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Title: Strategies towards enabling lithium metal in batteries: interphases and electrodes

Abstract

Despite the continuous increase in capacity, lithium-ion intercalation batteries are approaching their performance limits. As a result, research is intensifying on next-generation battery technologies. The use of a lithium metal anode promises the highest theoretical energy density and enables use of lithium-free or novel high-energy cathodes. However, the lithium metal anode suffers from poor morphological stability and Coulombic efficiency during cycling, especially in liquid electrolytes. In contrast to solid electrolytes, liquid electrolytes have the advantage of high ionic conductivity and good wetting of the anode, despite the lithium metal volume change during cycling. Rapid capacity fade due to inhomogeneous deposition and dissolution of lithium is the main hindrance to the successful utilization of the lithium metal anode in combination with liquid electrolytes. In this perspective, we discuss how experimental and theoretical insights can provide possible pathways for reversible cycling of two-dimensional lithium metal. Therefore, we discuss improvements in the understanding of lithium metal nucleation, deposition, and stripping on the nanoscale. As the solid–electrolyte interphase (SEI) plays a key role in the lithium morphology, we discuss how the proper SEI design might allow stable cycling. We highlight recent advances in conventional and (localized) highly concentrated electrolytes in view of their respectivemore » SEIs. We also discuss artificial interphases and three-dimensional host frameworks, which show prospects of mitigating morphological instabilities and suppressing large shape change on the electrode level.« less

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [1]; ORCiD logo [4]; ORCiD logo [5]; ORCiD logo [6]; ORCiD logo [7]; ORCiD logo [8]; ORCiD logo [9]; ORCiD logo [10]; ORCiD logo [11]; ORCiD logo [12];  [2]; ORCiD logo [13]; ORCiD logo [5];  [6]; ORCiD logo [6]; ORCiD logo [8]; ORCiD logo [11] more »; ORCiD logo [10]; ORCiD logo [10]; ORCiD logo [13]; ORCiD logo [12]; ORCiD logo [14]; ORCiD logo [15]; ORCiD logo [16]; ORCiD logo [4]; ORCiD logo [1] « less
+ Show Author Affiliations
  1. Helmholtz Institute Ulm (HIU), Ulm 89081, Germany, German Aerospace Center (DLR), Stuttgart 70569, Germany
  2. Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, IL 60439, USA
  3. Material Sciences Division, Argonne National Laboratory, Lemont, IL 60439, USA
  4. Energy Storage and Distributed Resources Division, Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA 94720, USA
  5. Energy and Environment Directorate, Pacific Northwest National Laboratory (PNNL), Richland, WA 99354, USA
  6. Institute of Energy and Climate Research IEK-9, Forschungszentrum Jülich GmbH, Jülich, Germany
  7. Helmholtz-Institute Münster (HI MS), IEK-12, Forschungszentrum Jülich GmbH, Münster, 48149, Germany
  8. University of Münster, MEET Battery Research Center, Münster, 48149, Germany
  9. Research Laboratory of Electronics, Massachusetts Institute of Technology (MIT), Cambridge, Massachusetts 02139, USA
  10. Department of Chemical Engineering, Texas A&M University, College Station, TX 77843, USA
  11. Institute for Applied Materials – Electrochemical Technologies (IAM-ET), Karlsruhe Institute of Technology (KIT), Karlsruhe 76021, Germany
  12. Helmholtz Institute Ulm (HIU), Ulm 89081, Germany, Karlsruhe Institute of Technology (KIT), Karlsruhe 76021, Germany
  13. Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory (PNNL), Richland, WA 99354, USA
  14. Research Laboratory of Electronics, Massachusetts Institute of Technology (MIT), Cambridge, Massachusetts 02139, USA, Department of Mechanical Engineering, Massachusetts Institute of Technology (MIT), Cambridge, MA 02139, USA, Department of Materials Science and Engineering, Massachusetts Institute of Technology (MIT), Cambridge, MA 02139, USA
  15. Helmholtz-Institute Münster (HI MS), IEK-12, Forschungszentrum Jülich GmbH, Münster, 48149, Germany, University of Münster, MEET Battery Research Center, Münster, 48149, Germany
  16. Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, IL 60439, USA, Material Science and Engineering, Stanford University, Stanford, CA 94305, USA
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE)
OSTI Identifier:
1811080
Alternate Identifier(s):
OSTI ID: 1819859; OSTI ID: 1830505; OSTI ID: 1840906
Report Number(s):
PNNL-SA-160592
Journal ID: ISSN 1754-5692; EESNBY
Grant/Contract Number:  
AC02-05CH11231; AC05-76RL01830; AC02-06CH11357
Resource Type:
Published Article
Journal Name:
Energy & Environmental Science
Additional Journal Information:
Journal Name: Energy & Environmental Science Journal Volume: 14 Journal Issue: 10; Journal ID: ISSN 1754-5692
Publisher:
Royal Society of Chemistry (RSC)
Country of Publication:
United Kingdom
Language:
English
Subject:
25 ENERGY STORAGE

