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oai:figshare.com:article/34037287 2026-10-01T00:07:58Z category_1 category_4 category_915 category_7 category_13 category_21 category_24 category_873 category_734 category_128 portal_63 item_type_6 month_year_10_2026

Molecular Tailoring of Succinonitrile Reshapes Na⁺ Solvation and Interfacial Chemistry in High-Voltage Solid-State Polymer Electrolytes for Sodium Metal Batteries Hu Fu (40740) Yuping Wu (200783) Wenyu Xu (2301838) Bolin Li (1559467) Zhirong Chen (4478053) Qinran Zhang (11828729) Haichen Li (1883455) Hongming Zhou (5100359) Biophysics Biochemistry Physical Sciences not elsewhere classified Medicine Genetics Biotechnology Evolutionary Biology Chemical Sciences not elsewhere classified Biological Sciences not elsewhere classified Hematology unstable electrode interfaces temperature ionic conductivity sup >–</ sup sup >+</ sup state polymer electrolytes stable gauche conformation sodium metal batteries resultant spe achieves performance polymer electrolytes modified spe induces 42 mah g 352 ms cm versus 485 cycles high ionic conductivity 3 </ sub succinonitrile reshapes na succinonitrile yields 1500 cycles yet suffer work demonstrates voltage tolerance voltage solid transference number significantly stabilizing pristine system plasticizer self novel plasticizer molecular tailoring molecular customization interfacial chemistry inadequate room ethylene oxide design suppresses capacity retention anchoring tfsi aggregation within 1 c Solid-state polymer electrolytes based on poly(ethylene oxide) are pivotal for high-safety, high-energy-density sodium metal batteries, yet suffer from inadequate room-temperature ionic conductivity and unstable electrode interfaces. Here, molecular tailoring of succinonitrile yields a novel plasticizer (SGa) featuring retained amide groups and a stable gauche conformation. This design suppresses the plasticizer self-aggregation within the poly(ethylene oxide) matrix, enhances polymer chain interactions, and optimizes Na⁺ solvation structures. Consequently, the resultant SPE achieves a high ionic conductivity of 0.352 mS cm^–1 and a Na⁺ transference number of 0.71. Molecular dynamics simulations reveal that SGa weakens strong Na⁺ coordination while anchoring TFSI^– anions, establishing a Na⁺-dominated fast conduction network. Crucially, the modified SPE induces a uniform, robust solid electrolyte interphase enriched in inorganic Na₃N, significantly stabilizing the Na anode. Na₃V₂(PO₄)₃|SPE|Na cell delivers 90.6% capacity retention after 1500 cycles at 1 C (versus 485 cycles for the pristine system) and exhibits superior rate capability (61.42 mAh g^–1 at 4 C) alongside high-voltage tolerance up to 4.5 V. Beyond addressing critical bottlenecks in sodium metal batteries, this work demonstrates the effectiveness of molecular customization in designing high-performance polymer electrolytes. 2026-09-30T00:00:00Z Text Journal contribution 10.1021/acsnano.6c11895.s001 https://figshare.com/articles/journal_contribution/Molecular_Tailoring_of_Succinonitrile_Reshapes_Na_sup_sup_Solvation_and_Interfacial_Chemistry_in_High-Voltage_Solid-State_Polymer_Electrolytes_for_Sodium_Metal_Batteries/34037287 CC BY-NC 4.0