Realizing high-capacity all-solid-state lithium-sulfur batteries using a low-density inorganic solid-state electrolyte

Wang, Daiwei; Jhang, Li-Ji; Kou, Rong; Liao, Meng; Zheng, Shiyao; Jiang, Heng; Shi, Pei; Li, Guo-Xing; Meng, Kui; Wang, Donghai

doi:10.1038/s41467-023-37564-z

Title: Realizing high-capacity all-solid-state lithium-sulfur batteries using a low-density inorganic solid-state electrolyte

Journal Article · 04 April 2023 · Nature Communications

DOI: https://doi.org/10.1038/s41467-023-37564-z · OSTI ID:1968540

; Jhang, Li-Ji; Kou, Rong; Liao, Meng; Zheng, Shiyao; Jiang, Heng; Shi, Pei; Li, Guo-Xing; Meng, Kui;

Abstract Lithium-sulfur all-solid-state batteries using inorganic solid-state electrolytes are considered promising electrochemical energy storage technologies. However, developing positive electrodes with high sulfur content, adequate sulfur utilization, and high mass loading is challenging. Here, to address these concerns, we propose using a liquid-phase-synthesized Li ₃ PS ₄ -2LiBH ₄ glass-ceramic solid electrolyte with a low density (1.491 g cm ⁻³ ), small primary particle size (~500 nm) and bulk ionic conductivity of 6.0 mS cm ⁻¹ at 25 °C for fabricating lithium-sulfur all-solid-state batteries. When tested in a Swagelok cell configuration with a Li-In negative electrode and a 60 wt% S positive electrode applying an average stack pressure of ~55 MPa, the all-solid-state battery delivered a high discharge capacity of about 1144.6 mAh g ⁻¹ at 167.5 mA g ⁻¹ and 60 °C. We further demonstrate that the use of the low-density solid electrolyte increases the electrolyte volume ratio in the cathode, reduces inactive bulky sulfur, and improves the content uniformity of the sulfur-based positive electrode, thus providing sufficient ion conduction pathways for battery performance improvement.

View Journal Article

Cite

Export

Save

Research Organization:: Pennsylvania State University, University Park, PA (United States)

Sponsoring Organization:: USDOE; USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO). Batteries for Advanced Transportation Technologies (BATT) Program

Grant/Contract Number:: EE0008862

OSTI ID:: 1968540

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 14; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United Kingdom

Language:: English

References (59)

