A unified predictive and generative solution for liquid electrolyte formulation

Liquid electrolytes are critical components of next-generation energy storage systems, enabling fast ion transport, minimizing interfacial resistance and ensuring electrochemical stability for long-term battery performance. However, measuring electrolyte properties and designing formulations remain experimentally and computationally expensive. Here we present a unified framework for designing liquid electrolyte formulation, integrating a forward predictive model with an inverse generative approach. Leveraging both computational and experimental data collected from the literature and extensive molecular simulations, we train a predictive model capable of accurately estimating electrolyte properties from ionic conductivity to solvation structure. Our physics-informed architecture preserves permutation invariance and incorporates empirical dependencies on temperature and salt concentration, making it broadly applicable to property prediction tasks across molecular mixtures. Furthermore, we introduce a generative machine learning framework for molecular mixture design with permutation invariance, demonstrated on electrolyte systems. This framework supports multi-condition-constrained generation, addressing the inherently multi-objective nature of materials design. As a proof of concept, we experimentally identified three liquid electrolytes exhibiting both high ionic conductivity and anion-rich solvation structures, one of which shows promising cycling stability. This unified framework advances data-driven electrolyte design and can be readily extended to other complex chemical systems beyond electrolytes. Yang et al. introduce a unified framework for liquid electrolyte design, integrating a forward predictive model with an inverse generative approach, where three generated high-conductivity candidates were identified and experimentally validated.