Elucidating the influence of structure and Ag+ -Na+ ion-exchange on crack-resistance and ionic conductivity of Na3Al1.8Si1.65 P-1.8 O-12 glass electrolyte


Glasses are emerging as promising and efficient solid electrolytes for all-solid-state sodium-ion batteries. However, they still suffer from poor ionic conductivity and crack-resistance, which need to be improved for better battery performance, reliability, and service life. The current study shows a significant enhancement in crack resistance (from 11.3 N to 32.9 N) for Na3Al (1.8) Si-1.65 P1.8O12 glass (Ag-0 glass) upon Na+ -Ag+ ion-exchange (IE) due to compressive stresses generated in the glass surface while the ionic conductivity values (similar to 10(-5) S/cm at 473 K) were retained. In this study, magic angle spinning-nuclear magnetic resonance (MAS-NMR), molecular dynamics (MD) simulations, Vickers micro hardness, and impedance spectroscopic techniques were used to evaluate the intermediate-range structure, atomic structure, crack resistance and conductivity of the glass. MAS-NMR and MD simulations confirm the presence of Si-OAl-O-P groups in the glass, thus enabling formation of Na percolated channel regions. AC-conductivity analysis for Ag-0 and ion-exchanged Ag-0 glass suggests that the mobility of Na+ ion increases with increasing temperature. It is observed that the measured mean square displacement (root < R-2(t(p))>) for sodium cations using AC-conductivity isotherms is nearly constant up to 448 K and then increases with increasing temperature up to 523 K. From the impedance spectra for ion-exchanged Ag-0 glass, it is identified that the increase in root < R-2 (t(nu))> and thereby, the mobility of sodium-ions for Ag-0 glass is due to the structural variations in the Ag-0 glass with increasing the temperature. Overall, the mechanisms presented in this article helps in formulating better glass based electrolyte materials for room temperature or high temperature sodium-ion batteries. (C) 2022 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.



subject category

Materials Science; Metallurgy & Metallurgical Engineering


Keshri, SR; Mandal, I; Ganisetti, S; Kasimuthumaniyan, S; Kumar, R; Gaddam, A; Shelke, A; Ajithkumar, TG; Gosvami, NN; Krishnan, NMA; Allu, AR

our authors


The authors thank Dr. Suman Kumari Mishra, Director, CSIRCGCRI for her continuous support and encouragement. This work was developed under the frame of the project funded by the Science and Engineering Research Board (SERB), DST, Govt. of India, India, through the Early Career Research Award (ECR/2018/00 0292). S. R. K., I. M. and A. R. A. acknowledge the financial support by DST-SERB (ECR/2018/0 00292). AG is grateful for the support from the Sao Paulo Research Foundation (FAPESP Processo n degrees 2021/06370-0) and CeRTEV (Center for Research, Technology, and Education in Vitreous Materials-process FAPESP n degrees 2013/07793-6). N.M.A.K. acknowledges the funding support received from SERB (ECR/2018/002228) and DST (DST/INSPIRE/04/2016/002774). The authors also thank the IIT Delhi HPC facility for providing the computational and storage resources.

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