High-throughput discovery of fluoride-ion conductors via a decoupled, dynamic, and iterative (DDI) framework
High-throughput discovery of fluoride-ion conductors via a decoupled, dynamic, and iterative (DDI) framework
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通过解耦动态迭代（DDI）框架高通量发现氟离子导体
DOI：
10.1038/s41524-022-00786-8
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发表时间：
2022-05-06
影响因子：
9.7
通讯作者：
Warren, Scott C.
中科院分区：
文献类型：
--
作者：
Sundberg, Jack D.;Druffel, Daniel L.;Warren, Scott C.
氟离子电池是锂离子电池的有前途的替代品，具有更高的理论容量和工作电压，但由于已知电解质和电极的离子电导率差，它们的成功有限。在这里，我们报告了一个高通量的计算筛选9747含氟材料的氟离子导体的搜索。通过结合经验、轻量级DFT和轻推弹性带（NEB）计算，我们确定了>10个具有高氟化物迁移率的晶体系统。我们应用了一种搜索策略，其中计算以任何顺序执行（解耦），计算资源根据需要重新分配（动态），预测模型重复更新（迭代）。与分层搜索不同，我们的解耦，动态和迭代框架（DDI）首先计算大量不同材料中氟化物离子迁移率的高质量势垒高度。这一高质量的数据集提供了一个基准，可以据此改进快速计算方法。这种精确的方法被用来测量6797个氟离子通道的势垒高度。最终的数据集使我们能够发现许多迷人的高性能导体，并推导出控制其性能的设计规则。这些材料将加速氟离子电池的实验研究，而设计规则将为理解离子传导提供更好的基础。
Fluoride-ion batteries are a promising alternative to lithium-ion batteries with higher theoretical capacities and working voltages, but they have experienced limited success due to the poor ionic conductivities of known electrolytes and electrodes. Here, we report a high-throughput computational screening of 9747 fluoride-containing materials in search of fluoride-ion conductors. Via a combination of empirical, lightweight DFT, and nudged elastic band (NEB) calculations, we identified >10 crystal systems with high fluoride mobility. We applied a search strategy where calculations are performed in any order (decoupled), computational resources are reassigned based on need (dynamic), and predictive models are repeatedly updated (iterative). Unlike hierarchical searches, our decoupled, dynamic, and iterative framework (DDI) began by calculating high-quality barrier heights for fluoride-ion mobility in a large and diverse group of materials. This high-quality dataset provided a benchmark against which a rapid calculation method could be refined. This accurate method was then used to measure the barrier heights for 6797 fluoride-ion pathways. The final dataset has allowed us to discover many fascinating, high-performance conductors and to derive the design rules that govern their performance. These materials will accelerate experimental research into fluoride-ion batteries, while the design rules will provide an improved foundation for understanding ionic conduction.