Abstract
Solid electrolytes, such as perovskite Li3xLa2/1−xTiO3, LixLa(1−x)/3NbO3 and garnet Li7La3Zr2O12 ceramic oxides, have attracted extensive attention in lithium-ion battery research due to their good chemical stability and the improvability of their ionic conductivity with great potential in solid electrolyte battery applications. These solid oxides eliminate safety issues and cycling instability, which are common challenges in the current commercial lithium-ion batteries based on organic liquid electrolytes. However, in practical applications, structural disorders such as point defects and grain boundaries play a dominating role in the ionic transport of these solid electrolytes, where defect engineering to tailor or improve the ionic conductive property is still seldom reported. Here, we demonstrate a defect engineering approach to alter the ionic conductive channels in LixLa(1−x)/3NbO3 (x = 0.1~0.13) electrolytes based on the rearrangements of La sites through a quenching process. The changes in the occupancy and interstitial defects of La ions lead to anisotropic modulation of ionic conductivity with the increase in quenching temperatures. Our trial in this work on the defect engineering of quenched electrolytes will offer opportunities to optimize ionic conductivity and benefit the solid electrolyte battery applications.
Highlights
Commercial lithium-ion batteries have shaped the new era and people’s daily lives, owing to their successful portable electronics applications in vehicles and mobile phones, etc
Among the available lithium-ion-conducting solid electrolytes, ceramic oxides (10−5~10−3 S·cm−1) such as perovskite materials Li3xLa2/1−xTiO3 (LLTO) [18,19,20,21] and LixLa(1−x)/3NbO3 (LLNO) [22,23,24], anti-perovskite Li3OX (X = Cl, Br)[25,26,27] and garnet structured Li7La3Zr2O12 (LLZO) [28,29,30,31] have received much attention due to their good electrochemical stability and considerable potential to push the limit of ionic conductivity towards a desired level (~10−2 S·cm−1) in the industrial application of batteries
Through aberration-corrected scanning transmission electron microscopy (STEM), we have identified the layered structure property of LLNO by atomic resolution annular dark/bright field (ADF/ABF) imaging, together with energy dispersive X-ray spectroscopy (EDX) mapping to visualize the layered chemical structure in atomic resolution
Summary
Commercial lithium-ion batteries have shaped the new era and people’s daily lives, owing to their successful portable electronics applications in vehicles and mobile phones, etc. Among the available lithium-ion-conducting solid electrolytes, ceramic oxides (10−5~10−3 S·cm−1) such as perovskite materials Li3xLa2/1−xTiO3 (LLTO) [18,19,20,21] and LixLa(1−x)/3NbO3 (LLNO) [22,23,24], anti-perovskite Li3OX (X = Cl, Br)[25,26,27] and garnet structured Li7La3Zr2O12 (LLZO) [28,29,30,31] have received much attention due to their good electrochemical stability and considerable potential to push the limit of ionic conductivity towards a desired level (~10−2 S·cm−1) in the industrial application of batteries. Our trial in this work on the defect characterization of the quenched single-crystal LLNO will offer new opportunities to optimize the ionic conductivity and benefit in its potential applications in the new solid electrolyte batteries
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