Citation Formats

Horstmann, Birger, Shi, Jiayan, Amine, Rachid, Werres, Martin, He, Xin, Jia, Hao, Hausen, Florian, Cekic-Laskovic, Isidora, Wiemers-Meyer, Simon, Lopez, Jeffrey, Galvez-Aranda, Diego, Baakes, Florian, Bresser, Dominic, Su, Chi-Cheung, Xu, Yaobin, Xu, Wu, Jakes, Peter, Eichel, Rüdiger-A., Figgemeier, Egbert, Krewer, Ulrike, Seminario, Jorge M., Balbuena, Perla B., Wang, Chongmin, Passerini, Stefano, Shao-Horn, Yang, Winter, Martin, Amine, Khalil, Kostecki, Robert, and Latz, Arnulf. Strategies towards enabling lithium metal in batteries: interphases and electrodes. United Kingdom: N. p., 2021. Web. doi:10.1039/D1EE00767J.
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Horstmann, Birger, Shi, Jiayan, Amine, Rachid, Werres, Martin, He, Xin, Jia, Hao, Hausen, Florian, Cekic-Laskovic, Isidora, Wiemers-Meyer, Simon, Lopez, Jeffrey, Galvez-Aranda, Diego, Baakes, Florian, Bresser, Dominic, Su, Chi-Cheung, Xu, Yaobin, Xu, Wu, Jakes, Peter, Eichel, Rüdiger-A., Figgemeier, Egbert, Krewer, Ulrike, Seminario, Jorge M., Balbuena, Perla B., Wang, Chongmin, Passerini, Stefano, Shao-Horn, Yang, Winter, Martin, Amine, Khalil, Kostecki, Robert, & Latz, Arnulf. Strategies towards enabling lithium metal in batteries: interphases and electrodes. United Kingdom. https://doi.org/10.1039/D1EE00767J
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Horstmann, Birger, Shi, Jiayan, Amine, Rachid, Werres, Martin, He, Xin, Jia, Hao, Hausen, Florian, Cekic-Laskovic, Isidora, Wiemers-Meyer, Simon, Lopez, Jeffrey, Galvez-Aranda, Diego, Baakes, Florian, Bresser, Dominic, Su, Chi-Cheung, Xu, Yaobin, Xu, Wu, Jakes, Peter, Eichel, Rüdiger-A., Figgemeier, Egbert, Krewer, Ulrike, Seminario, Jorge M., Balbuena, Perla B., Wang, Chongmin, Passerini, Stefano, Shao-Horn, Yang, Winter, Martin, Amine, Khalil, Kostecki, Robert, and Latz, Arnulf. Wed . "Strategies towards enabling lithium metal in batteries: interphases and electrodes". United Kingdom. https://doi.org/10.1039/D1EE00767J.
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@article{osti_1811080,
title = {Strategies towards enabling lithium metal in batteries: interphases and electrodes},
author = {Horstmann, Birger and Shi, Jiayan and Amine, Rachid and Werres, Martin and He, Xin and Jia, Hao and Hausen, Florian and Cekic-Laskovic, Isidora and Wiemers-Meyer, Simon and Lopez, Jeffrey and Galvez-Aranda, Diego and Baakes, Florian and Bresser, Dominic and Su, Chi-Cheung and Xu, Yaobin and Xu, Wu and Jakes, Peter and Eichel, Rüdiger-A. and Figgemeier, Egbert and Krewer, Ulrike and Seminario, Jorge M. and Balbuena, Perla B. and Wang, Chongmin and Passerini, Stefano and Shao-Horn, Yang and Winter, Martin and Amine, Khalil and Kostecki, Robert and Latz, Arnulf},
abstractNote = {Despite the continuous increase in capacity, lithium-ion intercalation batteries are approaching their performance limits. As a result, research is intensifying on next-generation battery technologies. The use of a lithium metal anode promises the highest theoretical energy density and enables use of lithium-free or novel high-energy cathodes. However, the lithium metal anode suffers from poor morphological stability and Coulombic efficiency during cycling, especially in liquid electrolytes. In contrast to solid electrolytes, liquid electrolytes have the advantage of high ionic conductivity and good wetting of the anode, despite the lithium metal volume change during cycling. Rapid capacity fade due to inhomogeneous deposition and dissolution of lithium is the main hindrance to the successful utilization of the lithium metal anode in combination with liquid electrolytes. In this perspective, we discuss how experimental and theoretical insights can provide possible pathways for reversible cycling of two-dimensional lithium metal. Therefore, we discuss improvements in the understanding of lithium metal nucleation, deposition, and stripping on the nanoscale. As the solid–electrolyte interphase (SEI) plays a key role in the lithium morphology, we discuss how the proper SEI design might allow stable cycling. We highlight recent advances in conventional and (localized) highly concentrated electrolytes in view of their respective SEIs. We also discuss artificial interphases and three-dimensional host frameworks, which show prospects of mitigating morphological instabilities and suppressing large shape change on the electrode level.},
doi = {10.1039/D1EE00767J},
journal = {Energy & Environmental Science},
number = 10,
volume = 14,
place = {United Kingdom},
year = {Wed Oct 13 00:00:00 EDT 2021},
month = {Wed Oct 13 00:00:00 EDT 2021}
}
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Review—SEI: Past, Present and Future
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  • Peled, E.; Menkin, S.
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High rate and stable cycling of lithium metal anode
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Lithium-ion batteries – Current state of the art and anticipated developments
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Lithium Mechanics: Roles of Strain Rate and Temperature and Implications for Lithium Metal Batteries
journal, January 2019

