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Title: High rate and stable cycling of lithium metal anode

Abstract

Lithium (Li) metal is an ideal anode material for rechargeable batteries. However, dendritic Li growth and limited Coulombic efficiency (CE) during repeated Li deposition/stripping processes have prevented the application of this anode in rechargeable Li metal batteries, especially for use at high current densities. Here, we report that the use of highly concentrated electrolytes composed of ether solvents and the lithium bis(fluorosulfonyl)imide (LiFSI) salt enables the high rate cycling of a Li metal anode at high CE (up to 99.1 %) without dendrite growth. With 4 M LiFSI in 1,2-dimethoxyethane (DME) as the electrolyte, a Li|Li cell can be cycled at high rates (10 mA cm-2) for more than 6000 cycles with no increase in the cell impedance, and a Cu|Li cell can be cycled at 4 mA cm-2 for more than 1000 cycles with an average CE of 98.4%. These excellent high rate performances can be attributed to the increased solvent coordination and increased availability of Li+ concentration in the electrolyte. Lastly, further development of this electrolyte may lead to practical applications for Li metal anode in rechargeable batteries. The fundamental mechanisms behind the high rate ion exchange and stability of the electrolytes also shine light on the stabilitymore » of other electrochemical systems.« less

Authors:
 [1];  [1];  [1];  [2];  [3];  [4];  [1]
  1. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Joint Center for Energy Storage Research; Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Energy & Environment Directorate
  2. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Energy & Environment Directorate
  3. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL)
  4. U.S. Army Research Lab., Adelphi, MD (United States). Sensor & Electron Devices Directorate
Publication Date:
Research Org.:
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States). Environmental Molecular Sciences Laboratory (EMSL)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1184948
Report Number(s):
PNNL-SA-107989
Journal ID: ISSN 2041-1723; 48379; 48316; KC0208010
Grant/Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 6; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE

Citation Formats

Qian, Jiangfeng, Henderson, Wesley A., Xu, Wu, Bhattacharya, Priyanka, Engelhard, Mark H., Borodin, Oleg, and Zhang, Jiguang. High rate and stable cycling of lithium metal anode. United States: N. p., 2015. Web. doi:10.1038/ncomms7362.
Qian, Jiangfeng, Henderson, Wesley A., Xu, Wu, Bhattacharya, Priyanka, Engelhard, Mark H., Borodin, Oleg, & Zhang, Jiguang. High rate and stable cycling of lithium metal anode. United States. https://doi.org/10.1038/ncomms7362
Qian, Jiangfeng, Henderson, Wesley A., Xu, Wu, Bhattacharya, Priyanka, Engelhard, Mark H., Borodin, Oleg, and Zhang, Jiguang. 2015. "High rate and stable cycling of lithium metal anode". United States. https://doi.org/10.1038/ncomms7362. https://www.osti.gov/servlets/purl/1184948.
@article{osti_1184948,
title = {High rate and stable cycling of lithium metal anode},
author = {Qian, Jiangfeng and Henderson, Wesley A. and Xu, Wu and Bhattacharya, Priyanka and Engelhard, Mark H. and Borodin, Oleg and Zhang, Jiguang},
abstractNote = {Lithium (Li) metal is an ideal anode material for rechargeable batteries. However, dendritic Li growth and limited Coulombic efficiency (CE) during repeated Li deposition/stripping processes have prevented the application of this anode in rechargeable Li metal batteries, especially for use at high current densities. Here, we report that the use of highly concentrated electrolytes composed of ether solvents and the lithium bis(fluorosulfonyl)imide (LiFSI) salt enables the high rate cycling of a Li metal anode at high CE (up to 99.1 %) without dendrite growth. With 4 M LiFSI in 1,2-dimethoxyethane (DME) as the electrolyte, a Li|Li cell can be cycled at high rates (10 mA cm-2) for more than 6000 cycles with no increase in the cell impedance, and a Cu|Li cell can be cycled at 4 mA cm-2 for more than 1000 cycles with an average CE of 98.4%. These excellent high rate performances can be attributed to the increased solvent coordination and increased availability of Li+ concentration in the electrolyte. Lastly, further development of this electrolyte may lead to practical applications for Li metal anode in rechargeable batteries. The fundamental mechanisms behind the high rate ion exchange and stability of the electrolytes also shine light on the stability of other electrochemical systems.},
doi = {10.1038/ncomms7362},
url = {https://www.osti.gov/biblio/1184948}, journal = {Nature Communications},
issn = {2041-1723},
number = ,
volume = 6,
place = {United States},
year = {Fri Feb 20 00:00:00 EST 2015},
month = {Fri Feb 20 00:00:00 EST 2015}
}

