Enabling long-term oxide based solid-state lithium metal battery through a near room-temperature sintering process

doi:10.1016/j.jcis.2023.09.125

Enabling long-term oxide based solid-state lithium metal battery through a near room-temperature sintering process

2024-01-01

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DOI：10.1016/j.jcis.2023.09.125

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The huge Li ion transport resistance through the grain boundaries (GBs) among rigid oxide particles forces the adoption of high-temperature sintering (HTS) process over 1000 degrees C. Nevertheless, the severe side reactions and uncontrollable lithium loss are always companied during the high-cost HTS process, which slows down the pace of oxide solid electrolyte (OSE) for practical application and accelerates the exploration of a new OSE sintering process. Herein, a near-room-temperature (60 degrees C) cold-sintering process is proposed by filling the GBs with a low-melting-point plastic crystal electrolyte (PCE). Due to the soft property and high-ionic conductivity of PCE, the Li ion transport rate through the GBs is 10 times faster than the bulk phase, endowing the OSE (Li1.5Al0.5Ge1.5(PO4)(3) chosen as a representative) with a room temperature ionic conductivity of 0.25 mS cm(-1). As proof of the concept, the assembled Li symmetrical cells perform a low over-potential of 50 mV with a capacity of 1 mA h cm(-2) and full cells delivers a capacity retention of roughly 70% after 820 cycles (1.5 years) at 0.1C.

Keywords:

Oxide solid state battery

Li metal battery

Cold sintering process

Molecular dynamic simulation

Density function calculation

Enabling long-term oxide based solid-state lithium metal battery through a near room-temperature sintering process

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