Effects of Applied Interfacial Pressure on Li-Metal Cycling Performance and Morphology in 4 M LiFSI in DME

Harrison, Katharine L.; Goriparti, Subrahmanyam; Merrill, Laura C.; Long, Daniel Martin; Warren, Benjamin; Roberts, Scott A.; Perdue, Brian R.; Casias, Zachary; Cuillier, Paul; Boyce, Brad L.; Jungjohann, Katherine L.

doi:10.1021/acsami.1c06488

Effects of Applied Interfacial Pressure on Li-Metal Cycling Performance and Morphology in 4 M LiFSI in DME

Journal Article · Mon Jun 28 00:00:00 EDT 2021 · ACS Applied Materials and Interfaces

DOI:https://doi.org/10.1021/acsami.1c06488· OSTI ID:1810402

^[1]; ^[1]; ^[1]; Long, Daniel Martin ^[1]; Warren, Benjamin ^[1]; ^[1]; Perdue, Brian R. ^[1]; Casias, Zachary ^[1]; Cuillier, Paul ^[1]; Boyce, Brad L. ^[1]; ^[1]

Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)

Lithium-metal anodes can theoretically enable 10x higher gravimetric capacity than conventional graphite anodes. However, Li-metal anode cycling has proven difficult due to porous and dendritic morphologies, extensive parasitic solid electrolyte interphase reactions, and formation of dead Li. We systematically investigate the effects of applied interfacial pressure on Li-metal anode cycling performance and morphology in the recently developed and highly efficient 4 M lithium bis(fluorosulfonyl)imide in 1,2-dimethoxyethane electrolyte. We present cycling, morphology, and impedance data at a current density of 0.5 mA/cm² and a capacity of 2 mAh/cm² at applied interfacial pressures of 0, 0.01, 0.1, 1, and 10 MPa. Cryo-focused ion beam milling and cryo-scanning electron microscopy imaging in cross section reveal that increasing the applied pressure during Li deposition from 0 to 10 MPa leads to greater than a fivefold reduction in thickness (and therefore volume) of the deposited Li. This suggests that pressure during cycling can have a profound impact on the practical volumetric energy density for Li-metal anodes. A “goldilocks zone” of cell performance is observed at intermediate pressures of 0.1–1 MPa. Increasing pressure from 0 to 1 MPa generally improves cell-to-cell reproducibility, cycling stability, and Coulombic efficiency. However, the highest pressure (10 MPa) results in high cell overpotential and evidence of soft short circuits, which likely result from transport limitations associated with increased pressure causing local pore closure in the separator. All cells exhibit at least some signs of cycling instability after 50 cycles when cycled to 2 mAh/cm² with thin 50 μm Li counter electrodes, though instability decreases with increasing pressure. In contrast, cells cycled to only 1 mAh/cm² perform well for 50 cycles, indicating that capacity plays an important role in cycling stability.

View Accepted Manuscript (DOE)

Research Organization:: Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC04-94AL85000; NA0003525

OSTI ID:: 1810402

Report Number(s):: SAND--2021-8908J; 697419

Journal Information:: ACS Applied Materials and Interfaces, Journal Name: ACS Applied Materials and Interfaces Journal Issue: 27 Vol. 13; ISSN 1944-8244

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

References (68)

