Issue 4, 2022

Multi-variable Bayesian optimization for a new composition with high Na+ conductivity in the Na3PS4 family

Abstract

Na3PS4 is an archetypal room-temperature (RT), Na+-conducting, solid-state electrolyte. Various compositional modifications of this compound via iso/aliovalent substitution are known to provide a high ionic conductivity (σion) that is comparable to that of liquid electrolytes. In this work, we implemented a Bayesian optimization (BO) algorithm to discover new compositions with a high σion in a multi-dimensional search space. BO has attracted a great deal of attention in materials research since it is successfully used as a closed-loop optimization strategy for materials discovery. The systematically designed search space used for our BO implementation consisted of compositional variables (A = Ca2+, Y3+, La3+; M1 = P5+, Sb5+; M2 = Si4+, Ge4+, Sn4+; Q = S2−, Se2−, Te2−; X = Cl, Br, I in (Na, A)(M1, M2, W)(Q, X)4) and processing variables (synthetic temperature and time). Na2.81(W0.22Si0.10Sb0.68)S3.93Br0.07 selected through BO was further refined via logical reasoning. Subsequently, Br-free Na2.88(W0.22Si0.10Sb0.68)S4 was discovered. Heavily co-doped Na3SbS4 by Si4+ and W6+ show high σion (20.2 and 7.4 mS cm−1) at RT and −20 °C, respectively, which can be ascribed to the notably low activation barrier (0.14 eV) in the Na3PS4 family. Herein, a low electronic conductivity (2 × 10−7 S cm−1) and stable Na plating/stripping is also discussed. These types of behavior suggest that Na2.88(W0.22Si0.10Sb0.68)S4 could be a promising solid-state electrolyte (SSE) of the Na3PS4 family.

Graphical abstract: Multi-variable Bayesian optimization for a new composition with high Na+ conductivity in the Na3PS4 family

Supplementary files

Article information

Article type
Paper
Submitted
18 Nov 2021
Accepted
25 Dec 2021
First published
28 Dec 2021

J. Mater. Chem. A, 2022,10, 1831-1839

Multi-variable Bayesian optimization for a new composition with high Na+ conductivity in the Na3PS4 family

J. Y. Seo, S. Shim, J. Lee, B. D. Lee, S. Park, W. B. Park, S. Han, M. Pyo and K. Sohn, J. Mater. Chem. A, 2022, 10, 1831 DOI: 10.1039/D1TA09886A

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