从十亿级分子空间中提取用于锂电池电解质设计的以腈为核心、醚辅助的基序层级
Extracting a nitrile-centered, ether-assisted motif hierarchy for lithium-battery electrolyte design from billion-scale molecular space
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中文总结 AI 辅助
该研究从十亿级GDB13分子空间中提取出以腈为核心、醚辅助的基序层级，结合生成模型与分子动力学模拟，为锂电池电解质设计提供了系统化的定量可解释方案。
中文摘要 AI 辅助
为锂电池设计电解质分子需要平衡电子稳定性与合适的Li+溶剂化能力，但在化学结构多样的分子中，其结构基础仍不明确。高通量筛选扩大了可搜索空间，但仅靠排名靠前的候选分子无法揭示重复出现的基序及其适用范围。我们使用电子-溶剂化描述符搜索了近十亿个GDB13结构，未明确指定官能团偏好或骨架约束。在不同的描述符权重下，高排名分子群体分为腈主导区域和同时包含大量腈与醚类分子的共存区域。这些区域共同定义了以腈为核心、醚辅助的基序层级：腈在广泛的权重范围内仍受青睐，而醚在更强的静电和极性约束下变得突出。将该层级编码到生成模型中，可将候选空间扩展至GDB13之外，无需明确的氟化奖励即可得到高分含氟结构。 explicit-solvent分子动力学模拟显示，代表性候选分子的配位作用弱且可交换，不会将碳酸乙烯酯从Li+周围的主要第一溶剂化壳层中置换出来；其对离子缔合和传输的影响取决于分子结构和浓度。这些结果确立了一个定量、可解释且受物理约束的基序层级，将已有的腈和醚化学系统化，用于锂电池电解质设计。
英文摘要
Designing electrolyte molecules for lithium batteries requires balancing electronic stability with appropriate Li+ solvation, yet the structural basis remains unclear across chemically diverse molecules. High-throughput screening expands the searchable space, but ranked candidates alone do not reveal recurring motifs or their applicability limits. We searched nearly one billion GDB13 structures using electronic--solvation descriptors without explicit functional-group preferences or scaffold constraints. Across descriptor weights, high-ranking populations separated into a nitrile-dominant regime and a coexistence regime containing substantial fractions of both nitrile- and ether-containing molecules. These regimes together define a nitrile-centered, ether-assisted motif hierarchy: nitrile remains favored across broad weight ranges, whereas ether becomes prominent under stronger electrostatic and polarity constraints. Encoding this hierarchy in a generative model expands the candidate space beyond GDB13 and yields high-scoring fluorinated structures without an explicit fluorination reward. Explicit-solvent molecular dynamics simulations show weak, exchangeable coordination of representative candidates without displacing ethylene carbonate from the dominant first solvation shell around Li+; effects on ion association and transport depend on molecular structure and concentration. These results establish a quantitative, interpretable and physically bounded motif hierarchy that systematizes established nitrile and ether chemistry for lithium-battery electrolyte design.