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journal, January 2018


Processing of Advanced Battery Materials—Laser Cutting of Pure Lithium Metal Foils
journal, August 2018


Accurate Determination of Coulombic Efficiency for Lithium Metal Anodes and Lithium Metal Batteries
journal, October 2017


Ultrathin Bilayer of Graphite/SiO 2 as Solid Interface for Reviving Li Metal Anode
journal, August 2019


Electroless Formation of Hybrid Lithium Anodes for Fast Interfacial Ion Transport
journal, September 2017


Stable Conversion Chemistry-Based Lithium Metal Batteries Enabled by Hierarchical Multifunctional Polymer Electrolytes with Near-Single Ion Conduction
journal, March 2019


Growth of conformal graphene cages on micrometre-sized silicon particles as stable battery anodes
journal, January 2016


Advances and issues in developing salt-concentrated battery electrolytes
journal, March 2019


2D MoS2 as an efficient protective layer for lithium metal anodes in high-performance Li–S batteries
journal, February 2018


Suppressing the effect of lithium dendritic growth by the addition of magnesium bis(trifluoromethanesulfonyl)amide
journal, January 2018


“Solvent-in-salt” systems for design of new materials in chemistry, biology and energy research
journal, January 2018


A hybrid electrolyte for long-life semi-solid-state lithium sulfur batteries
journal, January 2017


A new ether-based electrolyte for lithium sulfur batteries using a S@pPAN cathode
journal, January 2018


Highly concentrated electrolyte solutions for 4 V class potassium-ion batteries
journal, January 2018


Applications of 2D MXenes in energy conversion and storage systems
journal, January 2019


Expanded-graphite embedded in lithium metal as dendrite-free anode of lithium metal batteries
journal, January 2019


Improving the Li–S battery performance by applying a combined interface engineering approach on the Li 2 S cathode
journal, January 2019


A new approach to very high lithium salt content quasi-solid state electrolytes for lithium metal batteries using plastic crystals
journal, January 2019


Composite lithium electrode with mesoscale skeleton via simple mechanical deformation
journal, March 2019


Graphitized Carbon Fibers as Multifunctional 3D Current Collectors for High Areal Capacity Li Anodes
journal, June 2017


High Areal Capacity and Lithium Utilization in Anodes Made of Covalently Connected Graphite Microtubes
journal, August 2017


High-Voltage Lithium-Metal Batteries Enabled by Localized High-Concentration Electrolytes
journal, March 2018


Suppressing Li Metal Dendrites Through a Solid Li‐Ion Backup Layer
journal, August 2018


Passivation of Lithium Metal Anode via Hybrid Ionic Liquid Electrolyte toward Stable Li Plating/Stripping
journal, November 2016


A Concentrated Ternary‐Salts Electrolyte for High Reversible Li Metal Battery with Slight Excess Li
journal, December 2018


Efficient Li‐Ion‐Conductive Layer for the Realization of Highly Stable High‐Voltage and High‐Capacity Lithium Metal Batteries
journal, February 2019


3D Nanowire Arrayed Cu Current Collector toward Homogeneous Alloying Anode Deposition for Enhanced Sodium Storage
journal, June 2019


Eliminating Dendrites through Dynamically Engineering the Forces Applied during Li Deposition for Stable Lithium Metal Anodes
journal, December 2019


Fluorine and Lithium: Ideal Partners for High‐Performance Rechargeable Battery Electrolytes
journal, November 2019


Cation−Solvent, Cation−Anion, and Solvent−Solvent Interactions with Electrolyte Solvation in Lithium batteries
journal, January 2019


Atomic Layer Deposition of Li x Al y S Solid-State Electrolytes for Stabilizing Lithium-Metal Anodes
journal, April 2016


Electrolytes for Batteries with Earth-Abundant Metal Anodes
journal, November 2018


Effect of Cation Size on Solvation and Association with Superoxide Anion in Aprotic Solvents
journal, July 2019


An Electrolyte for Reversible Cycling of Sodium Metal and Intercalation Compounds
journal, December 2016


Electrode Edge Effects and the Failure Mechanism of Lithium-Metal Batteries
journal, October 2018


Fast Charging Lithium Batteries: Recent Progress and Future Prospects
journal, March 2019


