High areal capacity, long cycle life 4 V ceramic all-solid-state Li-ion batteries enabled by chloride solid electrolytes
Abstract
All-solid-state Li batteries (ASSBs) employing inorganic solid electrolytes offer improved safety and are exciting candidates for next-generation energy storage. Herein, we report a family of lithium mixed-metal chlorospinels, Li2InxSc0.666-xCl4 (0 ≤ x ≤ 0.666), with high ionic conductivity (up to 2.0 mS cm-1) owing to a highly disordered Li-ion distribution, and low electronic conductivity (4.7 × 10-10 S cm-1), which are implemented for high-performance ASSBs. Owing to the excellent interfacial stability of the SE against uncoated high-voltage cathode materials, ASSBs utilizing LiCoO2 or LiNi0.85Co0.1Mn0.05O2 exhibit superior rate capability and long-term cycling (up to 4.8 V versus Li+/Li) compared to state-of-the-art ASSBs. In particular, the ASSB with LiNi0.85Co0.1Mn0.05O2 exhibits a long life of >3,000 cycles with 80% capacity retention at room temperature. Additionally, high cathode loadings are also demonstrated in ASSBs with stable capacity retention of >4 mAh cm-2 (~190 mAh g-1).
- Authors:
-
- Univ. of Waterloo, ON (Canada). Waterloo Inst. for Nanotechnology; Argonne National Lab. (ANL), Argonne, IL (United States). Joint Center for Energy Storage Research (JCESR)
- Justus Liebig Univ., Giessen (Germany)
- Univ. of Waterloo, ON (Canada). Waterloo Inst. for Nanotechnology
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Publication Date:
- Research Org.:
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1869086
- Grant/Contract Number:
- AC05-00OR22725
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Energy
- Additional Journal Information:
- Journal Volume: 7; Journal Issue: 1; Journal ID: ISSN 2058-7546
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE; batteries; electronic properties and materials
Citation Formats
Zhou, Laidong, Zuo, Tong-Tong, Kwok, Chun Yuen, Kim, Se Young, Assoud, Abdeljalil, Zhang, Qiang, Janek, Jürgen, and Nazar, Linda F. High areal capacity, long cycle life 4 V ceramic all-solid-state Li-ion batteries enabled by chloride solid electrolytes. United States: N. p., 2022.
Web. doi:10.1038/s41560-021-00952-0.
Zhou, Laidong, Zuo, Tong-Tong, Kwok, Chun Yuen, Kim, Se Young, Assoud, Abdeljalil, Zhang, Qiang, Janek, Jürgen, & Nazar, Linda F. High areal capacity, long cycle life 4 V ceramic all-solid-state Li-ion batteries enabled by chloride solid electrolytes. United States. https://doi.org/10.1038/s41560-021-00952-0
Zhou, Laidong, Zuo, Tong-Tong, Kwok, Chun Yuen, Kim, Se Young, Assoud, Abdeljalil, Zhang, Qiang, Janek, Jürgen, and Nazar, Linda F. Mon .
"High areal capacity, long cycle life 4 V ceramic all-solid-state Li-ion batteries enabled by chloride solid electrolytes". United States. https://doi.org/10.1038/s41560-021-00952-0. https://www.osti.gov/servlets/purl/1869086.
@article{osti_1869086,
title = {High areal capacity, long cycle life 4 V ceramic all-solid-state Li-ion batteries enabled by chloride solid electrolytes},
author = {Zhou, Laidong and Zuo, Tong-Tong and Kwok, Chun Yuen and Kim, Se Young and Assoud, Abdeljalil and Zhang, Qiang and Janek, Jürgen and Nazar, Linda F.},
abstractNote = {All-solid-state Li batteries (ASSBs) employing inorganic solid electrolytes offer improved safety and are exciting candidates for next-generation energy storage. Herein, we report a family of lithium mixed-metal chlorospinels, Li2InxSc0.666-xCl4 (0 ≤ x ≤ 0.666), with high ionic conductivity (up to 2.0 mS cm-1) owing to a highly disordered Li-ion distribution, and low electronic conductivity (4.7 × 10-10 S cm-1), which are implemented for high-performance ASSBs. Owing to the excellent interfacial stability of the SE against uncoated high-voltage cathode materials, ASSBs utilizing LiCoO2 or LiNi0.85Co0.1Mn0.05O2 exhibit superior rate capability and long-term cycling (up to 4.8 V versus Li+/Li) compared to state-of-the-art ASSBs. In particular, the ASSB with LiNi0.85Co0.1Mn0.05O2 exhibits a long life of >3,000 cycles with 80% capacity retention at room temperature. Additionally, high cathode loadings are also demonstrated in ASSBs with stable capacity retention of >4 mAh cm-2 (~190 mAh g-1).},
doi = {10.1038/s41560-021-00952-0},
journal = {Nature Energy},
number = 1,
volume = 7,
place = {United States},
year = {Mon Jan 03 00:00:00 EST 2022},
month = {Mon Jan 03 00:00:00 EST 2022}
}
Works referenced in this record:
High-Voltage Superionic Halide Solid Electrolytes for All-Solid-State Li-Ion Batteries
journal, January 2020
- Park, Kern-Ho; Kaup, Kavish; Assoud, Abdeljalil
- ACS Energy Letters, Vol. 5, Issue 2
Energy storage emerging: A perspective from the Joint Center for Energy Storage Research
journal, June 2020
- Trahey, Lynn; Brushett, Fikile R.; Balsara, Nitash P.
