Nonflammable Lithium Metal Full Cells with Ultra-high Energy Density Based on Coordinated Carbonate Electrolytes

Cho, Sung-Ju; Yu, Dae-Eun; Pollard, Travis P.; Moon, Hyunseok; Jang, Minchul; Borodin, Oleg; Lee, Sang-Young

doi:10.1016/j.isci.2020.100844

Nonflammable Lithium Metal Full Cells with Ultra-high Energy Density Based on Coordinated Carbonate Electrolytes

Journal Article · Sat Feb 01 00:00:00 EST 2020 · iScience

DOI:https://doi.org/10.1016/j.isci.2020.100844· OSTI ID:1623688

Cho, Sung-Ju ^[1]; Yu, Dae-Eun ^[2]; Pollard, Travis P. ^[3]; Moon, Hyunseok ^[2]; Jang, Minchul ^[4]; Borodin, Oleg ^[3]; Lee, Sang-Young ^[2]

Ulsan National Institute of Science and Technology, Ulsan (Korea, Republic of). School of Energy and Chemical Engineering. Dept. of Energy Engineering; DOE/OSTI
Ulsan National Institute of Science and Technology, Ulsan (Korea, Republic of). School of Energy and Chemical Engineering. Dept. of Energy Engineering
Army Research Lab., Adelphi, MD (United States). Sensor and Electron Devices Directorate. Energy and Biomaterials Division. Battery Science Branch
LG Chem., Daejeon (Korea, Republic of). Battery R&D Center

Coupling thin Li metal anodes with high-capacity/high-voltage cathodes such as LiNi_0.8Co_0.1Mn_0.1O₂ (NCM811) is a promising way to increase lithium battery energy density. Yet, the realization of high-performance full cells remains a formidable challenge. Here, we demonstrate a new class of highly coordinated, nonflammable carbonate electrolytes based on lithium bis(fluorosulfonyl)imide (LiFSI) in propylene carbonate/fluoroethylene carbonate mixtures. Utilizing an optimal salt concentration (4 M LiFSI) of the electrolyte results in a unique coordination structure of Li⁺-FSI^--solvent cluster, which is critical for enabling the formation of stable interfaces on both the thin Li metal anode and high-voltage NCM811 cathode. Under highly demanding cell configuration and operating conditions (Li metal anode = 35 μm, areal capacity/charge voltage of NCM811 cathode = 4.8 mAh cm^-2/4.6 V, and anode excess capacity [relative to the cathode] = 0.83), the Li metal-based full cell provides exceptional electrochemical performance (energy densities = 679 Wh kg_cell^-1/1,024 Wh L_cell^-1) coupled with nonflammability.

View Accepted Manuscript (DOE)

Research Organization:: Army Research Lab., Adelphi, MD (United States). Sensor and Electron Devices Directorate. Energy and Biomaterials Division. Battery Science Branch

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE)

Grant/Contract Number:: AC36-08GO28308

OSTI ID:: 1623688

Journal Information:: iScience, Journal Name: iScience Journal Issue: 2 Vol. 23; ISSN 2589-0042

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

References (42)