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Correlating Structure and Function of Battery Interphases at Atomic Resolution Using Cryoelectron Microscopy
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Stabilization of Lithium-Metal Batteries Based on the in Situ Formation of a Stable Solid Electrolyte Interphase Layer
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Lithium dendrite growth mechanisms in liquid electrolytes
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An Artificial Solid Electrolyte Interphase Layer for Stable Lithium Metal Anodes
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Dynamic TGA–FTIR studies on the thermal stability of lithium/graphite with electrolyte in lithium-ion cell
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Theory of Impedance Spectroscopy for Lithium Batteries
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Deformation and Fracture of Polycrystalline Lithium Fluoride
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Decomposition of Imidazolium-Based Ionic Liquids in Contact with Lithium Metal
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Lithium Fluoride Additives for Stable Cycling of Lithium Batteries at High Current Densities
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Dendrite formation in silicon anodes of lithium-ion batteries
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Fractal growth of copper electrodeposits
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Long cycle life and dendrite-free lithium morphology in anode-free lithium pouch cells enabled by a dual-salt liquid electrolyte
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Elastic, plastic, and creep mechanical properties of lithium metal
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Designing Artificial Solid-Electrolyte Interphases for Single-Ion and High-Efficiency Transport in Batteries
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Nonaqueous Liquid Electrolytes for Lithium-Based Rechargeable Batteries
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The Impact of Li Grain Size on Coulombic Efficiency in Li Batteries
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Interactions between Lithium Growths and Nanoporous Ceramic Separators
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Studies of zinc whiskers formation and growth from bright zinc electrodeposits
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An In Vivo Formed Solid Electrolyte Surface Layer Enables Stable Plating of Li Metal
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Extremely Accessible Potassium Nitrate (KNO 3 ) as the Highly Efficient Electrolyte Additive in Lithium Battery
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Enabling high energy density Li-ion batteries through Li2O activation
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Preferential Solvation of Li+ Directs Formation of Interphase on Graphitic Anode
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Formation and Growth Mechanisms of Solid-Electrolyte Interphase Layers in Rechargeable Batteries
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Review on modeling of the anode solid electrolyte interphase (SEI) for lithium-ion batteries
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Li + Transference Numbers in Liquid Electrolytes Obtained by Very-Low-Frequency Impedance Spectroscopy at Variable Electrode Distances
journal, January 2016