- Proceedings of the National Academy of Sciences, Vol. 117, Issue 23
High-Throughput Screening of Solid-State Li-Ion Conductors Using Lattice-Dynamics Descriptors
journal, June 2019
- Muy, Sokseiha; Voss, Johannes; Schlem, Roman
- iScience, Vol. 16
Heat treatment protocol for modulating ionic conductivity via structural evolution of Li3-xYb1-xMxCl6 (M = Hf4+, Zr4+) new halide superionic conductors for all-solid-state batteries
journal, December 2021
- Park, Juhyoun; Han, Daseul; Kwak, Hiram
- Chemical Engineering Journal, Vol. 425
Elucidating the Limit of Li Insertion into the Spinel Li 4 Ti 5 O 12
journal, May 2019
- Liu, Haodong; Zhu, Zhuoying; Huang, Jason
- ACS Materials Letters, Vol. 1, Issue 1
New horizons for inorganic solid state ion conductors
journal, January 2018
- Zhang, Zhizhen; Shao, Yuanjun; Lotsch, Bettina
- Energy & Environmental Science, Vol. 11, Issue 8
A new halospinel superionic conductor for high-voltage all solid state lithium batteries
journal, January 2020
- Zhou, Laidong; Kwok, Chun Yuen; Shyamsunder, Abhinandan
- Energy & Environmental Science, Vol. 13, Issue 7
Origin of Outstanding Stability in the Lithium Solid Electrolyte Materials: Insights from Thermodynamic Analyses Based on First-Principles Calculations
journal, October 2015
- Zhu, Yizhou; He, Xingfeng; Mo, Yifei
- ACS Applied Materials & Interfaces, Vol. 7, Issue 42
Design Strategies, Practical Considerations, and New Solution Processes of Sulfide Solid Electrolytes for All-Solid-State Batteries
journal, April 2018
- Park, Kern Ho; Bai, Qiang; Kim, Dong Hyeon
- Advanced Energy Materials, Vol. 8, Issue 18
A lithium superionic conductor
journal, July 2011
- Kamaya, Noriaki; Homma, Kenji; Yamakawa, Yuichiro
- Nature Materials, Vol. 10, Issue 9, p. 682-686
The Working Principle of a Li 2 CO 3 /LiNbO 3 Coating on NCM for Thiophosphate-Based All-Solid-State Batteries
journal, March 2021
- Walther, Felix; Strauss, Florian; Wu, Xiaohan
- Chemistry of Materials, Vol. 33, Issue 6
Air-stable Li 3 InCl 6 electrolyte with high voltage compatibility for all-solid-state batteries
journal, January 2019
- Li, Xiaona; Liang, Jianwen; Luo, Jing
- Energy & Environmental Science, Vol. 12, Issue 9
Clarifying the relationship between redox activity and electrochemical stability in solid electrolytes
journal, January 2020
- Schwietert, Tammo K.; Arszelewska, Violetta A.; Wang, Chao
- Nature Materials, Vol. 19, Issue 4
High-power all-solid-state batteries using sulfide superionic conductors
journal, March 2016
- Kato, Yuki; Hori, Satoshi; Saito, Toshiya
- Nature Energy, Vol. 1, Issue 4
Single‐ or Poly‐Crystalline Ni‐Rich Layered Cathode, Sulfide or Halide Solid Electrolyte: Which Will be the Winners for All‐Solid‐State Batteries?
