Issue 14, 2019

Ab initio investigation of the stability of electrolyte/electrode interfaces in all-solid-state Na batteries

Abstract

All-solid-state batteries show great potential for achieving high energy density with less safety problems; however, (electro)chemical issues at the solid electrolyte/electrode interface may severely limit their performance. In this work, the electrochemical stability and chemical reactivity of a wide range of potential Na solid-state electrolyte chemistries were investigated using density functional theory calculations. In general, lower voltage limits are predicted for both the reduction and oxidation of Na compounds compared with those of their Li counterparts. The lower reduction limits for the Na compounds indicate their enhanced cathodic stability as well as the possibility of stable sodium metal cycling against a number of oxides and borohydrides. With increasing Na content (or chemical potential), improved cathodic stability but also reduced anodic stability are observed. An increase in the oxidation voltage is shown for Na polyanion systems, including borohydrides, NaSICON-type oxides, and aluminates, due to the covalent stabilization of the anions. In addition, the oxides exhibit remarkable chemical stability when in contact with various cathode materials (layered transition metal oxides and fluorophosphates), whereas the chalcogenides predictably display narrow electrochemical windows and high chemical reactivity. Our findings indicate some promising candidates for solid-state conductors and/or protective coating materials to enable the operation of high-energy-density all-solid-state Na batteries.

Graphical abstract: Ab initio investigation of the stability of electrolyte/electrode interfaces in all-solid-state Na batteries

Supplementary files

Article information

Article type
Paper
Submitted
01 nov 2018
Accepted
04 jan 2019
First published
11 feb 2019
This article is Open Access
Creative Commons BY license

J. Mater. Chem. A, 2019,7, 8144-8155

Ab initio investigation of the stability of electrolyte/electrode interfaces in all-solid-state Na batteries

V. Lacivita, Y. Wang, S. Bo and G. Ceder, J. Mater. Chem. A, 2019, 7, 8144 DOI: 10.1039/C8TA10498K

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