A Mechanically Robust and Highly Ion-Conductive Polymer-Blend Coating for High-Power and Long-Life Lithium-Ion Battery Anodes Li, Fu-Sheng; Wu, Yu-Shiang; Chou, Jackey Advanced Materials, Vol. 27, Issue 1 https://doi.org/10.1002/adma.201403880	journal	November 2014
Lithium-Sulfur Cells: The Gap between the State-of-the-Art and the Requirements for High Energy Battery Cells Hagen, Markus; Hanselmann, Dominik; Ahlbrecht, Katharina Advanced Energy Materials, Vol. 5, Issue 16, 1401986 https://doi.org/10.1002/aenm.201401986	journal	April 2015
Flexible Ion-Conducting Composite Membranes for Lithium Batteries Aetukuri, Nagaphani B.; Kitajima, Shintaro; Jung, Edward Advanced Energy Materials, Vol. 5, Issue 14 https://doi.org/10.1002/aenm.201500265	journal	May 2015
Accurate Determination of Coulombic Efficiency for Lithium Metal Anodes and Lithium Metal Batteries Adams, Brian D.; Zheng, Jianming; Ren, Xiaodi Advanced Energy Materials, Vol. 8, Issue 7 https://doi.org/10.1002/aenm.201702097	journal	October 2017
In-situ study of electrode stack growth in rechargeable cells at constant pressure Wilkinson, D. P.; Wainwright, D. Journal of Electroanalytical Chemistry, Vol. 355, Issue 1-2 https://doi.org/10.1016/0022-0728(93)80362-L	journal	August 1993
Effects of physical constraints on Li cyclability Wilkinson, D. P.; Blom, H.; Brandt, K. Journal of Power Sources, Vol. 36, Issue 4 https://doi.org/10.1016/0378-7753(91)80077-B	journal	December 1991
Progress and prospective of solid-state lithium batteries Takada, Kazunori Acta Materialia, Vol. 61, Issue 3, p. 759-770 https://doi.org/10.1016/j.actamat.2012.10.034	journal	February 2013
Mechanical properties of metallic lithium: from nano to bulk scales Fincher, Cole D.; Ojeda, Daniela; Zhang, Yuwei Acta Materialia, Vol. 186 https://doi.org/10.1016/j.actamat.2019.12.036	journal	March 2020
Lithium metal stripping/plating mechanisms studies: A metallurgical approach Gireaud, L.; Grugeon, S.; Laruelle, S. Electrochemistry Communications, Vol. 8, Issue 10, p. 1639-1649 https://doi.org/10.1016/j.elecom.2006.07.037	journal	October 2006
Effect of vinylene carbonate as additive to electrolyte for lithium metal anode Ota, Hitoshi; Shima, Kunihisa; Ue, Makoto Electrochimica Acta, Vol. 49, Issue 4 https://doi.org/10.1016/j.electacta.2003.09.010	journal	February 2004
Stress evolution in lithium metal electrodes Cho, Jung Hwi; Xiao, Xingcheng; Guo, Kai Energy Storage Materials, Vol. 24 https://doi.org/10.1016/j.ensm.2019.08.008	journal	January 2020
Planting CuGa2 seeds assisted with liquid metal for selective wrapping deposition of lithium Meng, Junwei; Li, Chilin Energy Storage Materials, Vol. 37 https://doi.org/10.1016/j.ensm.2021.02.024	journal	May 2021
Nonlinear aging of cylindrical lithium-ion cells linked to heterogeneous compression Bach, Tobias C.; Schuster, Simon F.; Fleder, Elena Journal of Energy Storage, Vol. 5 https://doi.org/10.1016/j.est.2016.01.003	journal	February 2016
Preventing lithium ion battery failure during high temperatures by externally applied compression Zhao, Yan; Patel, Yatish; Hunt, Ian A. Journal of Energy Storage, Vol. 13 https://doi.org/10.1016/j.est.2017.08.001	journal	October 2017
Characterizing the Li-Solid-Electrolyte Interface Dynamics as a Function of Stack Pressure and Current Density Wang, Michael J.; Choudhury, Rishav; Sakamoto, Jeff Joule, Vol. 3, Issue 9 https://doi.org/10.1016/j.joule.2019.06.017	journal	September 2019
