Abstract

Garnet-type solid electrolytes with cubic modification are considered to be one of the most promising candidates for SSLBs with desirable properties such as high ionic conductivity at room temperature, and wider electrochemical operational window.

Highlights

  • They suffer from poor rate capabilities at lower temperatures and are un-safe to operate at elevated temperatures, while the next-generation of LiBs using Li-metal anodes and a solid electrolyte are anticipated to overcome drawbacks associated with liquid-based LiBs and can deliver up to a two-fold increase in energy density.[3]

  • A water-soluble fuel i.e., carbohydrazide (CH6N4O) having a low melting point: B154 1C was utilized for synthesizing Al-substituted LLZO

  • To understand the formation mechanism of cubic Al-LLZO, the fuel to oxidizer ratio (F/O) ratio was systematically varied from a fuel-lean zone (F/O = 0.5) to fuel-rich zone (F/O = 4.0), followed by a calcination step of as-burnt powders at 900 1C for a duration of 4 h

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Summary

Experimental section

Stoichiometric amounts of LiNO3 (Alfa Aesar, CAS No 7790-69-4, 10 wt% excess Li source was added to compensate Li loss during the combustion reaction or sintering), La(NO3)3Á6H2O (Alfa Aesar, CAS No 10277-43-7), Al(NO3)3Á9H2O (Millipore Sigma, CAS No 7784-27-2) and ZrO(NO3)ÁxH2O (Millipore Sigma, CAS No 14985-18-3) were dissolved in a minimum amount of ultra-pure DI water at 80 1C. Carbohydrazide (CH6N4O) fuel (Millipore Sigma, CAS No 497-18-7) was dissolved in ultra-pure DI water and subsequently mixed/stirred with the precursor solution at 80 1C for about 10 min until gelation occurred. The green pellets were kept covered with the sacrificial mother powder (to prevent loss of Li) in the MgO crucible with a lid covering during sintering. The theoretical density of the Al-LLZO pellet was considered to be 5.1 g cmÀ3 29,53 and the relative density of the sintered pellets was calculated based on the volume and weight after sintering

Characterization
Results and discussion
Effect of sintering temperatures on microstructure and ionic conductivity
Conclusions

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