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
The synergetic effect of lithium polysulfide and lithium nitrate to prevent lithium dendrite growth Li, Weiyang; Yao, Hongbin; Yan, Kai Nature Communications, Vol. 6, Issue 1 https://doi.org/10.1038/ncomms8436	journal	June 2015
Solubility-mediated sustained release enabling nitrate additive in carbonate electrolytes for stable lithium metal anode Liu, Yayuan; Lin, Dingchang; Li, Yuzhang Nature Communications, Vol. 9, Issue 1 https://doi.org/10.1038/s41467-018-06077-5	journal	September 2018
Polymer–inorganic solid–electrolyte interphase for stable lithium metal batteries under lean electrolyte conditions Gao, Yue; Yan, Zhifei; Gray, Jennifer L. Nature Materials, Vol. 18, Issue 4 https://doi.org/10.1038/s41563-019-0305-8	journal	March 2019
Less is more Salvatierra, Rodrigo V.; Tour, James M. Nature Nanotechnology, Vol. 14, Issue 6 https://doi.org/10.1038/s41565-019-0430-1	journal	April 2019
Fluorine-donating electrolytes enable highly reversible 5-V-class Li metal batteries Suo, Liumin; Xue, Weijiang; Gobet, Mallory Proceedings of the National Academy of Sciences, Vol. 115, Issue 6 https://doi.org/10.1073/pnas.1712895115	journal	January 2018
The development of lithium ion secondary batteries Nishi, Y. 1996 Symposium on VLSI Circuits. Digest of Technical Papers https://doi.org/10.1109/vlsic.1996.507725	conference	January 1996
High Rate and Stable Cycling of Lithium Metal Anode Qian, Jiangfeng; Henderson, Wesley A.; Xu, Wu ECS Meeting Abstracts, Vol. MA2015-01, Issue 15, p. 1155-1155 https://doi.org/10.1149/ma2015-01/15/1155	journal	April 2015
Conversion Cathodes: Lithium-Iron Fluoride Battery with In Situ Surface Protection (Adv. Funct. Mater. 10/2016) Gu, Wentian; Borodin, Oleg; Zdyrko, Bogdan Advanced Functional Materials, Vol. 26, Issue 10 https://doi.org/10.1002/adfm.201670060	journal	March 2016
Ultrafine Silver Nanoparticles for Seeded Lithium Deposition toward Stable Lithium Metal Anode Yang, Chunpeng; Yao, Yonggang; He, Shuaiming Advanced Materials, Vol. 29, Issue 38 https://doi.org/10.1002/adma.201702714	journal	August 2017
A Review of Solid Electrolyte Interphases on Lithium Metal Anode Cheng, Xin-Bing; Zhang, Rui; Zhao, Chen-Zi Advanced Science, Vol. 3, Issue 3 https://doi.org/10.1002/advs.201500213	journal	November 2015
Understanding the Degradation Mechanisms of LiNi _0.5 Co _0.2 Mn _0.3 O ₂ Cathode Material in Lithium Ion Batteries Jung, Sung-Kyun; Gwon, Hyeokjo; Hong, Jihyun Advanced Energy Materials, Vol. 4, Issue 1 https://doi.org/10.1002/aenm.201300787	journal	August 2013
Failure Mechanism for Fast-Charged Lithium Metal Batteries with Liquid Electrolytes Lu, Dongping; Shao, Yuyan; Lozano, Terence Advanced Energy Materials, Vol. 5, Issue 3 https://doi.org/10.1002/aenm.201400993	journal	September 2014
High Voltage Operation of Ni-Rich NMC Cathodes Enabled by Stable Electrode/Electrolyte Interphases Zhao, Wengao; Zheng, Jianming; Zou, Lianfeng Advanced Energy Materials, Vol. 8, Issue 19 https://doi.org/10.1002/aenm.201800297	journal	March 2018
Kinetic Stability of Bulk LiNiO ₂ and Surface Degradation by Oxygen Evolution in LiNiO ₂ -Based Cathode Materials Kong, Fantai; Liang, Chaoping; Wang, Luhua Advanced Energy Materials, Vol. 9, Issue 2 https://doi.org/10.1002/aenm.201802586	journal	November 2018
Lithiophilic Sites in Doped Graphene Guide Uniform Lithium Nucleation for Dendrite-Free Lithium Metal Anodes Zhang, Rui; Chen, Xiao-Ru; Chen, Xiang Angewandte Chemie International Edition, Vol. 56, Issue 27 https://doi.org/10.1002/anie.201702099	journal	May 2017
The development of lithium ion secondary batteries Nishi, Yoshio The Chemical Record, Vol. 1, Issue 5 https://doi.org/10.1002/tcr.1024	journal	January 2001
Lithium ion, lithium metal, and alternative rechargeable battery technologies: the odyssey for high energy density Placke, Tobias; Kloepsch, Richard; Dühnen, Simon Journal of Solid State Electrochemistry, Vol. 21, Issue 7 https://doi.org/10.1007/s10008-017-3610-7	journal	May 2017
Highly Fluorinated Interphases Enable High-Voltage Li-Metal Batteries Fan, Xiulin; Chen, Long; Ji, Xiao Chem, Vol. 4, Issue 1 https://doi.org/10.1016/j.chempr.2017.10.017	journal	January 2018
Behavior of Lithium Metal Anodes under Various Capacity Utilization and High Current Density in Lithium Metal Batteries Jiao, Shuhong; Zheng, Jianming; Li, Qiuyan Joule, Vol. 2, Issue 1 https://doi.org/10.1016/j.joule.2017.10.007	journal	January 2018
Enabling High-Voltage Lithium-Metal Batteries under Practical Conditions Ren, Xiaodi; Zou, Lianfeng; Cao, Xia Joule, Vol. 3, Issue 7 https://doi.org/10.1016/j.joule.2019.05.006	journal	July 2019
Li-ion batteries and portable power source prospects for the next 5–10 years Broussely, Michel; Archdale, Graham Journal of Power Sources, Vol. 136, Issue 2 https://doi.org/10.1016/j.jpowsour.2004.03.031	journal	October 2004
