Rational Electrolyte Design for Elevated-Temperature and Thermally Stable Lithium-Ion Batteries with Nickel-Rich Cathodes

Jia, Hao; Broekhuis, Benjamin; Xu, Yaobin; Yang, Zhijie; Kautz, David; Zhong, Lirong; Engelhard, Mark H.; Zhao, Qian; Bowden, Mark E.; Matthews, Bethany E.; Connor, Callum; Lin, Feng; Wang, Chongmin; Xu, Wu

doi:10.1021/acsami.4c17629

Title: Rational Electrolyte Design for Elevated-Temperature and Thermally Stable Lithium-Ion Batteries with Nickel-Rich Cathodes

Journal Article · 14 January 2025 · ACS Applied Materials and Interfaces

DOI: https://doi.org/10.1021/acsami.4c17629 · OSTI ID:2507217

Jia, Hao ^[1]; Broekhuis, Benjamin ^[2];

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^[4]; Kautz, David ^[1];

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Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); Univ. of Texas, Austin, TX (United States)
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States). Environmental Molecular Sciences Laboratory (EMSL)
Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)

As the energy density of lithium-ion batteries (LIBs) increases, the shortened cycle life and the increased safety hazard of LIBs are drawing increasing concerns. To address such challenges, a series of localized high-concentration electrolytes (LHCEs) based on a solvating-solvent mixture of tetramethylene sulfone and trimethyl phosphate and a high flash-point diluent 1H,1H,5H-octafluoropentyl 1,1,2,2-tetrafluoroethyl ether were designed. The LHCEs exhibited non-flammability and greatly suppressed heat release at high temperatures, which would potentially improve the safety performance of the LIBs. Moreover, the optimal LHCE achieved capacity retentions of 87.1% and 81.7% in graphite||LiNi_0.8Mn_0.1Co_0.1O₂ cells after 500 cycles at 25 °C and 45 °C, respectively, which were significantly better than the conventional electrolyte, whose capacity retentions were only 75.2% and 38.5% under the same condition. Mechanistic studies revealed that the LHCE not only formed a more robust solid electrolyte interphase, but also exhibited improved anodic stability, compared with the conventional electrolyte. Further, this work sheds light in rational electrolyte design for high energy density LIBs with high battery performance and low safety concerns.

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Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States). Environmental Molecular Sciences Laboratory (EMSL)

Sponsoring Organization:: USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE Office of Science (SC), Biological and Environmental Research (BER); USDOE Office of Science (SC), Office of Workforce Development for Teachers & Scientists (WDTS)

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 2507217

Report Number(s):: PNNL-SA--202615

Journal Information:: ACS Applied Materials and Interfaces, Journal Name: ACS Applied Materials and Interfaces Journal Issue: 4 Vol. 17; ISSN 1944-8244

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

References (31)