A High Capacity All Solid‐State Li‐Sulfur Battery Enabled by Conversion‐Intercalation Hybrid Cathode Architecture Xu, Shiqi; Kwok, Chun Yuen; Zhou, Laidong Advanced Functional Materials, Vol. 31, Issue 2 https://doi.org/10.1002/adfm.202004239	journal	November 2020
A Self‐Limited Free‐Standing Sulfide Electrolyte Thin Film for All‐Solid‐State Lithium Metal Batteries Zhu, Gao‐Long; Zhao, Chen‐Zi; Peng, Hong‐Jie Advanced Functional Materials, Vol. 31, Issue 32 https://doi.org/10.1002/adfm.202101985	journal	June 2021
High‐Performance Li–SeS _x All‐Solid‐State Lithium Batteries Li, Xiaona; Liang, Jianwen; Luo, Jing Advanced Materials, Vol. 31, Issue 17 https://doi.org/10.1002/adma.201808100	journal	March 2019
High-Performance All-Solid-State Lithium-Sulfur Batteries Enabled by Amorphous Sulfur-Coated Reduced Graphene Oxide Cathodes Yao, Xiayin; Huang, Ning; Han, Fudong Advanced Energy Materials, Vol. 7, Issue 17 https://doi.org/10.1002/aenm.201602923	journal	May 2017
High Capacity All-Solid-State Lithium Batteries Enabled by Pyrite-Sulfur Composites Ulissi, Ulderico; Ito, Seitaro; Hosseini, Seyed Milad Advanced Energy Materials, Vol. 8, Issue 26 https://doi.org/10.1002/aenm.201801462	journal	July 2018
High Active Material Loading in All‐Solid‐State Battery Electrode via Particle Size Optimization Shi, Tan; Tu, Qingsong; Tian, Yaosen Advanced Energy Materials, Vol. 10, Issue 1 https://doi.org/10.1002/aenm.201902881	journal	November 2019
Lithium Argyrodite as Solid Electrolyte and Cathode Precursor for Solid‐State Batteries with Long Cycle Life Wang, Shuo; Tang, Mingxue; Zhang, Qinghua Advanced Energy Materials, Vol. 11, Issue 31 https://doi.org/10.1002/aenm.202101370	journal	July 2021
Lithium boro-hydride LiBH4 Gomes, S.; Hagemann, H.; Yvon, K. Journal of Alloys and Compounds, Vol. 346, Issue 1-2 https://doi.org/10.1016/S0925-8388(02)00668-0	journal	November 2002
Preparation of Li 7 P 3 S 11 glass-ceramic electrolyte by dissolution-evaporation method for all-solid-state lithium ion batteries Xu, R. C.; Xia, X. H.; Yao, Z. J. Electrochimica Acta, Vol. 219 https://doi.org/10.1016/j.electacta.2016.09.155	journal	November 2016
Improved interfacial electronic contacts powering high sulfur utilization in all-solid-state lithium–sulfur batteries Hou, Li-Peng; Yuan, Hong; Zhao, Chen-Zi Energy Storage Materials, Vol. 25 https://doi.org/10.1016/j.ensm.2019.09.037	journal	March 2020
CNTs@S composite as cathode for all-solid-state lithium-sulfur batteries with ultralong cycle life Zhang, Qiang; Huang, Ning; Huang, Zhen Journal of Energy Chemistry, Vol. 40 https://doi.org/10.1016/j.jechem.2019.03.006	journal	January 2020
High-Energy-Density Solid-Electrolyte-Based Liquid Li-S and Li-Se Batteries Jin, Yang; Liu, Kai; Lang, Jialiang Joule, Vol. 4, Issue 1 https://doi.org/10.1016/j.joule.2019.09.003	journal	January 2020
Microstructure engineering of solid-state composite cathode via solvent-assisted processing Zhang, Jibo; Chen, Zhaoyang; Ai, Qing Joule, Vol. 5, Issue 7 https://doi.org/10.1016/j.joule.2021.05.017	journal	July 2021
Additive effect of ionic liquids on the electrochemical property of a sulfur composite electrode for all-solid-state lithium–sulfur battery Kinoshita, Shunji; Okuda, Kazuya; Machida, Nobuya Journal of Power Sources, Vol. 269 https://doi.org/10.1016/j.jpowsour.2014.07.055	journal	December 2014
A synthesis of crystalline Li7P3S11 solid electrolyte from 1,2-dimethoxyethane solvent Ito, Seitaro; Nakakita, Moeka; Aihara, Yuichi Journal of Power Sources, Vol. 271 https://doi.org/10.1016/j.jpowsour.2014.08.024	journal	December 2014
Preparation of high lithium-ion conducting Li6PS5Cl solid electrolyte from ethanol solution for all-solid-state lithium batteries Yubuchi, So; Teragawa, Shingo; Aso, Keigo Journal of Power Sources, Vol. 293 https://doi.org/10.1016/j.jpowsour.2015.05.093	journal	October 2015
Composite cathode prepared by argyrodite precursor solution assisted by dispersant agents for bulk-type all-solid-state batteries Rosero-Navarro, Nataly Carolina; Miura, Akira; Tadanaga, Kiyoharu Journal of Power Sources, Vol. 396 https://doi.org/10.1016/j.jpowsour.2018.06.011	journal	August 2018
Structural change of Li2S–P2S5 sulfide solid electrolytes in the atmosphere Muramatsu, Hiromasa; Hayashi, Akitoshi; Ohtomo, Takamasa Solid State Ionics, Vol. 182, Issue 1 https://doi.org/10.1016/j.ssi.2010.10.013	journal	February 2011
Preparation of Li3PS4 solid electrolyte using ethyl acetate as synthetic medium Phuc, Nguyen Huu Huy; Totani, Mitsuhiro; Morikawa, Kei Solid State Ionics, Vol. 288 https://doi.org/10.1016/j.ssi.2015.11.032	journal	May 2016
Improvement of lithium ionic conductivity of Li3PS4 through suppression of crystallization using low-boiling-point solvent in liquid-phase synthesis Takahashi, Masakuni; Yang, Seunghoon; Yamamoto, Kentaro Solid State Ionics, Vol. 361 https://doi.org/10.1016/j.ssi.2021.115568	journal	March 2021
