期刊
CHEMISTRY OF MATERIALS
卷 31, 期 23, 页码 9699-9714出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.chemmater.9b03230
关键词
-
资金
- EPSRC [EP/N004884]
- Leverhulme Trust via the Leverhulme Research Centre for Functional Materials Design
- ISCF Faraday Challenge project: SOLBAT - The Solid-State (Li or Na) Metal-Anode Battery
- University of Liverpool
- EPSRC
- BBSRC
- University of Warwick through Birmingham Science City Advanced Materials Project 1 - Advantage West Midlands (AWM)
- European Regional Development Fund (ERDF)
- Royal Society
- University of Warwick through Birmingham Science City Advanced Materials Project 2 - Advantage West Midlands (AWM)
- EPSRC [EP/N004884/1, EP/S003053/1] Funding Source: UKRI
With the goal of finding new lithium solid electrolytes by a combined computational-experimental method, the exploration of the Li-Al-O-S phase field resulted in the discovery of a new sulfide Li3AlS3. The structure of the new phase was determined through an approach combining synchrotron X-ray and neutron diffraction with Li-6 and Al-27 magic-angle spinning nuclear magnetic resonance spectroscopy and revealed to be a highly ordered cationic polyhedral network within a sulfide anion hcp-type sublattice. The originality of the structure relies on the presence of Al2S6 repeating dimer units consisting of two edge-shared Al tetrahedra. We find that, in this structure type consisting of alternating tetrahedral layers with Li-only polyhedra layers, the formation of these dimers is constrained by the Al/S ratio of 1/3. Moreover, by comparing this structure to similar phases such as Li5AlS4 and Li4.4Al0.2Ge0.3S4 ((Al + Ge)/S = 1/4), we discovered that the AlS4 dimers not only influence atomic displacements and Li polyhedral distortions but also determine the overall Li polyhedral arrangement within the hcp lattice, leading to the presence of highly ordered vacancies in both the tetrahedral and Li-only layer. AC impedance measurements revealed a low lithium mobility, which is strongly impacted by the presence of ordered vacancies. Finally, a composition-structure property relationship understanding was developed to explain the extent of lithium mobility in this structure type.
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据