title: Infiltration of Solution-Processable Solid Electrolytes into Conventional Li-Ion-Battery Electrodes for All-Solid-State Li-Ion Batteries.
abstract: Bulk-type all-solid-state lithium-ion batteries (ASLBs) have the potential to be superior to conventional lithium-ion batteries (LIBs) in terms of safety and energy density. Sulfide SE materials are key to the development of bulk-type ASLBs because of their high ionic conductivity (max of ∼10-2S cm-1) and deformability. However, the severe reactivity of sulfide materials toward common polar solvents and the particulate nature of these electrolytes pose serious complications for the wet-slurry process used to fabricate ASLB electrodes, such as the availability of solvent and polymeric binders and the formation of ionic contacts and networks. In this work, we report a new scalable fabrication protocol for ASLB electrodes using conventional composite LIB electrodes and homogeneous SE solutions (Li6PS5Cl (LPSCl) in ethanol or 0.4LiI-0.6Li4SnS4in methanol). The liquefied LPSCl is infiltrated into the tortuous porous structures of LIB electrodes and solidified, providing intimate ionic contacts and favorable ionic percolation. The LPSCl-infiltrated LiCoO2and graphite electrodes show high reversible capacities (141 and 364 mA h g-1) at 0.14 mA cm-2(0.1 C) and 30 °C, which are not only superior to those for conventional dry-mixed and slurry-mixed ASLB electrodes but also comparable to those for liquid electrolyte cells. Good electrochemical performance of ASLBs employing the LPSCl-infiltrated LiCoO2and graphite electrodes at 100 °C is also presented, highlighting the excellent thermal stability and safety of ASLBs.
authors.affiliation: School of Energy and Chemical Engineering, Department of Energy Engineering, Ulsan National Institute of Science and Technology (UNIST) , Ulsan 44919, South Korea.
authors.forename: Dong Hyeon
authors.initials: DH
authors.lastname: Kim
authors.affiliation: School of Energy and Chemical Engineering, Department of Energy Engineering, Ulsan National Institute of Science and Technology (UNIST) , Ulsan 44919, South Korea.
authors.forename: Dae Yang
authors.initials: DY
authors.lastname: Oh
authors.affiliation: School of Energy and Chemical Engineering, Department of Energy Engineering, Ulsan National Institute of Science and Technology (UNIST) , Ulsan 44919, South Korea.
authors.forename: Kern Ho
authors.initials: KH
authors.lastname: Park
authors.affiliation: School of Energy and Chemical Engineering, Department of Energy Engineering, Ulsan National Institute of Science and Technology (UNIST) , Ulsan 44919, South Korea.
authors.forename: Young Eun
authors.initials: YE
authors.lastname: Choi
authors.affiliation: School of Energy and Chemical Engineering, Department of Energy Engineering, Ulsan National Institute of Science and Technology (UNIST) , Ulsan 44919, South Korea.
authors.forename: Young Jin
authors.initials: YJ
authors.lastname: Nam
authors.affiliation: School of Energy and Chemical Engineering, Department of Energy Engineering, Ulsan National Institute of Science and Technology (UNIST) , Ulsan 44919, South Korea.
authors.forename: Han Ah
authors.initials: HA
authors.lastname: Lee
authors.affiliation: Battery Research Center, Korea Electrotechnology Research Institute , 12 Bulmosan-ro 10 beon-gil, Changwon 642-120, South Korea.
authors.forename: Sang-Min
authors.initials: SM
authors.lastname: Lee
authors.affiliation: School of Energy and Chemical Engineering, Department of Energy Engineering, Ulsan National Institute of Science and Technology (UNIST) , Ulsan 44919, South Korea.
authors.forename: Yoon Seok
authors.identifier: 0000-0003-0357-9508
authors.initials: YS
authors.lastname: Jung
keywords: All-solid-state batteries; coatings; electrodes; infiltration; lithium-ion batteries; solid electrolytes; solution-process; sulfides