The Discharge Mechanism for Solid-State Lithium-Sulfur Batteries
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MRS Advances © 2019 Materials Research Society DOI: 10.1557/adv.2019.255
The Discharge Mechanism for Solid-State LithiumSulfur Batteries Erika Nagai1,2, Timothy S. Arthur*1, Patrick Bonnick1, Koji Suto1 and John Muldoon1 1
Toyota Research Institute of North America, 1555 Woodridge Avenue, Ann Arbor, MI 48105, USA
2
Toyota Motor Corporation, Higashifuji Technical Center, 1200 Mishuku, Susono, Shizuoka 410-1193, Japan
*Corresponding author: Timothy S. Arthur ([email protected])
Abstract
The electrochemical discharge mechanism is reported for all-solid lithium sulfur batteries. Upon milling with carbon fibers, the solid electrolyte used within the cathode composite becomes electrochemically active. Analysis with Raman spectroscopy and XPS revealed the importance of bridging S-S bond formation and breaking in lithium polysulfidophosphates during electrochemical lithiation of the active solid electrolyte. Remarkably, when sulfur is introduced as an active material in the cathode composite, lithium polysulfides are formed as an intermediate product before full lithiation into lithium sulfide. The synthesis of materials based on bridging S-S bonds is an important avenue to the design of new cathodes for allsolid batteries.
INTRODUCTION: To power the future of mobility, diverse energy storage systems are critical as society moves towards electric, hybrid and fuel-cell powered vehicles. Vehicle electrification carries additional complexities of safety, range and cost to achieve
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practical product development. Li-ion batteries have emerged as a leading candidate to replace Ni-MH batteries, however, the need for longer-lasting, faster-charging, furtherrange electric vehicles has diversified research into post-Li-ion battery materials, structure and systems [1-3]. One potential, attractive replacement is solid-state batteries; which premise is to replace the organic liquid electrolytes typically found in Li-ion batteries with a solid-state ion conductor [4,5]. Wide electrochemical windows, nonflammability, and the potential to realize the lithium metal anode are advantages pushing solid-state batteries to the fore-front of the next generation of energy storage. However, to compete with conventional, liquid electrolytes, achieving high Li + conductivity is a tremendous challenge. The field of solid-state ionics has progressed rapidly, and the variety of Liion conductors which can realize fast Li+ transport at moderate temperatures are enabling the next generation of electrochemical storage. Polymer, gel, molten salt and ceramic electrolytes have strengths and challenges when faced with integration into practical devices; however, sulfide-based electrolytes have emerged as contender whose conductivity can match, and surpass, organic-liquid electrolytes [6]. LGPS, Li7P3S11 glas
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