The Current Move of Lithium Ion Batteries Towards the Next Phase Kim, Tae-Hee; Park, Jeong-Seok; Chang, Sung Kyun Advanced Energy Materials, Vol. 2, Issue 7 https://doi.org/10.1002/aenm.201200028	journal	May 2012
Prospect and Reality of Ni-Rich Cathode for Commercialization Kim, Junhyeok; Lee, Hyomyung; Cha, Hyungyeon Advanced Energy Materials, Vol. 8, Issue 6 https://doi.org/10.1002/aenm.201702028	journal	November 2017
High‐Fluorinated Electrolytes for Li–S Batteries Zheng, Jing; Ji, Guangbin; Fan, Xiulin Advanced Energy Materials, Vol. 9, Issue 16 https://doi.org/10.1002/aenm.201803774	journal	February 2019
Advanced Electrolytes for Fast‐Charging High‐Voltage Lithium‐Ion Batteries in Wide‐Temperature Range Zhang, Xianhui; Zou, Lianfeng; Xu, Yaobin Advanced Energy Materials, Vol. 10, Issue 22 https://doi.org/10.1002/aenm.202000368	journal	April 2020
Li₂CO₃/LiF‐Rich Heterostructured Solid Electrolyte Interphase with Superior Lithiophilic and Li⁺‐Transferred Characteristics via Adjusting Electrolyte Additives Wu, Daxiong; He, Jian; Liu, Jiandong Advanced Energy Materials, Vol. 12, Issue 18 https://doi.org/10.1002/aenm.202200337	journal	March 2022
Is Nonflammability of Electrolyte Overrated in the Overall Safety Performance of Lithium Ion Batteries? A Sobering Revelation from a Completely Nonflammable Electrolyte Jia, Hao; Yang, Zhijie; Xu, Yaobin Advanced Energy Materials, Vol. 13, Issue 4 https://doi.org/10.1002/aenm.202203144	journal	December 2022
Fluorinating the Solid Electrolyte Interphase by Rational Molecular Design for Practical Lithium‐Metal Batteries Xie, Jin; Sun, Shu‐Yu; Chen, Xiang Angewandte Chemie, Vol. 134, Issue 29 https://doi.org/10.1002/ange.202204776	journal	June 2022
A Systematic Study on the Effects of Solvating Solvents and Additives in Localized High‐Concentration Electrolytes over Electrochemical Performance of Lithium‐Ion Batteries Jia, Hao; Kim, Ju‐Myung; Gao, Peiyuan Angewandte Chemie, Vol. 135, Issue 17 https://doi.org/10.1002/ange.202218005	journal	March 2023
Advanced Low‐Flammable Electrolytes for Stable Operation of High‐Voltage Lithium‐Ion Batteries Jia, Hao; Xu, Yaobin; Zhang, Xianhui Angewandte Chemie International Edition, Vol. 60, Issue 23 https://doi.org/10.1002/anie.202102403	journal	April 2021
Localized High‐Concentration Electrolytes with Low‐Cost Diluents Compatible with Both Cobalt‐Free LiNiO₂ Cathode and Lithium‐Metal Anode Guo, Zezhou; Cui, Zehao; Sim, Richard Small, Vol. 19, Issue 49 https://doi.org/10.1002/smll.202305055	journal	August 2023
Flame-retardant additives for lithium-ion batteries Hyung, Yoo E.; Vissers, Donald R.; Amine, Khalil Journal of Power Sources, Vol. 119-121 https://doi.org/10.1016/S0378-7753(03)00225-8	journal	June 2003
Sulfone-based high-voltage electrolytes for high energy density rechargeable lithium batteries: Progress and perspective Wu, Wenya; Bai, Ying; Wang, Xinran Chinese Chemical Letters, Vol. 32, Issue 4 https://doi.org/10.1016/j.cclet.2020.10.009	journal	April 2021
A localized high-concentration electrolyte with lithium bis(fluorosulfonyl) imide (LiFSI) salt and F-containing cosolvents to enhance the performance of Li\|\|LiNi0.8Co0.1Mn0.1O2 lithium metal batteries Huangzhang, Encheng; Zeng, Xueyi; Yang, Tianxiang Chemical Engineering Journal, Vol. 439 https://doi.org/10.1016/j.cej.2022.135534	journal	July 2022
Localized High-Concentration Sulfone Electrolytes for High-Efficiency Lithium-Metal Batteries Ren, Xiaodi; Chen, Shuru; Lee, Hongkyung Chem, Vol. 4, Issue 8 https://doi.org/10.1016/j.chempr.2018.05.002	journal	August 2018
LiFSI vs. LiPF6 electrolytes in contact with lithiated graphite: Comparing thermal stabilities and identification of specific SEI-reinforcing additives Eshetu, Gebrekidan Gebresilassie; Grugeon, Sylvie; Gachot, Grégory Electrochimica Acta, Vol. 102 https://doi.org/10.1016/j.electacta.2013.03.171	journal	July 2013
The Electrolyte Frontier: A Manifesto Amanchukwu, Chibueze V. Joule, Vol. 4, Issue 2 https://doi.org/10.1016/j.joule.2019.12.009	journal	February 2020
