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oai:figshare.com:article/34024646 2026-09-29T14:44:40Z category_1 category_4 category_13 category_873 category_45 category_61 category_69 category_133 category_135 portal_63 item_type_6 month_year_09_2026

Weak-Solvation Molecular Ion Gates Enabling Multipath Li⁺ Hopping and Air Stability in Garnet/Poly(ethylene oxide) Electrolytes Jiuzhi Cui (20728806) Zhen Fang (591405) Qiang Hu (122686) Yangyang Chen (1721638) Hong Yang (37298) Xingquan Liu (1510831) Xue-Jiao Nie (23631550) Jin-Zhi Guo (2566390) Jingxin Zhao (763933) Xing-Long Wu (1401565) Biophysics Biochemistry Genetics Chemical Sciences not elsewhere classified Sociology Developmental Biology Inorganic Chemistry Plant Biology Computational Biology sup >–</ sup sup >+</ sup restricting practical applications composite electrolyte delivers chemically anchoring 4 carboxyl group eliminates blocks ion migration accelerate coordination exchange 2 -( trifluoromethyl electrochemical stability window transport via coordination 4 </ sub 3 </ sub 12 </ sub weak coordination limits 2 mah cm 2 </ sub wsmi strategy proposed 6 </ sub air stability transport sites transport regions − cf transference number surface layer state batteries peo interface initial capacity ethylene oxide carrier density atmospheric moisture activating polymer 38 v 2000 h 1100 cycles Poly(ethylene oxide) (PEO)-based composite polymer electrolytes facilitate Li⁺ transport via coordination and decoordination. However, strong coordination impedes ion transport, while weak coordination limits the carrier density. This dilemma is further aggravated by the Li₂CO₃-passivated garnet surface that blocks ion migration, restricting practical applications. Here, we develop a weak-solvation molecular ion gate (WSMI) strategy by chemically anchoring 4-methoxy-2-(trifluoromethyl)benzoic acid onto Li_6.4La₃Zr_1.4Ta_0.6O₁₂ (LLZTO). The carboxyl group eliminates the alkaline Li₂CO₃ surface layer and forms a robust, chemically anchored WSMI interphase that shields LLZTO from atmospheric moisture, thus significantly enhancing air stability. Additionally, the −CF₃ groups enhance LiTFSI dissociation, weaken Li⁺-EO and Li⁺-TFSI^– interactions, and accelerate coordination exchange and interfacial hopping. Simultaneously, the ether-oxygen moieties provide Li⁺ -transport sites at the LLZTO/PEO interface, activating polymer, interfacial, and garnet-associated Li⁺ transport regions. As a result, the composite electrolyte delivers a Li⁺ transference number of 0.622 and an electrochemical stability window of 5.38 V (vs Li⁺/Li). Li||Li symmetric cells cycle stably for over 2000 h at 0.2 mA cm^–2 and 0.2 mAh cm^–2, and LiFePO₄||Li full cells retain 87.8% of their initial capacity after 1100 cycles at 1 C. The WSMI strategy proposed in this work provides valuable insights into tailoring interfacial chemical environments for all-solid-state batteries. 2026-09-29T00:00:00Z Text Journal contribution 10.1021/jacs.6c15811.s001 https://figshare.com/articles/journal_contribution/Weak-Solvation_Molecular_Ion_Gates_Enabling_Multipath_Li_sup_sup_Hopping_and_Air_Stability_in_Garnet_Poly_ethylene_oxide_Electrolytes/34024646 CC BY-NC 4.0