN-L)
- OpenAlex
- W2900175974
- Cited by
- 150
- References
- 2
- Citations by year
- 2026: 21 · 2025: 19 · 2024: 24 · 2023: 31 · 2022: 14 · 2021: 21 · 2020: 9 · 2019: 11
- FWCI
- 3.92
- Type
- journal article
- Language
- en
- Open access
- closed
- Locations
- ACS Energy Letters (publishedVersion)
- Funders
- Vehicle Technologies Program (DE-AC02-05CH11231)
- Topics
- Physical Sciences › Engineering › Electrical and Electronic Engineering › Advanced Battery Materials and Technologies
- Physical Sciences › Engineering › Electrical and Electronic Engineering › Advancements in Battery Materials
- Physical Sciences › Engineering › Automotive Engineering › Advanced Battery Technologies Research
- Keywords
- lithium metal batteries, cathode degradation, capacity fade, cathode electrolyte interphase, polydopamine coating, interfacial stability, cycling stability
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