Interface Stability in Solid-State Batteries Richards, William D.; Miara, Lincoln J.; Wang, Yan Chemistry of Materials, Vol. 28, Issue 1 https://doi.org/10.1021/acs.chemmater.5b04082	journal	December 2015
Li ₄ PS ₄ I: A Li ⁺ Superionic Conductor Synthesized by a Solvent-Based Soft Chemistry Approach Sedlmaier, Stefan J.; Indris, Sylvio; Dietrich, Christian Chemistry of Materials, Vol. 29, Issue 4 https://doi.org/10.1021/acs.chemmater.7b00013	journal	February 2017
Experimental Assessment of the Practical Oxidative Stability of Lithium Thiophosphate Solid Electrolytes Dewald, Georg F.; Ohno, Saneyuki; Kraft, Marvin A. Chemistry of Materials, Vol. 31, Issue 20 https://doi.org/10.1021/acs.chemmater.9b01550	journal	September 2019
Interfaces and Interphases in All-Solid-State Batteries with Inorganic Solid Electrolytes Banerjee, Abhik; Wang, Xuefeng; Fang, Chengcheng Chemical Reviews, Vol. 120, Issue 14 https://doi.org/10.1021/acs.chemrev.0c00101	journal	June 2020
Approaching Practically Accessible Solid-State Batteries: Stability Issues Related to Solid Electrolytes and Interfaces Chen, Rusong; Li, Qinghao; Yu, Xiqian Chemical Reviews, Vol. 120, Issue 14 https://doi.org/10.1021/acs.chemrev.9b00268	journal	November 2019
Tailoring Solution-Processable Li Argyrodites Li _{6+ x} P _{1– x} M _x S ₅ I (M = Ge, Sn) and Their Microstructural Evolution Revealed by Cryo-TEM for All-Solid-State Batteries Song, Yong Bae; Kim, Dong Hyeon; Kwak, Hiram Nano Letters, Vol. 20, Issue 6 https://doi.org/10.1021/acs.nanolett.0c01028	journal	May 2020
High-Energy All-Solid-State Lithium Batteries with Ultralong Cycle Life Yao, Xiayin; Liu, Deng; Wang, Chunsheng Nano Letters, Vol. 16, Issue 11 https://doi.org/10.1021/acs.nanolett.6b03448	journal	October 2016
High Ionic Conductivity of Liquid-Phase-Synthesized Li ₃ PS ₄ Solid Electrolyte, Comparable to That Obtained via Ball Milling Yamamoto, Kentaro; Yang, Seunghoon; Takahashi, Masakuni ACS Applied Energy Materials, Vol. 4, Issue 3 https://doi.org/10.1021/acsaem.0c02771	journal	February 2021
Confining Sulfur in Porous Carbon by Vapor Deposition to Achieve High-Performance Cathode for All-Solid-State Lithium–Sulfur Batteries Alzahrani, Atif S.; Otaki, Mitsutoshi; Wang, Daiwei ACS Energy Letters, Vol. 6, Issue 2 https://doi.org/10.1021/acsenergylett.0c01956	journal	January 2021
Solvent-Engineered Design of Argyrodite Li ₆ PS ₅ X (X = Cl, Br, I) Solid Electrolytes with High Ionic Conductivity Zhou, Laidong; Park, Kern-Ho; Sun, Xiaoqi ACS Energy Letters, Vol. 4, Issue 1 https://doi.org/10.1021/acsenergylett.8b01997	journal	November 2018
Elucidating Reversible Electrochemical Redox of Li ₆ PS ₅ Cl Solid Electrolyte Tan, Darren H. S.; Wu, Erik A.; Nguyen, Han ACS Energy Letters, Vol. 4, Issue 10 https://doi.org/10.1021/acsenergylett.9b01693	journal	August 2019
Mechanochemically Prepared Li ₂ S–P ₂ S ₅ –LiBH ₄ Solid Electrolytes with an Argyrodite Structure Sakuda, Atsushi; Yamauchi, Akihiro; Yubuchi, So ACS Omega, Vol. 3, Issue 5 https://doi.org/10.1021/acsomega.8b00377	journal	May 2018
Structural transformation of non-oxide chalcogenide glasses. The short-range order of lithium sulfide (Li2S)-phosphorus pentasulfide (P2S5) glasses studied by quantitative phosphorus-31, lithium-6, and lithium-7 high-resolution solid-state NMR Eckert, Hellmut; Zhang, Zhengming; Kennedy, John H. Chemistry of Materials, Vol. 2, Issue 3 https://doi.org/10.1021/cm00009a017	journal	May 1990
Structural Evolution and Li Dynamics in Nanophase Li ₃ PS ₄ by Solid-State and Pulsed-Field Gradient NMR Gobet, Mallory; Greenbaum, Steve; Sahu, Gayatri Chemistry of Materials, Vol. 26, Issue 11 https://doi.org/10.1021/cm5012058	journal	May 2014
Anomalous High Ionic Conductivity of Nanoporous β-Li₃PS₄ Liu, Zengcai; Fu, Wujun; Payzant, E. Andrew Journal of the American Chemical Society, Vol. 135, Issue 3, p. 975-978 https://doi.org/10.1021/ja3110895	journal	January 2013
An Iodide-Based Li ₇ P ₂ S ₈ I Superionic Conductor Rangasamy, Ezhiylmurugan; Liu, Zengcai; Gobet, Mallory Journal of the American Chemical Society, Vol. 137, Issue 4 https://doi.org/10.1021/ja508723m	journal	January 2015
Lithium battery chemistries enabled by solid-state electrolytes Manthiram, Arumugam; Yu, Xingwen; Wang, Shaofei Nature Reviews Materials, Vol. 2, Issue 4 https://doi.org/10.1038/natrevmats.2016.103	journal	February 2017
Li–O₂ and Li–S batteries with high energy storage Bruce, Peter G.; Freunberger, Stefan A.; Hardwick, Laurence J. Nature Materials, Vol. 11, Issue 1, p. 19-29 https://doi.org/10.1038/nmat3191	journal	January 2012
A complex hydride lithium superionic conductor for high-energy-density all-solid-state lithium metal batteries Kim, Sangryun; Oguchi, Hiroyuki; Toyama, Naoki Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-019-09061-9	journal	March 2019