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Ionic conductivity in Li 3 N single crystals
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Evolution of Strategies for Modern Rechargeable Batteries
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Countersolvent Electrolytes for Lithium‐Metal Batteries
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Lithium metal stripping beneath the solid electrolyte interphase
journal, August 2018

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The effect of electroplating parameters and substrate material on tin whisker formation
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Nanoscale Nucleation and Growth of Electrodeposited Lithium Metal
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Cycling a Lithium Metal Anode at 90 °C in a Liquid Electrolyte
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Fluoroethylene Carbonate as Electrolyte Additive in Tetraethylene Glycol Dimethyl Ether Based Electrolytes for Application in Lithium Ion and Lithium Metal Batteries
journal, January 2015

  • Heine, Jennifer; Hilbig, Peter; Qi, Xin
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Lithiophilic Sites in Doped Graphene Guide Uniform Lithium Nucleation for Dendrite-Free Lithium Metal Anodes
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Recent Advances in Mitigation of Whiskers from Electroplated Tin
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Bottom-Up Lithium Growth Triggered by Interfacial Activity Gradient on Porous Framework for Lithium-Metal Anode
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Alloy Negative Electrodes for Li-Ion Batteries
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Poor Man’s Atomic Layer Deposition of LiF for Additive-Free Growth of Lithium Columns
journal, October 2018

Solvation Rule for Solid‐Electrolyte Interphase Enabler in Lithium‐Metal Batteries
journal, August 2020

Fluorine-donating electrolytes enable highly reversible 5-V-class Li metal batteries
journal, January 2018

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Overcoming the Interfacial Limitations Imposed by the Solid–Solid Interface in Solid‐State Batteries Using Ionic Liquid‐Based Interlayers
journal, April 2020

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A Review of Solid Electrolyte Interphases on Lithium Metal Anode
journal, November 2015

In situ NMR observation of the formation of metallic lithium microstructures in lithium batteries
journal, May 2010

  • Bhattacharyya, Rangeet; Key, Baris; Chen, Hailong
  • Nature Materials, Vol. 9, Issue 6
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Revealing SEI Morphology: In-Depth Analysis of a Modeling Approach
journal, January 2017

  • Single, Fabian; Horstmann, Birger; Latz, Arnulf
  • Journal of The Electrochemical Society, Vol. 164, Issue 11
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In situ Microscopic Observation of Sodium Deposition/Dissolution on Sodium Electrode
journal, March 2016

  • Yui, Yuhki; Hayashi, Masahiko; Nakamura, Jiro
  • Scientific Reports, Vol. 6, Issue 1
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Electrolyte additive enabled fast charging and stable cycling lithium metal batteries
journal, March 2017

Circumventing huge volume strain in alloy anodes of lithium batteries
journal, April 2020

Superconcentrated electrolytes for a high-voltage lithium-ion battery
journal, June 2016

  • Wang, Jianhui; Yamada, Yuki; Sodeyama, Keitaro
  • Nature Communications, Vol. 7, Issue 1
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A Flexible Solid Electrolyte Interphase Layer for Long-Life Lithium Metal Anodes
journal, January 2018

  • Li, Nian-Wu; Shi, Yang; Yin, Ya-Xia
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Ionomer-Liquid Electrolyte Hybrid Ionic Conductor for High Cycling Stability of Lithium Metal Electrodes
journal, September 2015

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  • Scientific Reports, Vol. 5, Issue 1
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Implantable Solid Electrolyte Interphase in Lithium-Metal Batteries
journal, February 2017

2-Fluoropyridine: A novel electrolyte additive for lithium metal batteries with high areal capacity as well as high cycling stability
journal, August 2020

