Institution: | 1. MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage, School of Chemistry and Chemical Engineering, Harbin Institute of Technology (HIT), Harbin, 150001 P. R. China;2. CAS Key Laboratory of Analytical Chemistry for Living Biosystems, Beijing National Laboratory for Molecular Sciences (BNLMS), Institute of Chemistry, Chinese Academy of Sciences (CAS), Beijing, 100190 P. R. China;3. CAS Key Laboratory of Molecular Nanostructure and Nanotechnology, CAS Research/Education Center for Excellence in Molecular Sciences, Beijing National Laboratory for Molecular Sciences (BNLMS), Institute of Chemistry, Chinese Academy of Sciences (CAS), Beijing, 100190 P. R. China;4. CAS Key Laboratory of Molecular Nanostructure and Nanotechnology, CAS Research/Education Center for Excellence in Molecular Sciences, Beijing National Laboratory for Molecular Sciences (BNLMS), Institute of Chemistry, Chinese Academy of Sciences (CAS), Beijing, 100190 P. R. China
School of Chemical Sciences, University of Chinese Academy of Sciences (UCAS), Beijing, 100049 P. R. China;5. CAS Key Laboratory of Analytical Chemistry for Living Biosystems, Beijing National Laboratory for Molecular Sciences (BNLMS), Institute of Chemistry, Chinese Academy of Sciences (CAS), Beijing, 100190 P. R. China
School of Chemical Sciences, University of Chinese Academy of Sciences (UCAS), Beijing, 100049 P. R. China |
Abstract: | In overcoming the Li+ desolvation barrier for low-temperature battery operation, a weakly-solvated electrolyte based on carboxylate solvent has shown promises. In case of an organic-anion-enriched primary solvation sheath (PSS), we found that the electrolyte tends to form a highly swollen, unstable solid electrolyte interphase (SEI) that shows a high permeability to the electrolyte components, accounting for quickly declined electrochemical performance of graphite-based anode. Here we proposed a facile strategy to tune the swelling property of SEI by introducing an inorganic anion switch into the PSS, via LiDFP co-solute method. By forming a low-swelling, Li3PO4-rich SEI, the electrolyte-consuming parasitic reactions and solvent co-intercalation at graphite-electrolyte interface are suppressed, which contributes to efficient Li+ transport, reversible Li+ (de)intercalation and stable structural evolution of graphite anode in high-energy Li-ion batteries at a low temperature of ?20 °C. |