Growth of lithium-indium dendrites in all-solid-state lithium-based batteries with sulfide electrolytes Luo, Shuting; Wang, Zhenyu; Li, Xuelei Nature Communications, Vol. 12, Issue 1 https://doi.org/10.1038/s41467-021-27311-7	journal	November 2021
High-energy and durable lithium metal batteries using garnet-type solid electrolytes with tailored lithium-metal compatibility Kim, Sewon; Kim, Ju-Sik; Miara, Lincoln Nature Communications, Vol. 13, Issue 1 https://doi.org/10.1038/s41467-022-29531-x	journal	April 2022
A non-academic perspective on the future of lithium-based batteries Frith, James T.; Lacey, Matthew J.; Ulissi, Ulderico Nature Communications, Vol. 14, Issue 1 https://doi.org/10.1038/s41467-023-35933-2	journal	January 2023
Benchmarking the performance of all-solid-state lithium batteries Randau, Simon; Weber, Dominik A.; Kötz, Olaf Nature Energy, Vol. 5, Issue 3 https://doi.org/10.1038/s41560-020-0565-1	journal	March 2020
Clarifying the relationship between redox activity and electrochemical stability in solid electrolytes Schwietert, Tammo K.; Arszelewska, Violetta A.; Wang, Chao Nature Materials, Vol. 19, Issue 4 https://doi.org/10.1038/s41563-019-0576-0	journal	January 2020
A dynamic stability design strategy for lithium metal solid state batteries Ye, Luhan; Li, Xin Nature, Vol. 593, Issue 7858 https://doi.org/10.1038/s41586-021-03486-3	journal	May 2021
Fabrication of ultrathin solid electrolyte membranes of β-Li ₃ PS ₄ nanoflakes by evaporation-induced self-assembly for all-solid-state batteries Wang, Hui; Hood, Zachary D.; Xia, Younan Journal of Materials Chemistry A, Vol. 4, Issue 21 https://doi.org/10.1039/C6TA02294D	journal	January 2016
Three-dimensional bilayer garnet solid electrolyte based high energy density lithium metal–sulfur batteries Fu, Kun (Kelvin); Gong, Yunhui; Hitz, Gregory T. Energy & Environmental Science, Vol. 10, Issue 7 https://doi.org/10.1039/C7EE01004D	journal	January 2017
Fast synthesis of Li ₂ S–P ₂ S ₅ –LiI solid electrolyte precursors Phuc, Nguyen Huu Huy; Yamamoto, Tokoharu; Muto, Hiroyuki Inorganic Chemistry Frontiers, Vol. 4, Issue 10 https://doi.org/10.1039/C7QI00353F	journal	January 2017
Preparation of sulfide solid electrolytes in the Li ₂ S–P ₂ S ₅ system by a liquid phase process Calpa, Marcela; Rosero-Navarro, Nataly Carolina; Miura, Akira Inorganic Chemistry Frontiers, Vol. 5, Issue 2 https://doi.org/10.1039/C7QI00737J	journal	January 2018
Instantaneous preparation of high lithium-ion conducting sulfide solid electrolyte Li ₇ P ₃ S ₁₁ by a liquid phase process Calpa, Marcela; Rosero-Navarro, Nataly Carolina; Miura, Akira RSC Adv., Vol. 7, Issue 73 https://doi.org/10.1039/C7RA09081A	journal	January 2017
Designing solution chemistries for the low-temperature synthesis of sulfide-based solid electrolytes Lim, Hee-Dae; Yue, Xiujun; Xing, Xing Journal of Materials Chemistry A, Vol. 6, Issue 17 https://doi.org/10.1039/C8TA01800F	journal	January 2018
High-performance all-solid-state lithium–sulfur batteries with sulfur/carbon nano-hybrids in a composite cathode Zhang, Yibo; Liu, Ting; Zhang, Qinghua Journal of Materials Chemistry A, Vol. 6, Issue 46 https://doi.org/10.1039/C8TA08420C	journal	January 2018
Substitutional disorder: structure and ion dynamics of the argyrodites Li 6 PS 5 Cl, Li 6 PS 5 Br and Li 6 PS 5 I Hanghofer, I.; Brinek, M.; Eisbacher, S. L. Physical Chemistry Chemical Physics, Vol. 21, Issue 16 https://doi.org/10.1039/C9CP00664H	journal	January 2019
A quasi-solid-state Li–S battery with high energy density, superior stability and safety Cao, Yi; Zuo, Pengjian; Lou, Shuaifeng Journal of Materials Chemistry A, Vol. 7, Issue 11 https://doi.org/10.1039/C9TA00146H	journal	January 2019
A high performance all solid state lithium sulfur battery with lithium thiophosphate solid electrolyte Bonnick, Patrick; Niitani, Keita; Nose, Masafumi Journal of Materials Chemistry A, Vol. 7, Issue 42 https://doi.org/10.1039/C9TA06971B	journal	January 2019
Synthesis of sulfide solid electrolytes from Li₂S and P₂S₅ in anisole Maniwa, Riku; Calpa, Marcela; Rosero-Navarro, Nataly Carolina Journal of Materials Chemistry A, Vol. 9, Issue 1 https://doi.org/10.1039/D0TA08658D	journal	January 2021
The carrier transition from Li atoms to Li vacancies in solid-state lithium alloy anodes Lu, Yang; Zhao, Chen-Zi; Zhang, Rui Science Advances, Vol. 7, Issue 38 https://doi.org/10.1126/sciadv.abi5520	journal	September 2021
Application of Rod-Like Li ₆ PS ₅ Cl Directly Synthesized by a Liquid Phase Process to Sheet-Type Electrodes for All-Solid-State Lithium Batteries Choi, Sunho; Ann, Jiu; Do, Jiyae Journal of The Electrochemical Society, Vol. 166, Issue 3 https://doi.org/10.1149/2.0301903jes	journal	December 2018
All Solid-State Lithium–Sulfur Battery Using a Glass-Type P ₂ S ₅ –Li ₂ S Electrolyte: Benefits on Anode Kinetics Yamada, Takanobu; Ito, Seitaro; Omoda, Ryo Journal of The Electrochemical Society, Vol. 162, Issue 4 https://doi.org/10.1149/2.0441504jes	journal	January 2015

