锂离子导电固态电解质(SSE)的发展对于提高能量密度至关重要。操作可靠性,和前所未有的安全性,以取代最先进的锂离子电池(LIB)。在这方面,我们在这里介绍了添加MgO的NASICON型LAGP玻璃陶瓷电解质的成功熔铸合成,其组成为Li1.5Al0.3Mg0.1Ge1.6(PO4)3,即LAMGP。研究了三种不同的附加氧化物的影响,目的是提高晶粒内聚力,从而提高锂离子电导率。具体来说,氧化钇(Y2O3,5mol%),加入氧化硼(B2O3,0.7摩尔%)和氧化硅(SiO2,2.4摩尔%),产生LAMGP-Y,LAMGP-B和LAMGP-Si,分别。它们的影响在热方面进行了详尽的比较,结晶,结构/形态和离子传导特征。在三种氧化物中,B2O3能够积极作用于晶界,而不会导致晶粒变形和绝缘二次相形成,与经过相同热处理的商业LAGP的0.08mScm-1相比,在20°C下实现了0.21mScm-1的增强的离子电导率。通过LAMGP-B系统评估了高达4.8V与Li/Li的显着阳极氧化稳定性,这说明了其与高能(高V)阴极结合使用的前景广阔。
The development of Li-ion conducting solid-state electrolytes (SSEs) is crucial to achieve increased energy density, operative reliability, and unprecedented safety to replace the state-of-the-art Li-ion battery (LIB). In this regard, we here present the successful melt-casting synthesis of a MgO-added NASICON-type LAGP glass-ceramic electrolyte with composition Li1.5Al0.3Mg0.1Ge1.6(PO4)3, namely LAMGP. The effects of three different additional oxides are investigated, with the aim to improve grain cohesion and consequently enhance Li-ion conductivity. Specifically, yttrium oxide (Y2O3, 5 mol%), boron oxide (B2O3, 0.7 mol%) and silicon oxide (SiO2, 2.4 %mol) are added, yielding LAMGP-Y, LAMGP-B and LAMGP-Si, respectively. Their effects are exhaustively compared in terms of thermal, crystalline, structural/morphological and ion conducting features. Among the three oxides, B2O3 is able to positively act on grain boundaries without bringing along grains deformation and insulating secondary phases formation, achieving enhanced ionic conductivity of 0.21 mS cm-1 at 20 °C as compared to 0.08 mS cm-1 for a commercial LAGP subjected to the same thermal treatment. A remarkable anodic oxidation stability up to 4.8 V vs Li+/Li is assessed by LAMGP-B system, which accounts for promising prospects for its use in combination with high-energy (high-V) cathodes.