journal, April 2021
- Han, Yoonjae; Jung, Sung Hoo; Kwak, Hiram
- Advanced Energy Materials, Vol. 11, Issue 21
Interfaces and Interphases in All-Solid-State Batteries with Inorganic Solid Electrolytes
journal, June 2020
- Banerjee, Abhik; Wang, Xuefeng; Fang, Chengcheng
- Chemical Reviews, Vol. 120, Issue 14
Li 3 BO 3 –Li 2 CO 3 : Rationally Designed Buffering Phase for Sulfide All-Solid-State Li-Ion Batteries
journal, October 2018
- Jung, Sung Hoo; Oh, Kyungbae; Nam, Young Jin
- Chemistry of Materials, Vol. 30, Issue 22
Impact of Cathode Material Particle Size on the Capacity of Bulk-Type All-Solid-State Batteries
journal, March 2018
- Strauss, Florian; Bartsch, Timo; de Biasi, Lea
- ACS Energy Letters, Vol. 3, Issue 4
Tern�re Halogenide vom Typ A3MX6. VI [1]. Tern�re Chloride der Selten-Erd-Elemente mit Lithium, Li3MCl6 (M ? Tb?Lu, Y, Sc): Synthese, Kristallstrukturen und Ionenbewegung
journal, July 1997
- Bohnsack, Andreas; Stenzel, Frauke; Zajonc, Armin
- Zeitschrift f�r anorganische und allgemeine Chemie, Vol. 623, Issue 7
Interphase Engineering Enabled All-Ceramic Lithium Battery
journal, March 2018
- Han, Fudong; Yue, Jie; Chen, Cheng
- Joule, Vol. 2, Issue 3
Lithium Ytterbium-Based Halide Solid Electrolytes for High Voltage All-Solid-State Batteries
journal, June 2021
- Kim, Se Young; Kaup, Kavish; Park, Kern-Ho
- ACS Materials Letters, Vol. 3, Issue 7
New Family of Argyrodite Thioantimonate Lithium Superionic Conductors
journal, October 2019
- Zhou, Laidong; Assoud, Abdeljalil; Zhang, Qiang
- Journal of the American Chemical Society, Vol. 141, Issue 48
All-Solid-State Batteries with Thick Electrode Configurations
journal, January 2018
- Kato, Yuki; Shiotani, Shinya; Morita, Keisuke
- The Journal of Physical Chemistry Letters, Vol. 9, Issue 3
High-energy long-cycling all-solid-state lithium metal batteries enabled by silver–carbon composite anodes
journal, March 2020
- Lee, Yong-Gun; Fujiki, Satoshi; Jung, Changhoon
- Nature Energy, Vol. 5, Issue 4
Guidelines for All-Solid-State Battery Design and Electrode Buffer Layers Based on Chemical Potential Profile Calculation
journal, May 2019
- Nakamura, Takashi; Amezawa, Koji; Kulisch, Jörn
- ACS Applied Materials & Interfaces, Vol. 11, Issue 22
Solid-State Chemistries Stable with High-Energy Cathodes for Lithium-Ion Batteries
journal, September 2019
- Nolan, Adelaide M.; Liu, Yunsheng; Mo, Yifei
- ACS Energy Letters, Vol. 4, Issue 10
Visualization of the Interfacial Decomposition of Composite Cathodes in Argyrodite-Based All-Solid-State Batteries Using Time-of-Flight Secondary-Ion Mass Spectrometry
journal, April 2019
- Walther, Felix; Koerver, Raimund; Fuchs, Till
- Chemistry of Materials, Vol. 31, Issue 10
Benchmarking the performance of all-solid-state lithium batteries
journal, March 2020
- Randau, Simon; Weber, Dominik A.; Kötz, Olaf
- Nature Energy, Vol. 5, Issue 3
Characterization of Electronic and Ionic Transport in Li 1- x Ni 0.33 Mn 0.33 Co 0.33 O 2 (NMC 333 ) and Li 1- x Ni 0.50 Mn 0.20 Co 0.30 O 2 (NMC 523 ) as a Function of Li Content
journal, January 2016
- Amin, Ruhul; Chiang, Yet-Ming
- Journal of The Electrochemical Society, Vol. 163, Issue 8
Ionic conductivity of quenched alkali niobate and tantalate glasses
journal, September 1978
- Glass, A. M.; Nassau, K.; Negran, T. J.