A review on electrolyte additives for lithium-ion batteries Zhang, Sheng Shui Journal of Power Sources, Vol. 162, Issue 2, p. 1379-1394 https://doi.org/10.1016/j.jpowsour.2006.07.074	journal	November 2006
Lithium bis(fluorosulfonyl)imide (LiFSI) as conducting salt for nonaqueous liquid electrolytes for lithium-ion batteries: Physicochemical and electrochemical properties Han, Hong-Bo; Zhou, Si-Si; Zhang, Dai-Jun Journal of Power Sources, Vol. 196, Issue 7 https://doi.org/10.1016/j.jpowsour.2010.12.040	journal	April 2011
The role of mechanically induced separator creep in lithium-ion battery capacity fade Peabody, Christina; Arnold, Craig B. Journal of Power Sources, Vol. 196, Issue 19, p. 8147-8153 https://doi.org/10.1016/j.jpowsour.2011.05.023	journal	October 2011
Suppressed lithium dendrite growth in lithium batteries using ionic liquid electrolytes: Investigation by electrochemical impedance spectroscopy, scanning electron microscopy, and in situ 7Li nuclear magnetic resonance spectroscopy Schweikert, Nina; Hofmann, Andreas; Schulz, Michael Journal of Power Sources, Vol. 228 https://doi.org/10.1016/j.jpowsour.2012.11.124	journal	April 2013
Non-uniform aging of cycled commercial LiFePO4//graphite cylindrical cells revealed by post-mortem analysis Klett, Matilda; Eriksson, Rickard; Groot, Jens Journal of Power Sources, Vol. 257 https://doi.org/10.1016/j.jpowsour.2014.01.105	journal	July 2014
Lithium plating in a commercial lithium-ion battery – A low-temperature aging study Petzl, Mathias; Kasper, Michael; Danzer, Michael A. Journal of Power Sources, Vol. 275 https://doi.org/10.1016/j.jpowsour.2014.11.065	journal	February 2015
Effects of external pressure on the performance and ageing of single-layer lithium-ion pouch cells Mussa, Abdilbari Shifa; Klett, Matilda; Lindbergh, Göran Journal of Power Sources, Vol. 385 https://doi.org/10.1016/j.jpowsour.2018.03.020	journal	May 2018
Sericin protein as a conformal protective layer to enable air-endurable Li metal anodes and high-rate Li-S batteries Wu, Han; Wu, Qingping; Chu, Fulu Journal of Power Sources, Vol. 419 https://doi.org/10.1016/j.jpowsour.2019.02.033	journal	April 2019
Liquid cell transmission electron microscopy observation of lithium metal growth and dissolution: Root growth, dead lithium and lithium flotsams Kushima, Akihiro; So, Kang Pyo; Su, Cong Nano Energy, Vol. 32 https://doi.org/10.1016/j.nanoen.2016.12.001	journal	February 2017
Recent advances in all-solid-state rechargeable lithium batteries Sun, Chunwen; Liu, Jin; Gong, Yudong Nano Energy, Vol. 33 https://doi.org/10.1016/j.nanoen.2017.01.028	journal	March 2017
Insights into morphological evolution and cycling behaviour of lithium metal anode under mechanical pressure Yin, Xuesong; Tang, Wei; Jung, Im Doo Nano Energy, Vol. 50 https://doi.org/10.1016/j.nanoen.2018.06.003	journal	August 2018
Pressure-Driven Interface Evolution in Solid-State Lithium Metal Batteries Zhang, Xin; Wang, Q. Jane; Harrison, Katharine L. Cell Reports Physical Science, Vol. 1, Issue 2 https://doi.org/10.1016/j.xcrp.2019.100012	journal	February 2020