Electric Vehicles Batteries: Requirements and Challenges Deng, Jie; Bae, Chulheung; Denlinger, Adam Joule, Vol. 4, Issue 3 https://doi.org/10.1016/j.joule.2020.01.013	journal	March 2020
Comparative study of trimethyl phosphite and trimethyl phosphate as electrolyte additives in lithium ion batteries Yao, X. L.; Xie, S.; Chen, C. H. Journal of Power Sources, Vol. 144, Issue 1 https://doi.org/10.1016/j.jpowsour.2004.11.042	journal	June 2005
Sulfone-based electrolytes for high energy density lithium-ion batteries Jia, Hao; Xu, Yaobin; Zou, Lianfeng Journal of Power Sources, Vol. 527 https://doi.org/10.1016/j.jpowsour.2022.231171	journal	April 2022
Fluoroethylene Carbonate and Vinylene Carbonate Reduction: Understanding Lithium-Ion Battery Electrolyte Additives and Solid Electrolyte Interphase Formation Michan, Alison L.; Parimalam, Bharathy. S.; Leskes, Michal Chemistry of Materials, Vol. 28, Issue 22 https://doi.org/10.1021/acs.chemmater.6b02282	journal	November 2016
LiPF ₆ Stabilizer and Transition-Metal Cation Scavenger: A Bifunctional Bipyridine-Based Ligand for Lithium-Ion Battery Application Jia, Hao; Billmann, Bastian; Onishi, Hitoshi Chemistry of Materials, Vol. 31, Issue 11 https://doi.org/10.1021/acs.chemmater.9b00555	journal	May 2019
In Situ Interfacial Tuning To Obtain High-Performance Nickel-Rich Cathodes in Lithium Metal Batteries Ma, Hyunsoo; Hwang, Daeyeon; Ahn, Young Jun ACS Applied Materials & Interfaces https://doi.org/10.1021/acsami.0c06830	journal	June 2020
Beyond Doping and Coating: Prospective Strategies for Stable High-Capacity Layered Ni-Rich Cathodes Sun, H. Hohyun; Ryu, Hoon-Hee; Kim, Un-Hyuck ACS Energy Letters, Vol. 5, Issue 4 https://doi.org/10.1021/acsenergylett.0c00191	journal	March 2020
Nonaqueous Liquid Electrolytes for Lithium-Based Rechargeable Batteries Xu, Kang Chemical Reviews, Vol. 104, Issue 10, p. 4303-4418 https://doi.org/10.1021/cr030203g	journal	October 2004
High lithium oxide prevalence in the lithium solid–electrolyte interphase for high Coulombic efficiency Hobold, Gustavo M.; Wang, Chongzhen; Steinberg, Katherine Nature Energy https://doi.org/10.1038/s41560-024-01494-x	journal	April 2024
Mechanism of cycling degradation and strategy to stabilize a nickel-rich cathode Yang, Xuerui; Chen, Jiawei; Zheng, Qinfeng Journal of Materials Chemistry A, Vol. 6, Issue 33 https://doi.org/10.1039/C8TA03041C	journal	January 2018
Revealing electrolyte oxidation via carbonate dehydrogenation on Ni-based oxides in Li-ion batteries by in situ Fourier transform infrared spectroscopy Zhang, Yirui; Katayama, Yu; Tatara, Ryoichi Energy & Environmental Science, Vol. 13, Issue 1 https://doi.org/10.1039/C9EE02543J	journal	January 2020
Nonflammable Trimethyl Phosphate Solvent-Containing Electrolytes for Lithium-Ion Batteries: I. Fundamental Properties Wang, Xianming; Yasukawa, Eiki; Kasuya, Shigeaki Journal of The Electrochemical Society, Vol. 148, Issue 10 https://doi.org/10.1149/1.1397773	journal	January 2001
Nonflammable Trimethyl Phosphate Solvent-Containing Electrolytes for Lithium-Ion Batteries: II. The Use of an Amorphous Carbon Anode Wang, Xianming; Yasukawa, Eiki; Kasuya, Shigeaki Journal of The Electrochemical Society, Vol. 148, Issue 10 https://doi.org/10.1149/1.1397774	journal	January 2001
Review—Localized High-Concentration Electrolytes for Lithium Batteries Cao, Xia; Jia, Hao; Xu, Wu Journal of The Electrochemical Society, Vol. 168, Issue 1 https://doi.org/10.1149/1945-7111/abd60e	journal	January 2021
Flammability of Li-Ion Battery Electrolytes: Flash Point and Self-Extinguishing Time Measurements Hess, Steffen; Wohlfahrt-Mehrens, Margret; Wachtler, Mario Journal of The Electrochemical Society, Vol. 162, Issue 2 https://doi.org/10.1149/2.0121502jes	journal	January 2015

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Title: Rational Electrolyte Design for Elevated-Temperature and Thermally Stable Lithium-Ion Batteries with Nickel-Rich Cathodes

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