Electrochemical properties of all-solid-state lithium secondary batteries using Li-argyrodite Li 6 PS 5 Cl as solid elec
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Electrochemical properties of all-solid-state lithium secondary batteries using Liargyrodite Li6PS5Cl as solid electrolyte Sylvain Boulineau, Jean-Marie Tarascon, Vincent Seznec and Virginie Viallet LRCS, CNRS-UMR 7314, Université de Picardie Jules Verne, 33 Rue Saint Leu, 80039 Amiens, France
ABSTRACT Highly ion-conductive Li6PS5Cl Li-argyrodites were prepared through a high energy ball milling. Electrical and electrochemical properties were investigated. Ball-milled compounds exhibit a high conductivity of 1.3310-4 S/cm with an activation energy of 0.3-0.4 eV and an electrochemical stability up to 7V vs. lithium. These results are obtained after only 10 hours of milling and with no additional heat treatment. To validate the use of the Li6PS5Cl-based solid electrolyte, all-solid-state batteries using LiCoO2 and Li4Ti5O12 as active material have been realized. The optimization of the electrode composition led to a maximum of 46 and 27 mAh per gram of composite for LiCoO2 and Li4Ti5O12-based half-cells respectively. The assembled all-solid-state LiCoO2 / Li6PS5Cl / Li4Ti5O12 battery presents a sustainable reversible capacity of 27 mAh per gram of active material and a coulomb efficiency close to 99%.
INTRODUCTION Because of its high energy density and long cycle life, the lithium ion battery technology is the most attractive energy storage and output source for mobile devices. It is also regarded as the technology of choice for the electrification of transport enlisting Hybrid Electric Vehicles (HEV) and Electric Vehicles (EV), provided that safety-related issues linked to the use of an organic liquid electrolyte which may induce sizeable risks of fire and explosion [1] are satisfactorily addressed. In this respect, so-called “all-solid-state” batteries, employing non-flammable solid electrolytes, have been recognized, and developed as good, safer, alternatives [2, 3]. Argyrodites, a class of compounds derived from the mineral Ag8GeS6 [4], may possess high + Ag or Cu+ ion conductivities, as reported for γ-Ag9AlSe6 or Cu6PS5Cl. From preliminary impedance measurements, Deiseroth et al. [5] reported in 2008 on cubic Li-containing Argyrodites of general formula Li7-xPS6-xXx (0 < x < 1; X = Cl, Br, I) and with promising high values for Li+ ion conductivities; they ranged from 10-2 to 10-3 S/cm, i.e. close to the conductivity of standard liquid electrolytes. In 2010, Pecher et al. reported values close to 410-7 S/cm for Li6PS5I [6]. During the course of our study, Rao et al. independently confirmed a high ionic conductivity of 310-3 S/cm and 710-3 S/cm at 298K for Li6PS5Cl and Li6PS5Br, respectively; both were prepared through mechanical milling and then heated for 5h at 550°C [7]. Stadler et al. recently reported on the use of Br-containing Li-argyrodites compositions (samples provided by Deiseroth; 1.010-4 S/cm at 298K, electrochemically stable from 1 to 5V vs. Li/Li+) in all-solid-state batteries using carbon coated Li4Ti5O12 (c-LTO) and Li-Al alloy as
active positive and negative electrode materials respective
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