用分层协同深度学习,高效发现高性能固态电解质。
A Hierarchical Synergistic Deep Learning Framework Integrating Composition, Structure, and Ionic Transport for Solid-State Electrolyte Discovery

- 四模块分步筛选:成分、结构、输运预估与动力学验证
- 从三千万候选中找出97个高导电材料,最高导电率达59.0 mS/cm
- 揭示锂离子跳跃网络是导电关键,为材料设计提供新方向
无机固态电解质需兼具高室温离子电导率、宽电化学窗口、优异电子绝缘性及良好机械柔韧性。单一模型因训练数据分布偏差、跨属性数据异构及稀缺动力学数据,在大规模化学空间中难以实现可靠的多目标筛选。为此,我们构建了分层协同的深度学习框架,通过四个互补模块依次提升效率、精度与可靠性。自研L-G-DCNN和基于DenseGNN的多保真模型分别作为成分与结构专家,用于热力学粗筛与多属性评估;MatterSim与系统特异性DeePMD模型提供输运预估与动力学验证。系统性基准测试显示各模块均优于主流方法,回溯验证确立模块级精度与端到端流程可靠性的双重闭环。应用于30,364,908个来自Alex/ICSD的候选物,框架识别出97个高性能候选,室温电导率在0.109–59.0 mS/cm之间,含94种卤化物、1种硼氢化物和2种氧化物。与独立实验数据一致表明,94种卤化物中有76种位于已知高导电结构区域。分析揭示,锂离子跳跃网络连通性而非几何锂位点数量,是决定室温离子电导率的核心因素。锂空位工程可有效提升氧化物输运性能,而O²⁻骨架的内在刚性暗示氧化物电解质存在性能上限。
原文摘要 · Abstract (English)
Inorganic solid-state electrolytes must combine high room-temperature ionic conductivity, a wide electrochemical window, excellent electronic insulation, and favorable mechanical compliance. Single models struggle to support reliable multi-objective screening across vast chemical spaces because of training-data distribution mismatch, cross-property dataset heterogeneity, and scarce kinetic transport data. To overcome these limitations, we develop a hierarchical synergistic deep-learning framework that sequentially coordinates efficiency, accuracy, and reliability through four complementary modules. The in-house-developed L-G-DCNN and a multi-fidelity implementation built on DenseGNN serve as compositional and structural experts for thermodynamic coarse screening and multi-property evaluation, respectively; MatterSim and system-specific DeePMD models provide transport pre-assessment and kinetic validation. Systematic benchmarks show that each module outperforms mainstream counterparts in its task, while retrospective validation establishes dual closed-loop verification of module-level accuracy and end-to-end workflow reliability. Applied to 30,364,908 Alex/ICSD-derived candidates, the framework identifies 97 high-performance candidates with room-temperature ionic conductivities of 0.109--59.0 mS/cm, including 94 halides, one borohydride, and two oxides. Consistency with independent experimental data confirms that 76 of the 94 halides fall within reported high-conductivity structural regions. Analysis reveals that Li$^{+}$ jump-network connectivity, rather than the number of geometric Li sites, is the core determinant of room-temperature ionic conductivity. Li-defect engineering effectively enhances oxide transport, whereas the inherent rigidity of the O$^{2-}$ framework suggests a potential upper limit on oxide electrolyte performance.
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