Microstructure and Pressure-Driven Electrodeposition Stability in Solid-State Batteries Verma, Ankit; Kawakami, Hiroki; Wada, Hiroyuki Cell Reports Physical Science, Vol. 2, Issue 1 https://doi.org/10.1016/j.xcrp.2020.100301	journal	January 2021
Use of a Be-dome holder for texture and strain characterization of Li metal thin films via sin ² ( ψ ) methodology Rodriguez, Mark A.; Harrison, Katharine L.; Goriparti, Subrahmanyam Powder Diffraction, Vol. 35, Issue 2 https://doi.org/10.1017/S0885715620000305	journal	June 2020
Toward a Fundamental Understanding of the Lithium Metal Anode in Solid-State Batteries—An Electrochemo-Mechanical Study on the Garnet-Type Solid Electrolyte Li _6.25 Al _0.25 La ₃ Zr ₂ O ₁₂ Krauskopf, Thorben; Hartmann, Hannah; Zeier, Wolfgang G. ACS Applied Materials & Interfaces, Vol. 11, Issue 15 https://doi.org/10.1021/acsami.9b02537	journal	March 2019
Efficient Lithium Metal Cycling over a Wide Range of Pressures from an Anion-Derived Solid-Electrolyte Interphase Framework Wang, Hansen; Huang, William; Yu, Zhiao ACS Energy Letters, Vol. 6, Issue 2 https://doi.org/10.1021/acsenergylett.0c02533	journal	February 2021
Next-Generation Lithium Metal Anode Engineering via Atomic Layer Deposition Kozen, Alexander C.; Lin, Chuan-Fu; Pearse, Alexander J. ACS Nano, Vol. 9, Issue 6 https://doi.org/10.1021/acsnano.5b02166	journal	May 2015
Lithium Self-Discharge and Its Prevention: Direct Visualization through In Situ Electrochemical Scanning Transmission Electron Microscopy Harrison, Katharine L.; Zavadil, Kevin R.; Hahn, Nathan T. ACS Nano, Vol. 11, Issue 11 https://doi.org/10.1021/acsnano.7b05513	journal	September 2017
Effects of Cesium Cations in Lithium Deposition via Self-Healing Electrostatic Shield Mechanism Ding, Fei; Xu, Wu; Chen, Xilin The Journal of Physical Chemistry C, Vol. 118, Issue 8 https://doi.org/10.1021/jp4127754	journal	February 2014
Issues and challenges facing rechargeable lithium batteries Tarascon, J.-M.; Armand, M. Nature, Vol. 414, Issue 6861, p. 359-367 https://doi.org/10.1038/35104644	journal	November 2001
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
Making Li-metal electrodes rechargeable by controlling the dendrite growth direction Liu, Yadong; Liu, Qi; Xin, Le Nature Energy, Vol. 2, Issue 7 https://doi.org/10.1038/nenergy.2017.83	journal	June 2017
Interconnected hollow carbon nanospheres for stable lithium metal anodes Zheng, Guangyuan; Lee, Seok Woo; Liang, Zheng Nature Nanotechnology, Vol. 9, Issue 8 https://doi.org/10.1038/nnano.2014.152	journal	July 2014
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
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
High-energy lithium metal pouch cells with limited anode swelling and long stable cycles Niu, Chaojiang; Lee, Hongkyung; Chen, Shuru Nature Energy, Vol. 4, Issue 7 https://doi.org/10.1038/s41560-019-0390-6	journal	May 2019
Long cycle life and dendrite-free lithium morphology in anode-free lithium pouch cells enabled by a dual-salt liquid electrolyte Weber, Rochelle; Genovese, Matthew; Louli, A. J. Nature Energy, Vol. 4, Issue 8 https://doi.org/10.1038/s41560-019-0428-9	journal	July 2019
Diagnosing and correcting anode-free cell failure via electrolyte and morphological analysis Louli, A. J.; Eldesoky, A.; Weber, Rochelle Nature Energy, Vol. 5, Issue 9 https://doi.org/10.1038/s41560-020-0668-8	journal	August 2020
