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Elucidating Ion Transport Phenomena in Sulfide/Polymer composite electrolytes for Practical solid-state Batteries

Nano-Micro Letters 2023年第10期15卷 416-432页

作者： Kyeong‑Seok Oh Ji Eun Lee Yong‑Hyeok Lee Yi‑Su Jeong Imanuel Kristanto Hong‑Seok Min Sang‑Mo Kim Young Jun Hong Sang Kyu Kwak Sang‑Young Lee Department of Chemical and Biomolecular Engineering Yonsei University50 Yonsei‑roSeodaemun‑guSeoul 03722Republic of Korea Department of Chemical and Biological Engineering Korea University145 Anam‑roSeongbuk‑guSeoul 02841Republic of Korea School of Energy and Chemical Engineering Ulsan National Institute of Science and Technology(UNIST)50 UNIST‑gilEonyang‑eupUlju‑gunUlsan 44919Republic of Korea Hyundai Motor Company 150Hyundaiyeonguso‑roNamyang‑eupHwaseong‑siGyeonggi‑do 18280Republic of Korea

Despite the enormous interest in inorganic/polymer composite solid-state electrolytes(CSEs)for solid-state batteries(SSBs),the underlying ion transport phenomena in CSEs have not yet been ***,we address this issue by formulating a mechanistic understanding of bi-percolating ion channels formation and ion conduction across inorganic-polymer electrolyte interfaces in CSEs.A model CSE is composed of argyrodite-type Li_6PS_5Cl(LPSCl)and gel polymer electrolyte(GPE,including Li~+-glyme complex as an ion-conducting medium).The percolation threshold of the LPSCl phase in the CSE strongly depends on the elasticity of the GPE ***,manipulating the solvation/desolvation behavior of the Li~+-glyme complex in the GPE facilitates ion conduction across the LPSCl-GPE *** resulting scalable CSE(area=8×6(cm×cm),thickness~40μm)can be assembled with a high-mass-loading LiNi_(0.7)Co_(0.15)Mn_(0.15)O_(2)cathode(areal-mass-loading=39 mg cm~(-2))and a graphite anode(negative(N)/positive(P)capacity ratio=1.1)in order to fabricate an SSB full cell with bi-cell *** this constrained cell condition,the SSB full cell exhibits high volumetric energy density(480 Wh L_(cell)~(-1))and stable cyclability at 25℃,far exceeding the values reported by previous CSE-based SSBs.

关键词： solid-state batteries composite solid-state electrolytes Ion transport phenomena Bi-percolating ion channels Interfacial resistance

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Ultrathin salt-free polymer-in-ceramic electrolyte for solid-state sodium batteries

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eScience 2021年第2期1卷 194-202页

作者： Bin Tang Yibo Zhao Zhiyi Wang Shiwei Chen Yifan Wu Yuming Tseng Lujiang Li Yunlong Guo Zhen Zhou Shou-Hang Bo Engineering Research Center of Advanced Functional Material Manufacturing of Ministry of Education School of Chemical EngineeringZhengzhou UniversityZhengzhou450001PR China University of Michigan-Shanghai Jiao Tong University Joint Institute Shanghai Jiao Tong University800 Dong Chuan Rd.Minhang DistrictShanghai200240PR China Department of Chemistry City University of Hong KongTat Chee AvenueKowloonHong Kong SAR999077PR China School of Materials Science and Engineering Institute of New Energy Material ChemistryKey Laboratory of Advanced Energy Materials Chemistry(Ministry of Education)Renewable Energy Conversion and Storage Center(ReCast)Nankai UniversityTianjin300350PR China School of Chemistry and Chemical Engineering Shanghai Jiao Tong University800 Dong Chuan Rd.Minhang DistrictShanghai200240PR China

The practical energy density of solid-state batteries remains limited,partly because of the lack of a general method to fabricate thin membranes for solid-state electrolytes with high ionic conductivity and low area-specific resistance(ASR).Herein,we use an ultrahigh concentration of a ceramic ion conductor(Na_(3)SbS_(4))to build an ionconduction“highway”,and a polymer(polyethylene oxide,2 wt%)as a flexible host to prepare a polymer-inceramic ion-conducting membrane of approximately 40μ*** the use of any salt(e.g.,NaPF_(6)),the resulting membrane exhibits a threefold increase in electronic ASR and a twofold decrease in ionic ASR compared with a pure ceramic *** activation energy for sodium-ion transport is only 190 meV in the membrane,similar to that in pure ceramic,suggesting ion transport predominantly occurs through a percolated network of ion-conducting ceramic *** salt-free design also provides an opportunity to suppress dendritic metal electrodeposits,according to a recently refined chemomechanical model of metal *** work suggests that salt is not always necessary in composite solid-state electrolytes,which broadens the choice of polymers to allow the optimization of other desired attributes,such as mechanical strength,chemical/electrochemical stability,and cost.

关键词： composite solid-state electrolytes Hydrostatic hot-pressing Salt-free Polymer-in-ceramic

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