Computational and Experimental Investigations of Na-Ion Conduction in Cubic Na3PSe4,Chemistry of Materials

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Computational and Experimental Investigations of Na-Ion Conduction in Cubic Na3PSe4
Chemistry of Materials ( IF 7.2 ) Pub Date : 2015-12-18 00:00:00 , DOI: 10.1021/acs.chemmater.5b04013
Shou-Hang Bo _{1,

2} , Yan Wang ₁ , Jae Chul Kim _{1,

2} , William Davidson Richards ₁ , Gerbrand Ceder _{1,

2,

3}

Affiliation

All-solid-state Na-ion batteries that operate at or close to room temperature are a promising next-generation battery technology with enhanced safety and reduced manufacturing cost. An indispensable component of this technology is the solid-state electrolyte that allows rapid shuttling of the mobile cation (i.e., Na⁺) between the cathode and anode. However, there are very few fast Na-ion conductors with ionic conductivity approaching that of the liquid counterparts (i.e., 1 mS cm^–1). In this work, we present the synthesis and characterization of a fast Na-ion conductor, cubic Na₃PSe₄. This material possesses a room-temperature ionic conductivity exceeding 0.1 mS cm^–1 and does not require high-temperature sintering to minimize grain boundary resistance, making it a promising solid-state electrolyte candidate for all-solid-state Na-ion battery applications. On the basis of density functional theory, nudged elastic band, and molecular dynamics investigations, we demonstrate that the framework of cubic Na₃PSe₄ only permits rapid Na⁺ diffusion with the presence of defects, and that the formation of the Na vacancy (charge-balanced by slight Se^2– oxidation) is more energetically favorable among the various defects considered. This finding provides important guidelines to further improve Na-ion conductivity in this class of materials.

中文翻译：

立方Na ₃ PSe ₄中钠离子传导的计算和实验研究

在室温或接近室温下运行的全固态Na离子电池是一种有前途的下一代电池技术，具有增强的安全性和降低的制造成本。该技术必不可少的组成部分是固态电解质，它可使阴极和阳极之间的移动阳离子（即Na ⁺）快速穿梭。但是，几乎没有离子电导率接近液体对应电导率（即1 mS cm ^–1）的快速Na离子导体。在这项工作中，我们介绍了快速的Na离子导体立方Na ₃ PSe ₄的合成和表征。该材料的室温离子电导率超过0.1 mS cm ^–1而且不需要高温烧结就可以使晶界电阻最小化，这使其成为用于全固态Na离子电池应用的有前途的固态电解质候选材料。根据密度泛函理论，微动的弹性带和分子动力学研究，我们证明了立方Na ₃ PSe ₄的框架仅允许Na ⁺快速扩散且存在缺陷，并且形成了Na空位（电荷在所考虑的各种缺陷中，通过少量的Se ^2–氧化而平衡）在能量上更有利。该发现提供了重要的指导方针，以进一步提高此类材料中的钠离子电导率。

更新日期：2015-12-18

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