High-Performance Cells Containing Lithium Metal Anodes, LiNi _0.6 Co _0.2 Mn _0.2 O ₂ (NCM 622) Cathodes, and Fluoroethylene Carbonate-Based Electrolyte Solution with Practical Loading Salitra, Gregory; Markevich, Elena; Afri, Michal ACS Applied Materials & Interfaces, Vol. 10, Issue 23 https://doi.org/10.1021/acsami.8b07004	journal	May 2018
Very Stable Lithium Metal Stripping–Plating at a High Rate and High Areal Capacity in Fluoroethylene Carbonate-Based Organic Electrolyte Solution Markevich, Elena; Salitra, Gregory; Chesneau, Frederick ACS Energy Letters, Vol. 2, Issue 6 https://doi.org/10.1021/acsenergylett.7b00300	journal	May 2017
Correlating Li ⁺ Solvation Sheath Structure with Interphasial Chemistry on Graphite von Wald Cresce, Arthur; Borodin, Oleg; Xu, Kang The Journal of Physical Chemistry C, Vol. 116, Issue 50 https://doi.org/10.1021/jp303610t	journal	December 2012
On Electrolyte-Dependent Formation of Solid Electrolyte Interphase Film in Lithium-Ion Batteries: Strong Sensitivity to Small Structural Difference of Electrolyte Molecules Takenaka, Norio; Suzuki, Yuichi; Sakai, Hirofumi The Journal of Physical Chemistry C, Vol. 118, Issue 20 https://doi.org/10.1021/jp5018696	journal	May 2014
Insight into the Atomic Structure of Cycled Lithium-Rich Layered Oxide Li _1.20 Mn _0.54 Co _0.13 Ni _0.13 O ₂ Using HAADF STEM and Electron Nanodiffraction Genevois, Cécile; Koga, Hideyuki; Croguennec, Laurence The Journal of Physical Chemistry C, Vol. 119, Issue 1 https://doi.org/10.1021/jp509388j	journal	December 2014
A stable lithium-rich surface structure for lithium-rich layered cathode materials Kim, Sangryun; Cho, Woosuk; Zhang, Xiaobin Nature Communications, Vol. 7, Issue 1 https://doi.org/10.1038/ncomms13598	journal	November 2016
High rate and stable cycling of lithium metal anode Qian, Jiangfeng; Henderson, Wesley A.; Xu, Wu Nature Communications, Vol. 6, Issue 1 https://doi.org/10.1038/ncomms7362	journal	February 2015
Electrolyte additive enabled fast charging and stable cycling lithium metal batteries Zheng, Jianming; Engelhard, Mark H.; Mei, Donghai Nature Energy, Vol. 2, Issue 3 https://doi.org/10.1038/nenergy.2017.12	journal	March 2017
Reviving the lithium metal anode for high-energy batteries Lin, Dingchang; Liu, Yayuan; Cui, Yi Nature Nanotechnology, Vol. 12, Issue 3 https://doi.org/10.1038/nnano.2017.16	journal	March 2017
Status and challenges in enabling the lithium metal electrode for high-energy and low-cost rechargeable batteries Albertus, Paul; Babinec, Susan; Litzelman, Scott Nature Energy, Vol. 3, Issue 1 https://doi.org/10.1038/s41560-017-0047-2	journal	December 2017
Stable cycling of high-voltage lithium metal batteries in ether electrolytes Jiao, Shuhong; Ren, Xiaodi; Cao, Ruiguo Nature Energy, Vol. 3, Issue 9 https://doi.org/10.1038/s41560-018-0199-8	journal	July 2018
Langmuir–Blodgett artificial solid-electrolyte interphases for practical lithium metal batteries Kim, Mun Sek; Ryu, Ji-Hyun Nature Energy, Vol. 3, Issue 10 https://doi.org/10.1038/s41560-018-0237-6	journal	September 2018
Pathways for practical high-energy long-cycling lithium metal batteries Liu, Jun; Bao, Zhenan; Cui, Yi Nature Energy, Vol. 4, Issue 3 https://doi.org/10.1038/s41560-019-0338-x	journal	February 2019
Non-flammable electrolyte enables Li-metal batteries with aggressive cathode chemistries Fan, Xiulin; Chen, Long; Borodin, Oleg Nature Nanotechnology, Vol. 13, Issue 8 https://doi.org/10.1038/s41565-018-0183-2	journal	July 2018
Self-smoothing anode for achieving high-energy lithium metal batteries under realistic conditions Niu, Chaojiang; Pan, Huilin; Xu, Wu Nature Nanotechnology, Vol. 14, Issue 6 https://doi.org/10.1038/s41565-019-0427-9	journal	April 2019
Bisalt ether electrolytes: a pathway towards lithium metal batteries with Ni-rich cathodes Alvarado, Judith; Schroeder, Marshall A.; Pollard, Travis P. Energy & Environmental Science, Vol. 12, Issue 2 https://doi.org/10.1039/C8EE02601G	journal	January 2019
Materials for lithium-ion battery safety Liu, Kai; Liu, Yayuan; Lin, Dingchang Science Advances, Vol. 4, Issue 6 https://doi.org/10.1126/sciadv.aas9820	journal	June 2018
Advanced Model for Solid Electrolyte Interphase Electrodes in Liquid and Polymer Electrolytes Peled, E. Journal of The Electrochemical Society, Vol. 144, Issue 8 https://doi.org/10.1149/1.1837858	journal	January 1997
A Safe Electrolyte Based on Propylene Carbonate and Non-Flammable Hydrofluoroether for High-Performance Lithium Ion Batteries Shi, Pei; Fang, Shaohua; Luo, Dong Journal of The Electrochemical Society, Vol. 164, Issue 9 https://doi.org/10.1149/2.1181709jes	journal	January 2017
Electrolyte Solvation and Ionic Association Seo, Daniel M.; Borodin, Oleg; Han, Sang-Don Journal of The Electrochemical Society, Vol. 159, Issue 5 https://doi.org/10.1149/2.jes112264	journal	January 2012

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