Similar Records

Incorporating Solvate and Solid Electrolytes for All‐Solid‐State Li ₂ S Batteries with High Capacity and Long Cycle Life

Journal Article · 2019 · Advanced Energy Materials · OSTI ID:1518512

Shin, Minjeong; Gewirth, Andrew A.

Electrochemical properties of all solid state Li/S battery

Journal Article · 2012 · Materials Research Bulletin · OSTI ID:22215504

Yu, Ji-Hyun; Park, Jin-Woo; Wang, Qing; +6 more

Development of bulk-type all-solid-state lithium-sulfur battery using LiBH{sub 4} electrolyte

Journal Article · 2014 · Applied Physics Letters · OSTI ID:22310992

Unemoto, Atsushi; Ikeshoji, Tamio; Yasaku, Syun; +5 more

Related Subjects

25 ENERGY STORAGE
36 MATERIALS SCIENCE
42 ENGINEERING
77 NANOSCIENCE AND NANOTECHNOLOGY
Li+ transport kinetics
Lithium-sulfur
all-solid-state batteries
batteries
energy storage
glass-ceramic solid electrolyte
high-sulfur-content cathodes
inorganic solid-state electrolytes
ion conduction pathways
low-density solid electrolyte
materials for energy and catalysis
polysulfide dissolution
sulfur-based positive electrode

Title: Realizing high-capacity all-solid-state lithium-sulfur batteries using a low-density inorganic solid-state electrolyte

Citation Formats

References (59)

Similar Records

Related Subjects