Chemical design and data-driven innovation: a cross-scale review of flame-retardant electrolytes for safe high-energy-density batteries

TY - JOUR

T1 - Chemical design and data-driven innovation

T2 - a cross-scale review of flame-retardant electrolytes for safe high-energy-density batteries

AU - Wu, Yongchun

AU - Zhang, Yuanxing

AU - Liu, Yunjiang

AU - Hao, Yunbo

AU - Lu, Xiaojin

AU - Li, Haocheng

AU - Zhang, Yuxiang

AU - Li, Zihan

AU - Wu, Hanfeng

AU - Zhang, Xinyu

AU - Ma, Ming

AU - Wu, Borong

AU - Wu, Feng

AU - Mu, Daobin

N1 - Publisher Copyright: © 2026 Elsevier B.V.

PY - 2026/7/15

Y1 - 2026/7/15

N2 - High-energy-density lithium batteries, essential for electric vehicles and large-scale energy storage, face intensified safety risks, with thermal runaway remaining a critical barrier to deployment. Flame-retardant electrolytes offer a direct materials-level route to mitigate fire hazards, yet practical implementation requires concurrently meeting stringent demands on ionic transport, interfacial compatibility, and mechanical/thermal robustness. In this cross-scale review, we integrate “mechanism–assessment–design–computation” to guide the development of high-safety flame-retardant electrolytes for solid-state batteries. We first compare thermal runaway pathways in polymer- and inorganic-electrolyte cells from both abuse-triggered initiation and internally driven propagation, and establish a multidimensional safety assessment framework encompassing flame retardancy, thermal stability, mechanical integrity, and chemical/electrochemical stability. We then summarize chemical design strategies for two major classes of solid flame-retardant electrolytes: (i) polymer-based composite electrolytes enabled by flame-retardant additives—including inorganic fillers, halogen/phosphorus/nitrogen/silicon chemistries, and MOFs/derivatives—and (ii) intrinsically flame-retardant polymer electrolytes (in situ copolymerized and gel-like systems) together with inorganic solid electrolytes (oxides, sulfides, and halides). For each class, we elucidate composition–structure–property relationships, gas- and condensed-phase flame-inhibition mechanisms, and performance regulation strategies, with emphasis on interface engineering and thermodynamics–kinetics coupling to reconcile stability with fast ion transport. Finally, we highlight how quantum chemical calculations and (ab initio/classical) molecular dynamics reveal atomistic decomposition and transport, how finite-element and fluid-dynamics simulations enable cell-level safety evaluation, and how materials genomics and AI accelerate multi-objective screening, reverse design, and optimization. We also distill remaining bottlenecks—conductivity–flammability trade-offs in polymers, interfacial impedance and air/moisture sensitivity in inorganic solids—and outline scalable, cost-effective pathways toward practical implementation. This review consolidates current knowledge and provides actionable principles for translating safer electrolytes toward practical high-energy batteries.

AB - High-energy-density lithium batteries, essential for electric vehicles and large-scale energy storage, face intensified safety risks, with thermal runaway remaining a critical barrier to deployment. Flame-retardant electrolytes offer a direct materials-level route to mitigate fire hazards, yet practical implementation requires concurrently meeting stringent demands on ionic transport, interfacial compatibility, and mechanical/thermal robustness. In this cross-scale review, we integrate “mechanism–assessment–design–computation” to guide the development of high-safety flame-retardant electrolytes for solid-state batteries. We first compare thermal runaway pathways in polymer- and inorganic-electrolyte cells from both abuse-triggered initiation and internally driven propagation, and establish a multidimensional safety assessment framework encompassing flame retardancy, thermal stability, mechanical integrity, and chemical/electrochemical stability. We then summarize chemical design strategies for two major classes of solid flame-retardant electrolytes: (i) polymer-based composite electrolytes enabled by flame-retardant additives—including inorganic fillers, halogen/phosphorus/nitrogen/silicon chemistries, and MOFs/derivatives—and (ii) intrinsically flame-retardant polymer electrolytes (in situ copolymerized and gel-like systems) together with inorganic solid electrolytes (oxides, sulfides, and halides). For each class, we elucidate composition–structure–property relationships, gas- and condensed-phase flame-inhibition mechanisms, and performance regulation strategies, with emphasis on interface engineering and thermodynamics–kinetics coupling to reconcile stability with fast ion transport. Finally, we highlight how quantum chemical calculations and (ab initio/classical) molecular dynamics reveal atomistic decomposition and transport, how finite-element and fluid-dynamics simulations enable cell-level safety evaluation, and how materials genomics and AI accelerate multi-objective screening, reverse design, and optimization. We also distill remaining bottlenecks—conductivity–flammability trade-offs in polymers, interfacial impedance and air/moisture sensitivity in inorganic solids—and outline scalable, cost-effective pathways toward practical implementation. This review consolidates current knowledge and provides actionable principles for translating safer electrolytes toward practical high-energy batteries.

KW - AI-driven design

KW - Flame-retardant electrolytes

KW - Multiscale simulation

KW - Safety assessment

KW - Solid-state batteries

KW - Thermal runaway

UR - https://www.scopus.com/pages/publications/105033094863

U2 - 10.1016/j.ccr.2026.217801

DO - 10.1016/j.ccr.2026.217801

M3 - Review article

AN - SCOPUS:105033094863

SN - 0010-8545

VL - 559

JO - Coordination Chemistry Reviews

JF - Coordination Chemistry Reviews

M1 - 217801

ER -