xamxamIIPOII〇P1-3Sintering-based fabrication of ASSB40STEM(DF)STEM(DF)TiAlx: 0.01~0.02• LiTiO(PO4)• AlPO4y: 0.05~0.1• LiCoPO4• AlPO4y: 0.01~0.02• LiTiO(PO4)• AlPO4(LATP)Significantly high sinterability of Co-LATP originates from low-Tm phase (LiPO3)series (A)• Co2+ in exchange for Ti4+• Li1.3+2xAl0.3CoxTi1.7-x(PO4)3series (B)• Co2+ in exchange for Li+• Li1.3-2yCoyAl0.3Ti1.7(PO4)3• No significant densification• Coexist with LiCoPO4, AlPO4Miyoshi et al., ACS Appl. Energy Mater. 2022, 5, 7515.Phases in series(A)Phases in series(B)LATP-LCP800℃℃(A)〇〇〇LiCoPO4LiTiOPO4LiPO3AlPO4series(A) vs. series(B)Relative density vs. Co-contentHighly sinterable compositions include:(XRD) LiCoPO4, LiTiO(PO4)STEM/EDS(x=0.1) Co-LATP (shaded in the phase diagram) is sinterable. High sinterability is ascribed to equilibrium formation of a low-melting-point compound, LiPO3, which turns into liquid to assist mass transport during sintering. The influence of Co introduction on the ionic conduction behavior will be studied. Sintering aids suggested by the mechanism will be examined.Positive electrodeElectrolyteNegative electrodeCoexisting phases @ x, y=0.1LATP (Li1.3Al0.3Ti1.7(PO4)3)• NASICON-type electrolyte• Chemically stable• σ(bulk) > 10-3 Sꞏcm-1• Low tolerance for reductionLCP (LiCoPO4)• Olivine-type positive electrode• Chemically stable• 4.8V vs Li+/Li• Low σ(electronic)(STEM) Li-P-O phaseIdentification with XRDx: 0.05~0.3• LiCoPO4• LiTiO(PO4)• LiPO3Identification with XRDHigh sinterability previously observed forthe mixture of LATP-LCPSinterability and phases of Co-introduced LATP Densification of electrolyte Electrolyte-electrode bonding Low-T sintering: poor densification High-T sintering: resistive phases formdilemma as to high-T sintering:densification and resistive phasesDensification via low-T sinteringKey Words: all-solid-state battery, solid electrolyte, low-temperature sinteringKey Words: all-solid-state battery, solid electrolyte, low-temperature sinteringTheme underDiscussionDiscussionFuture PlanResults and discussionConclusion(B)〇Tm(oC)>8001085665~2000For realization of all-solid-state batteries (ASSB), it is essential to densify the electrolyte materials to increase interface area between the materials with sufficient conductance. While high-temperature sintering is necessary to reduce interfacial resistance, undesirable resistive phases may form as the reaction products between electrolyte and electrode materials.The study is devoted to lower the sintering temperature of oxide-based solid-state electrolyte. Focusing on the high sinterability previously observed for the mixture of NASICON-typesolid electrolyte and olivine-type positive electrode, the mechanism of the sinterability improvement is studied to provide a guideline for lowering sintering temperature.Battery Interface Control Group, GREEN Shogo MIYOSHIE-mail：： MIYOSHI.Shogo@nims.go.jpIntroductionSinterability Improvement of NASICON-type Sinterability Improvement of NASICON-type Electrolyte for Solid-state BatteryElectrolyte for Solid-state Battery
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