Origin of lithium whisker formation and growth under stress He, Yang; Ren, Xiaodi; Xu, Yaobin Nature Nanotechnology, Vol. 14, Issue 11 https://doi.org/10.1038/s41565-019-0558-z	journal	October 2019
Quantifying inactive lithium in lithium metal batteries Fang, Chengcheng; Li, Jinxing; Zhang, Minghao Nature, Vol. 572, Issue 7770 https://doi.org/10.1038/s41586-019-1481-z	journal	August 2019
Effect of nanopatterning on mechanical properties of Lithium anode Campbell, Colin; Lee, Yong Min; Cho, Kuk Young Scientific Reports, Vol. 8, Issue 1 https://doi.org/10.1038/s41598-018-20773-8	journal	February 2018
The critical role of lithium nitrate in the gas evolution of lithium–sulfur batteries Jozwiuk, Anna; Berkes, Balázs B.; Weiß, Thomas Energy & Environmental Science, Vol. 9, Issue 8 https://doi.org/10.1039/C6EE00789A	journal	January 2016
Dead lithium: mass transport effects on voltage, capacity, and failure of lithium metal anodes Chen, Kuan-Hung; Wood, Kevin N.; Kazyak, Eric Journal of Materials Chemistry A, Vol. 5, Issue 23 https://doi.org/10.1039/C7TA00371D	journal	January 2017
Cycling behaviour of Li/Li4Ti5O12 cells studied by electrochemical impedance spectroscopy Schweikert, Nina; Hahn, Horst; Indris, Sylvio Physical Chemistry Chemical Physics, Vol. 13, Issue 13 https://doi.org/10.1039/c0cp01889a	journal	January 2011
Metallic anodes for next generation secondary batteries Kim, Hansu; Jeong, Goojin; Kim, Young-Ugk Chemical Society Reviews, Vol. 42, Issue 23 https://doi.org/10.1039/c3cs60177c	journal	January 2013
Quantifying the promise of lithium–air batteries for electric vehicles Gallagher, Kevin G.; Goebel, Steven; Greszler, Thomas Energy & Environmental Science, Vol. 7, Issue 5 https://doi.org/10.1039/c3ee43870h	journal	January 2014
Self-heating–induced healing of lithium dendrites Li, Lu; Basu, Swastik; Wang, Yiping Science, Vol. 359, Issue 6383 https://doi.org/10.1126/science.aap8787	journal	March 2018
A Study of Capacity Fade in Cylindrical and Prismatic Lithium-Ion Batteries Rubino, Robert S.; Gan, Hong; Takeuchi, Esther S. Journal of The Electrochemical Society, Vol. 148, Issue 9 https://doi.org/10.1149/1.1390344	journal	January 2001
The Surface Film Formed on a Lithium Metal Electrode in a New Imide Electrolyte, Lithium Bis(perfluoroethylsulfonylimide) [LiN(C[sub 2]F[sub 5]SO[sub 2])[sub 2]] Naoi, Katsuhiko Journal of The Electrochemical Society, Vol. 146, Issue 2 https://doi.org/10.1149/1.1391629	journal	January 1999
Influence of Electrolyte on Lithium Cycling Efficiency with Pressurized Electrode Stack Hirai, Toshiro Journal of The Electrochemical Society, Vol. 141, Issue 3 https://doi.org/10.1149/1.2054778	journal	January 1994
Effect of Additives on Lithium Cycling Efficiency Hirai, Toshiro; Yoshimatsu, Isamu; Yamaki, Jun‐ichi Journal of The Electrochemical Society, Vol. 141, Issue 9, p. 2300-2305 https://doi.org/10.1149/1.2055116	journal	January 1994
The Importance of Interphase Contacts in Li Ion Electrodes: The Meaning of the High-Frequency Impedance Arc Gaberscek, Miran; Moskon, Joze; Erjavec, Bostjan Electrochemical and Solid-State Letters, Vol. 11, Issue 10 https://doi.org/10.1149/1.2964220	journal	January 2008
High Energy Rechargeable Li-S Cells for EV Application: Status, Remaining Problems and Solutions Mikhaylik, Yuriy V.; Kovalev, Igor; Schock, Riley 216th ECS Meeting, ECS Transactions https://doi.org/10.1149/1.3414001	conference	January 2010
