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A disruptive sintering technique, Cold Sintering Process (CSP), has been used to produce cold-sintered samples of Bi 2 O 3 -doped Li 1.3 Al 0.3 Ti 1.7 (PO 4) 3 (LATP) as solid-state electrolyte (SSE). An in operando impedance study has been performed to shed light on this sintering process. In this work, Bi 2 O 3 and 3 m acetic acid solution sintering aids were synergistically added to LATP powders to sinter at low temperature. Effects of Transient Liquid Phase (TLP) content on the sintering behavior, phase composition, microstructure, and electrochemical properties were all investigated for a LATP doped with 2 wt% Bi 2 O 3 (optimal content) solid-state electrolyte (SSE). The data revealed that the final electrical properties, which are the key parameter decisive for their application, are defined by the following sintering parameters: Transient Liquid Phase (TLP) content, temperature, pressure, and dwell time. Using acetic acid 3 m as TLP, LATP-based samples can be cold-sintered at optimized sintering conditions of 150 °C and 700 MPa of uniaxial pressure for 90 min. The resultant SSE shows a high ionic conductivity (4.5·10−5 S cm−1) at room temperature (RT) and relative density (∼95%), which demonstrates the effectiveness of the low-temperature sintering process by optimizing the ionic conductivity of LATP-based SSE, also reducing preparation costs and CO 2 emissions. [ABSTRACT FROM AUTHOR]

In the present work, a Polymer-In-Ceramics (PIC) solid electrolyte based on Li 1.3 Al 0.3 Ti 1.7 (PO 4) 3 (LATP) and PEO n -LiTFSI (poly(ethylene oxide) - lithium bis(trifluoromethanesulfonyl)imide) is obtained via Cold Sintering Process (CSP), at a temperature of 150 °C without any post-heat treatment, this is 900 °C below the traditional sintering temperature. This novel study demonstrates the effect of the Transient Liquid Phase content (TLP) and the composition of the polymeric active filler on the final Composite Solid Electrolyte (CSE) properties, with the sintering process being monitored by in-operando Electrochemical Impedance Spectroscopy (EIS). Firstly, the 15 wt% of TLP is stated as the optimal liquid content based on the electrical answer and workability. Then, the (EO:Li+) molar ratio is studied from (1:1) to (8:1). The highest ionic conductivity of 1.04·10−4 S cm−1 and a relative density above 98% are achieved at room temperature when the TLP content is 15 wt% and the molar ratio (2:1), with the LATP content set in 90 wt%. Moreover, the activation energy (Ea) is drastically reduced, from 0.388 eV (LATP ceramic electrolyte) to 0.298 eV (PIC electrolyte), with a lithium transference number (t Li +) close to 1. Therefore, this research work proposes a potential solid electrolyte to substitute the traditional liquid electrolytes. • Modification strategies of ceramic electrolytes sintering are focused on. • Cold Sintering Process method to sinter LATP-based Composite Solid Electrolyte. • The future of ASSLBs using Polymer-in-Ceramic electrolytes is discussed. • PEO n -LiTFSI doping of ceramic electrolytes to improve the ionic conductivity. [ABSTRACT FROM AUTHOR]