- Journal of Applied Physics, Vol. 49, Issue 9
Approaching Practically Accessible Solid-State Batteries: Stability Issues Related to Solid Electrolytes and Interfaces
journal, November 2019
- Chen, Rusong; Li, Qinghao; Yu, Xiqian
- Chemical Reviews, Vol. 120, Issue 14
Processing thin but robust electrolytes for solid-state batteries
journal, February 2021
- Balaish, Moran; Gonzalez-Rosillo, Juan Carlos; Kim, Kun Joong
- Nature Energy, Vol. 6, Issue 3
Kinetic pathways of ionic transport in fast-charging lithium titanate
journal, February 2020
- Zhang, Wei; Seo, Dong-Hwa; Chen, Tina
- Science, Vol. 367, Issue 6481
Solid Halide Electrolytes with High Lithium-Ion Conductivity for Application in 4 V Class Bulk-Type All-Solid-State Batteries
journal, September 2018
- Asano, Tetsuya; Sakai, Akihiro; Ouchi, Satoru
- Advanced Materials, Vol. 30, Issue 44
Ultra-high-voltage Ni-rich layered cathodes in practical Li metal batteries enabled by a sulfonamide-based electrolyte
journal, March 2021
- Xue, Weijiang; Huang, Mingjun; Li, Yutao
- Nature Energy, Vol. 6, Issue 5
High Active Material Loading in All‐Solid‐State Battery Electrode via Particle Size Optimization
journal, November 2019
- Shi, Tan; Tu, Qingsong; Tian, Yaosen
- Advanced Energy Materials, Vol. 10, Issue 1
LiNbO3-coated LiCoO2 as cathode material for all solid-state lithium secondary batteries
journal, July 2007
- Ohta, Narumi; Takada, Kazunori; Sakaguchi, Isao
- Electrochemistry Communications, Vol. 9, Issue 7
Experimental Assessment of the Practical Oxidative Stability of Lithium Thiophosphate Solid Electrolytes
journal, September 2019
- Dewald, Georg F.; Ohno, Saneyuki; Kraft, Marvin A.
- Chemistry of Materials, Vol. 31, Issue 20
Site-Occupation-Tuned Superionic Li x ScCl 3+ x Halide Solid Electrolytes for All-Solid-State Batteries
journal, March 2020
- Liang, Jianwen; Li, Xiaona; Wang, Shuo
- Journal of the American Chemical Society, Vol. 142, Issue 15
Evolution of Structure and Lithium Dynamics in LiNi 0.8 Mn 0.1 Co 0.1 O 2 (NMC811) Cathodes during Electrochemical Cycling
journal, March 2019
- Märker, Katharina; Reeves, Philip J.; Xu, Chao
- Chemistry of Materials, Vol. 31, Issue 7
Direct Visualization of the Interfacial Degradation of Cathode Coatings in Solid State Batteries: A Combined Experimental and Computational Study
journal, June 2020
- Zhang, Ya‐Qian; Tian, Yaosen; Xiao, Yihan
- Advanced Energy Materials, Vol. 10, Issue 27
Chemo-mechanical expansion of lithium electrode materials – on the route to mechanically optimized all-solid-state batteries
journal, January 2018
- Koerver, Raimund; Zhang, Wenbo; de Biasi, Lea
- Energy & Environmental Science, Vol. 11, Issue 8
Lithium Chlorides and Bromides as Promising Solid‐State Chemistries for Fast Ion Conductors with Good Electrochemical Stability
journal, June 2019
- Wang, Shuo; Bai, Qiang; Nolan, Adelaide M.
- Angewandte Chemie International Edition, Vol. 58, Issue 24
Computational Screening of Cathode Coatings for Solid-State Batteries
journal, May 2019
- Xiao, Yihan; Miara, Lincoln J.; Wang, Yan
- Joule, Vol. 3, Issue 5
Editors’ Choice—Quantifying the Impact of Charge Transport Bottlenecks in Composite Cathodes of All-Solid-State Batteries
journal, April 2021
- Minnmann, Philip; Quillman, Lars; Burkhardt, Simon
- Journal of The Electrochemical Society, Vol. 168, Issue 4
New Cost‐Effective Halide Solid Electrolytes for All‐Solid‐State Batteries: Mechanochemically Prepared Fe 3+ ‐Substituted Li 2 ZrCl 6
journal, January 2021
- Kwak, Hiram; Han, Daseul; Lyoo, Jeyne
- Advanced Energy Materials, Vol. 11, Issue 12
Effect of composite electrode thickness on the electrochemical performances of all-solid-state li-ion batteries
journal, April 2017
- Kubanska, Agnieszka; Castro, Laurent; Tortet, Laurence
- Journal of Electroceramics, Vol. 38, Issue 2-4
Inorganic Solid-State Electrolytes for Lithium Batteries: Mechanisms and Properties Governing Ion Conduction
journal, December 2015
- Bachman, John Christopher; Muy, Sokseiha; Grimaud, Alexis
- Chemical Reviews, Vol. 116, Issue 1
Li 2 ZrO 3 -Coated NCM622 for Application in Inorganic Solid-State Batteries: Role of Surface Carbonates in the Cycling Performance
journal, December 2020
- Strauss, Florian; Teo, Jun Hao; Maibach, Julia
- ACS Applied Materials & Interfaces, Vol. 12, Issue 51
Revealing Nanoscale Solid–Solid Interfacial Phenomena for Long-Life and High-Energy All-Solid-State Batteries
journal, October 2019
- Banerjee, Abhik; Tang, Hanmei; Wang, Xuefeng
- ACS Applied Materials & Interfaces, Vol. 11, Issue 46