Exploring the Impact of Mechanical Pressure on the Performance of Anode-Free Lithium Metal Cells Louli, A. J.; Genovese, Matthew; Weber, Rochelle Journal of The Electrochemical Society, Vol. 166, Issue 8 https://doi.org/10.1149/2.0091908jes	journal	January 2019
Lithium Mechanics: Roles of Strain Rate and Temperature and Implications for Lithium Metal Batteries LePage, William S.; Chen, Yuxin; Kazyak, Eric Journal of The Electrochemical Society, Vol. 166, Issue 2 https://doi.org/10.1149/2.0221902jes	journal	January 2019
Stress Evolution in Lithium-Ion Composite Electrodes during Electrochemical Cycling and Resulting Internal Pressures on the Cell Casing Nadimpalli, Siva P. V.; Sethuraman, Vijay A.; Abraham, Daniel P. Journal of The Electrochemical Society, Vol. 162, Issue 14 https://doi.org/10.1149/2.0341514jes	journal	January 2015
Critical Link between Materials Chemistry and Cell-Level Design for High Energy Density and Low Cost Lithium-Sulfur Transportation Battery Eroglu, Damla; Zavadil, Kevin R.; Gallagher, Kevin G. Journal of The Electrochemical Society, Vol. 162, Issue 6 https://doi.org/10.1149/2.0611506jes	journal	January 2015
Rethinking How External Pressure Can Suppress Dendrites in Lithium Metal Batteries Zhang, Xin; Wang, Q. Jane; Harrison, Katharine L. Journal of The Electrochemical Society, Vol. 166, Issue 15 https://doi.org/10.1149/2.0701914jes	journal	January 2019
Symmetrical Impedance Study on Inactivation Induced Degradation of Lithium Electrodes for Batteries Beyond Lithium-Ion Woo, Jung-Je; Maroni, Victor A.; Liu, Gao Journal of The Electrochemical Society, Vol. 161, Issue 5 https://doi.org/10.1149/2.089405jes	journal	January 2014
Effects of Carbonate Solvents and Lithium Salts on Morphology and Coulombic Efficiency of Lithium Electrode Ding, Fei; Xu, Wu; Chen, Xilin Journal of The Electrochemical Society, Vol. 160, Issue 10 https://doi.org/10.1149/2.100310jes	journal	January 2013
Investigation of Electronic Resistance in Lithium-Ion Batteries by AC Impedance Spectroscopy Takeno, Mitsuhiro; Fukutsuka, Tomokazu; Miyazaki, Kohei Journal of The Electrochemical Society, Vol. 164, Issue 14 https://doi.org/10.1149/2.1381714jes	journal	January 2017
Nanoindentation of high-purity vapor deposited lithium films: A mechanistic rationalization of diffusion-mediated flow Herbert, Erik G.; Hackney, Stephen A.; Thole, Violet Journal of Materials Research, Vol. 33, Issue 10 https://doi.org/10.1557/jmr.2018.84	journal	May 2018

Similar Records

Working Principle of an Ionic Liquid Interlayer During Pressureless Lithium Stripping on Li _6.25 Al _0.25 La ₃ Zr ₂ O ₁₂ (LLZO) Garnet‐Type Solid Electrolyte

Journal Article · Fri Mar 26 00:00:00 EDT 2021 · Batteries & Supercaps · OSTI ID:1772837

A Highly Reversible, Dendrite‐Free Lithium Metal Anode Enabled by a Lithium‐Fluoride‐Enriched Interphase

Journal Article · Thu Feb 13 23:00:00 EST 2020 · Advanced Materials · OSTI ID:1599685

Related Subjects

25 ENERGY STORAGE
batteries
electrochemical cells
electrodes
electrolytes
high concentration electrolyte
interfacial pressure
lithium
lithium-metal anodes
morphology

Effects of Applied Interfacial Pressure on Li-Metal Cycling Performance and Morphology in 4 M LiFSI in DME

Citation Formats

References (68)

Similar Records

Related Subjects