Ashton, Thomas E; Baker, Peter J; Shakespeare, Yiana S; Commandeur, Daniel; Darr, Jawwad A; (2022) Phase Evolution and Li Diffusion in LATP Solid-State Electrolyte Synthesized via a Direct Heat-Cycling Method. Advanced Energy and Sustainability Research , Article 2200017. 10.1002/aesr.202200017. (In press).

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Abstract

Herein, the direct synthesis of phase-pure lithium aluminum titanium phosphate (Li_{1.3}Al_{0.3}Ti_{1.7}(PO_{4})_{3}, LATP) solid-electrolyte powder in 220 min and relatively low temperatures (850 °C) is achieved via a new (cyclic) fast heat treatment (c-FHT) route. The complex structural evolution highlights rate-limited lithium incorporation of intermediate metal phosphates formed prior to the final phase-pure LATP. The prepared LATP product powder displays similar bulk (2 × 10^{−10} cm^{2} s^{−1}) and local (3 × 10^{−10} cm^{2} s^{−1}) values for lithium diffusion coefficients (D_{Li}) characterized by electrochemical impedance spectroscopy and muon spin relaxation (μSR), respectively. The similarity between both D_{Li} values suggests excellent retention of inter- and intraparticle lithium diffusion, which is attributed to the absence of deleterious surface impurities such as AlPO4. A low-energy barrier (E_{a} = 73 meV) of lithium diffusion is also estimated from the μSR data.

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