El-Shinawi Hany, El-Dafrawy Shady M, Tarek Mahmoud, Molouk Ahmed F S, Cussen Edmund J, Cussen Serena A
Department of Chemistry, Faculty of Science, Mansoura University Mansoura 35516 Egypt
Department of Materials Science and Engineering, University of Sheffield Sir Robert Hadfield Building Sheffield S1 3JD UK.
RSC Adv. 2024 Mar 4;14(11):7557-7563. doi: 10.1039/d3ra08968a. eCollection 2024 Feb 29.
All-solid-state batteries present promising high-energy-density alternatives to conventional Li-ion chemistries, and Li-stuffed garnets based on LiLaZrO (LLZO) remain a forerunner for candidate solid-electrolytes. One route to access fast-ion conduction in LLZO phases is to stabilize the cubic LLZO phase by doping on the Li sites with aliovalent ions such as Al or Ga. Despite prior attempts, the stabilization of the cubic phase of isostructural LiLaSnO (LLSO) by doping on the Li sites has up to now not been realised. Here, we report a novel cubic fast-ion conducting LiLaSnO-type phase stabilized by doping Ga in place of Li. 0.3 mole of gallium per formula unit of LLSO were needed to fully stabilize the cubic garnet, allowing structural and electrochemical characterizations of the new material. A modified sol-gel synthesis approach is introduced in this study to realise Ga-doping in LLSO, which offers a viable route to preparing new Sn-based candidate solid-electrolytes for all-solid-state battery applications.
全固态电池为传统锂离子化学体系提供了具有高能量密度潜力的替代方案，基于LiLaZrO（LLZO）的锂填充石榴石仍然是候选固体电解质的领跑者。在LLZO相中实现快速离子传导的一种途径是通过用诸如Al或Ga等异价离子掺杂锂位点来稳定立方LLZO相。尽管此前进行了尝试，但迄今为止，通过在锂位点上掺杂来稳定同结构LiLaSnO（LLSO）的立方相尚未实现。在此，我们报告了一种通过掺杂Ga替代Li来稳定的新型立方快速离子传导LiLaSnO型相。每公式单位的LLSO需要0.3摩尔的镓才能完全稳定立方石榴石，从而能够对新材料进行结构和电化学表征。本研究引入了一种改进的溶胶 - 凝胶合成方法来实现LLSO中的Ga掺杂，这为制备用于全固态电池应用的新型Sn基候选固体电解质提供了一条可行的途径。