Li2O-Reinforced Solid Electrolyte Interphase on Three-Dimensional Sponges for Dendrite-Free Lithium Deposition
journal, November 2018

Quantitative phase-field modeling of dendritic electrodeposition
journal, July 2015

Micromorphological Studies of Lithium Electrodes in Alkyl Carbonate Solutions Using in Situ Atomic Force Microscopy
journal, December 2000

  • Cohen, Yaron S.; Cohen, Yair; Aurbach, Doron
  • The Journal of Physical Chemistry B, Vol. 104, Issue 51
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Galvanic Corrosion of Lithium‐Powder‐Based Electrodes
journal, March 2020

  • Kolesnikov, Aleksei; Kolek, Martin; Dohmann, Jan Frederik
  • Advanced Energy Materials, Vol. 10, Issue 15
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Study of the electrochemical deposition of Mg in the atomic level: Why it prefers the non-dendritic morphology
journal, August 2012

Ionic Liquid Electrolytes for Li–Air Batteries: Lithium Metal Cycling
journal, May 2014

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Heterogeneous Nucleation and Growth of Lithium Electrodeposits on Negative Electrodes
journal, January 2013

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Microscopic observations of the formation, growth and shrinkage of lithium moss during electrodeposition and dissolution
journal, August 2014

Investigation of solvation in lithium ion battery electrolytes by NMR spectroscopy
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Natural SEI-Inspired Dual-Protective Layers via Atomic/Molecular Layer Deposition for Long-Life Metallic Lithium Anode
journal, November 2019

Critical Evaluation of the Use of 3D Carbon Networks Enhancing the Long-Term Stability of Lithium Metal Anodes
journal, October 2019

Suppression of Dendrite Formation via Pulse Charging in Rechargeable Lithium Metal Batteries
journal, December 2012

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Electrolytes and Interphases in Li-Ion Batteries and Beyond
journal, October 2014

High-Performance Lithium Metal Negative Electrode with a Soft and Flowable Polymer Coating
journal, November 2016

Local, submicron, strain gradients as the cause of Sn whisker growth
journal, June 2009

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Recent Progress in Understanding Solid Electrolyte Interphase on Lithium Metal Anodes
journal, December 2020

  • Wu, Haiping; Jia, Hao; Wang, Chongmin
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Calendar Aging of Lithium-Ion Batteries: I. Impact of the Graphite Anode on Capacity Fade
journal, January 2016

  • Keil, Peter; Schuster, Simon F.; Wilhelm, Jörn
  • Journal of The Electrochemical Society, Vol. 163, Issue 9
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Glassy Li metal anode for high-performance rechargeable Li batteries
journal, July 2020

Direct Calculation of Li-Ion Transport in the Solid Electrolyte Interphase
journal, September 2012

  • Shi, Siqi; Lu, Peng; Liu, Zhongyi
  • Journal of the American Chemical Society, Vol. 134, Issue 37
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Advanced Electrolytes for Fast‐Charging High‐Voltage Lithium‐Ion Batteries in Wide‐Temperature Range
journal, April 2020

  • Zhang, Xianhui; Zou, Lianfeng; Xu, Yaobin
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Composition analysis of the passive film on the carbon electrode of a lithium-ion battery with an EC-based electrolyte
journal, March 1998

Observations on the growth of whisker crystals from zinc electroplate
journal, August 1975

Enabling Ether-Based Electrolytes for Long Cycle Life of Lithium-Ion Batteries at High Charge Voltage
journal, November 2020

  • Jia, Hao; Xu, Yaobin; Burton, Sarah D.
  • ACS Applied Materials & Interfaces, Vol. 12, Issue 49
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Lithium Planar Deposition vs Whisker Growth: Crucial Role of Surface Diffusion
journal, December 2020

  • Rulev, Alexey A.; Kondratyeva, Yevgeniya O.; Yashina, Lada V.
  • The Journal of Physical Chemistry Letters, Vol. 11, Issue 24
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Novel dual-salts electrolyte solution for dendrite-free lithium-metal based rechargeable batteries with high cycle reversibility
journal, December 2014

