Synthetic accessibility and stability rules of NASICONs

Bin Ouyang; Jingyang Wang; Tanjin He; Christopher J Bartel; Haoyan Huo; Yan Wang; Valentina Lacivita; Haegyeom Kim; Gerbrand Ceder

doi:10.1038/s41467-021-26006-3

Synthetic accessibility and stability rules of NASICONs

Nat Commun. 2021 Oct 1;12(1):5752. doi: 10.1038/s41467-021-26006-3.

Authors

Bin Ouyang^#^{1

2}, Jingyang Wang^#^{1

2}, Tanjin He^{1

2}, Christopher J Bartel^{1

2}, Haoyan Huo^{1

2}, Yan Wang³, Valentina Lacivita³, Haegyeom Kim¹, Gerbrand Ceder^{4

5}

Affiliations

¹ Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA, USA.
² Department of Materials Science and Engineering, University of California, Berkeley, CA, USA.
³ Advanced Material Lab, Samsung Research America, 10 Wilson Rd., Cambridge, MA, USA.
⁴ Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA, USA. gceder@berkeley.edu.
⁵ Department of Materials Science and Engineering, University of California, Berkeley, CA, USA. gceder@berkeley.edu.

^# Contributed equally.

Abstract

In this paper we develop the stability rules for NASICON-structured materials, as an example of compounds with complex bond topology and composition. By first-principles high-throughput computation of 3881 potential NASICON phases, we have developed guiding stability rules of NASICON and validated the ab initio predictive capability through the synthesis of six attempted materials, five of which were successful. A simple two-dimensional descriptor for predicting NASICON stability was extracted with sure independence screening and machine learned ranking, which classifies NASICON phases in terms of their synthetic accessibility. This machine-learned tolerance factor is based on the Na content, elemental radii and electronegativities, and the Madelung energy and can offer reasonable accuracy for separating stable and unstable NASICONs. This work will not only provide tools to understand the synthetic accessibility of NASICON-type materials, but also demonstrates an efficient paradigm for discovering new materials with complicated composition and atomic structure.