Zhang, Bin, Yin, Qing, Peng, Shouxun, Zhao, Zeyu, Shi, Meiyu, Li, Xiwen, Li, Zheng, Xiao, Bin, Gu, Xiuquan, Zhi, Mingjia, Chubenko, Eugene, Bondarenko, Vitaly, Bandarenka, Hanna  ORCID: https://orcid.org/0000-0003-4254-8261 and Sui, Yanwei
2026.
Anion-participating solvation in multi-salt cooperative electrolytes for enhanced low-temperature Li-storage capability.
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10.1007/s11581-026-07336-y
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Abstract
Low-temperature operation remains a major challenge because sluggish Li+ transport and aggravated polarization severely compromise energy delivery and cyclability. Here we develop a wide-temperature tri-salt electrolyte comprising LiBF4, LiFSI and LiDFOB in a PC/DME/iBA solvent matrix. With an optimized formulation (0.75 M LiBF4, 0.2 M LiFSI, 0.05 M LiDFOB, PC : DME : iBA = 25:65:10, v/v/v, T-electrolyte), Li||LiCoO2 batteries deliver high reversibility, strong rate capability and durable cycling from − 20 to 40 °C. Remarkably, at −20 °C, the optimized electrolyte sustains 143.5 mAh g− 1 at 0.2 C and preserves 129.7 mAh g− 1 after 500 cycles, corresponding to ~ 85.5% of the room-temperature capacity, whereas a conventional low-temperature electrolyte rapidly decays to 47.2 mAh g− 1 over the same cycles. Raman spectroscopy and molecular dynamics (MD) simulations reveal that anions and iBA participation reconstruct the Li+ solvation sheath by suppressing PC over-coordination and lowering representative cluster binding energies, thereby reducing the desolvation penalty and promoting anion-derived inorganic-enriched interphases. XPS reveals that the T-electrolyte stabilizes both Solid Electrolyte Interphase (SEI) and Cathode Electrolyte Interphase (CEI) by promoting LiF/LiSOxF/borate-rich inorganic passivation while suppressing uncontrolled carbonate/ether decomposition, and by forming a self-limited cathode CEI in which ROCO2Li semicarbonates act as a compliant scaffold to preserve interfacial integrity under cycling at − 20 °C. This work establishes a practical solvation-interphase design strategy for enhanced Li-storage at low temperature.
| Item Type: | Article |
|---|---|
| Date Type: | Published Online |
| Status: | In Press |
| Schools: | Schools > Physics and Astronomy |
| Additional Information: | RRS policy applied |
| Publisher: | Springer |
| ISSN: | 0947-7047 |
| Date of First Compliant Deposit: | 26 August 2026 |
| Date of Acceptance: | 26 June 2026 |
| Last Modified: | 07 Sep 2026 22:00 |
| URI: | https://orca.cardiff.ac.uk/id/eprint/188409 |
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