Physical and Electrochemical Properties of N -Alkyl- N -methylpyrrolidinium Bis(fluorosulfonyl)imide Ionic Liquids: PY 13 FSI and PY 14 FSI
journal, October 2008

  • Zhou, Qian; Henderson, Wesley A.; Appetecchi, Giovanni B.
  • The Journal of Physical Chemistry B, Vol. 112, Issue 43
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Fluorinated Solid-Electrolyte Interphase in High-Voltage Lithium Metal Batteries
journal, November 2019

Lithium Nitrate Solvation Chemistry in Carbonate Electrolyte Sustains High-Voltage Lithium Metal Batteries
journal, September 2018

  • Yan, Chong; Yao, Yu-Xing; Chen, Xiang
  • Angewandte Chemie International Edition, Vol. 57, Issue 43
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Direct Observation of SEI Formation and Lithiation in Thin-Film Silicon Electrodes via in Situ Electrochemical Atomic Force Microscopy
journal, August 2019

  • Benning, Svenja; Chen, Chunguang; Eichel, Rüdiger-A.
  • ACS Applied Energy Materials, Vol. 2, Issue 9
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Interface engineering of sulfide electrolytes for all-solid-state lithium batteries
journal, November 2018

Solubility-mediated sustained release enabling nitrate additive in carbonate electrolytes for stable lithium metal anode
journal, September 2018

A Sustainable Solid Electrolyte Interphase for High‐Energy‐Density Lithium Metal Batteries Under Practical Conditions
journal, February 2020

  • Zhang, Xue‐Qiang; Li, Tao; Li, Bo‐Quan
  • Angewandte Chemie International Edition, Vol. 59, Issue 8
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Fluorine and Lithium: Ideal Partners for High‐Performance Rechargeable Battery Electrolytes
journal, November 2019

  • Aspern, N.; Röschenthaler, G. ‐V.; Winter, M.
  • Angewandte Chemie International Edition, Vol. 58, Issue 45
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An ultrastable lithium metal anode enabled by designed metal fluoride spansules
journal, March 2020

Li plating as unwanted side reaction in commercial Li-ion cells – A review
journal, April 2018

New Insights on the Structure of Electrochemically Deposited Lithium Metal and Its Solid Electrolyte Interphases via Cryogenic TEM
journal, November 2017

Interface Stability in Solid-State Batteries
journal, December 2015

A new class of Solvent-in-Salt electrolyte for high-energy rechargeable metallic lithium batteries
journal, February 2013

  • Suo, Liumin; Hu, Yong-Sheng; Li, Hong
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In Situ Chemical Imaging of Solid-Electrolyte Interphase Layer Evolution in Li–S Batteries
journal, May 2017

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  • Chemistry of Materials, Vol. 29, Issue 11
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Effects of Polymer Coatings on Electrodeposited Lithium Metal
journal, August 2018

  • Lopez, Jeffrey; Pei, Allen; Oh, Jin Young
  • Journal of the American Chemical Society, Vol. 140, Issue 37
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Atomic structure of sensitive battery materials and interfaces revealed by cryo–electron microscopy
journal, October 2017

Mesoscale Anatomy of Dead Lithium Formation
journal, March 2020

  • Tewari, Deepti; Rangarajan, Sobana P.; Balbuena, Perla B.
  • The Journal of Physical Chemistry C, Vol. 124, Issue 12
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A Yolk-Shell Design for Stabilized and Scalable Li-Ion Battery Alloy Anodes
journal, May 2012

  • Liu, Nian; Wu, Hui; McDowell, Matthew T.
  • Nano Letters, Vol. 12, Issue 6
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Thermodynamic Overpotentials and Nucleation Rates for Electrodeposition on Metal Anodes
journal, January 2019

  • Nagy, Kyle S.; Kazemiabnavi, Saeed; Thornton, Katsuyo
  • ACS Applied Materials & Interfaces, Vol. 11, Issue 8
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Electrolyte roadblocks to a magnesium rechargeable battery
journal, January 2012

  • Muldoon, John; Bucur, Claudiu B.; Oliver, Allen G.
  • Energy & Environmental Science, Vol. 5, Issue 3, p. 5941-5950
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