锂-硼-硫结晶体系中结合超离子传导和有利的分解产物：稳定固体锂离子电解质的新机制。,ACS Applied Materials & Interfaces

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锂-硼-硫结晶体系中结合超离子传导和有利的分解产物：稳定固体锂离子电解质的新机制。
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2020-07-23 , DOI: 10.1021/acsami.9b19091
Austin D Sendek _{1,

2,

3} , Evan R Antoniuk ₄ , Ekin D Cubuk ₅ , Brandi Ransom ₂ , Brian E Francisco ₆ , Josh Buettner-Garrett ₆ , Yi Cui ₂ , Evan J Reed ₂

Affiliation

我们报告了一种固态锂离子电解质，该电解质有望同时展现出快速的离子电导率，宽的电化学稳定性，低成本和低质量密度。我们报告了基于出色的密度泛函理论（DFT）的室温单晶锂-硼-硫（Li-BS）体系中两相的室温离子电导率值：62（+9，-2）mS cm ^-1在李₅乙₇小号₁₃和80（-56，-41）。MS厘米^-1的Li ₉乙₁₉ š ₃₃。我们报告了两个附加相的重要离子电导率值：在Li ₂ B ₂ S中为0.0056至0.16 mS / cm ^–1之间Li ₃ BS _3中为₅和0.0031至9.7 mS cm ^–1之间，具体取决于所使用的室温外推方案。据我们所知，我们的预测使Li ₉ B ₁₉ S ₃₃和Li ₅ B ₇ S ₁₃成为任何晶体材料的DFT计算的单晶离子电导率的第二和第三高。我们计算出这些材料的热力学电化学稳定性窗口宽度对于Li ₅ B ₇ S ₁₃为0.50 V，对于Li ₂ B ₂ S ₅为0.16 V，对于Li为0.45 V₃ BS ₃和0.60 V的Li ₉ B ₁₉ S ₃₃。与包括Li ₁₀ GeP ₂ S ₁₂（LGPS）在内的最著名的基于硫化物的固态锂离子电解质材料相比，这些材料分别具有相似或更好的离子电导率和电化学稳定性。但是，我们预测，由Li–B–S系统中的各种成分合成的电解质材料可能会显示出更宽的0.63 V的热力学电化学稳定性窗口，并可能高达3 V或更高。Li–B–S系统的基本成本也很低，约为0.05 USD / m ²每10μm厚度，明显低于含锗LGPS的厚度，并且质量密度低于2 g / cm ³。这些快速传导阶段最初是通过基于机器学习的方法来筛选12,000多种固体电解质候选物而引起我们注意的，此处提供的证据表明该模型取得了令人鼓舞的成功。

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Combining Superionic Conduction and Favorable Decomposition Products in the Crystalline Lithium-Boron-Sulfur System: A New Mechanism for Stabilizing Solid Li-Ion Electrolytes.

We report a solid-state Li-ion electrolyte predicted to exhibit simultaneously fast ionic conductivity, wide electrochemical stability, low cost, and low mass density. We report exceptional density functional theory (DFT)-based room-temperature single-crystal ionic conductivity values for two phases within the crystalline lithium–boron–sulfur (Li–B–S) system: 62 (+9, −2) mS cm^–1 in Li₅B₇S₁₃ and 80 (−56, −41) mS cm^–1 in Li₉B₁₉S₃₃. We report significant ionic conductivity values for two additional phases: between 0.0056 and 0.16 mS/cm ^–1 in Li₂B₂S₅ and between 0.0031 and 9.7 mS cm^–1 in Li₃BS₃ depending on the room-temperature extrapolation scheme used. To our knowledge, our prediction gives Li₉B₁₉S₃₃ and Li₅B₇S₁₃ the second and third highest reported DFT-computed single-crystal ionic conductivities of any crystalline material. We compute the thermodynamic electrochemical stability window widths of these materials to be 0.50 V for Li₅B₇S₁₃, 0.16 V for Li₂B₂S₅, 0.45 V for Li₃BS₃, and 0.60 V for Li₉B₁₉S₃₃. Individually, these materials exhibit similar or better ionic conductivity and electrochemical stability than the best-known sulfide-based solid-state Li-ion electrolyte materials, including Li₁₀GeP₂S₁₂ (LGPS). However, we predict that electrolyte materials synthesized from a range of compositions in the Li–B–S system may exhibit even wider thermodynamic electrochemical stability windows of 0.63 V and possibly as high as 3 V or greater. The Li–B–S system also has a low elemental cost of approximately 0.05 USD/m² per 10 μm thickness, which is significantly lower than that of germanium-containing LGPS, and a comparable mass density below 2 g/cm³. These fast-conducting phases were initially brought to our attention by a machine learning-based approach to screen over 12,000 solid electrolyte candidates, and the evidence provided here represents an inspiring success for this model.

更新日期：2020-08-26

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