Selective deposition and stable encapsulation of lithium through heterogeneous seeded growth
journal, February 2016


A facile surface chemistry route to a stabilized lithium metal anode
journal, July 2017


A lithium-ion oxygen battery with a Si anode lithiated in situ by a Li 3 N-containing cathode
journal, January 2018


Elucidating electrolyte decomposition under electron-rich environments at the lithium-metal anode
journal, January 2017


Monolayer InP 3 as a reversible anode material for ultrafast charging lithium- and sodium-ion batteries: a theoretical study
journal, January 2018


Water-tolerant lithium metal cycling in high lithium concentration phosphonium-based ionic liquid electrolytes
journal, January 2018


First principles studies of self-diffusion processes on metallic lithium surfaces
journal, January 2019


Liquid Structures and Transport Properties of Lithium Bis(fluorosulfonyl)amide/Glyme Solvate Ionic Liquids for Lithium Batteries
journal, January 2019


High-capacity rechargeable batteries based on deeply cyclable lithium metal anodes
journal, May 2018


In operando plasmonic monitoring of electrochemical evolution of lithium metal
journal, October 2018


The energy-storage frontier: Lithium-ion batteries and beyond
journal, November 2015


Magnetic Field–Suppressed Lithium Dendrite Growth for Stable Lithium‐Metal Batteries
journal, April 2019


Suppressing Lithium Dendrite Growth via Sinusoidal Ripple Current Produced by Triboelectric Nanogenerators
journal, April 2019


Ein Hybrid‐Anion für ionische Flüssigkeiten und Batterieelektrolytanwendungen: Halb Triflamid, halb Carbonat
journal, February 2019


High‐Energy Rechargeable Metallic Lithium Battery at −70 °C Enabled by a Cosolvent Electrolyte
journal, March 2019


Self‐Healable Solid Polymeric Electrolytes for Stable and Flexible Lithium Metal Batteries
journal, December 2019


Electrolytes for Dual‐Carbon Batteries
journal, March 2019


High-Performance Anode Materials for Rechargeable Lithium-Ion Batteries
journal, March 2018


Pathways for practical high-energy long-cycling lithium metal batteries
journal, February 2019


The Impact of Li Grain Size on Coulombic Efficiency in Li Batteries
journal, October 2016


High-voltage positive electrode materials for lithium-ion batteries
journal, January 2017


Recent advances in inorganic 2D materials and their applications in lithium and sodium batteries
journal, January 2017


Suppression of dendritic lithium growth in lithium metal-based batteries
journal, January 2018


Bisalt ether electrolytes: a pathway towards lithium metal batteries with Ni-rich cathodes
journal, January 2019


A graphite intercalation compound associated with liquid Na–K towards ultra-stable and high-capacity alkali metal anodes
journal, January 2019


Review—Li Metal Anode in Working Lithium-Sulfur Batteries
journal, June 2017


Solid Electrolyte Interphase Film on Lithium Metal Anode in Mixed-Salt System
journal, January 2019


Deterioration Analysis of Lithium Metal Anode in Full Cell during Long-Term Cycles
journal, January 2019


Rechargeable Mg–Li hybrid batteries: status and challenges
journal, September 2016


Mg Doped Li–LiB Alloy with In Situ Formed Lithiophilic LiB Skeleton for Lithium Metal Batteries
journal, March 2020


A Highly Reversible Room-Temperature Sodium Metal Anode
journal, November 2015


Dendrites and Pits: Untangling the Complex Behavior of Lithium Metal Anodes through Operando Video Microscopy
journal, October 2016


High-Purity Lithium Metal Films from Aqueous Mineral Solutions
journal, January 2018


A reversible dendrite-free high-areal-capacity lithium metal electrode
journal, April 2017


Accommodating lithium into 3D current collectors with a submicron skeleton towards long-life lithium metal anodes
journal, August 2015


Designing solid-liquid interphases for sodium batteries
journal, October 2017


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


High-energy-density dual-ion battery for stationary storage of electricity using concentrated potassium fluorosulfonylimide
journal, October 2018


Achieving three-dimensional lithium sulfide growth in lithium-sulfur batteries using high-donor-number anions
journal, January 2019


Publisher Correction: Aligning academia and industry for unified battery performance metrics
journal, January 2019


Stabilizing polymer electrolytes in high-voltage lithium batteries
journal, July 2019


A new ether-based electrolyte for dendrite-free lithium-metal based rechargeable batteries
journal, February 2016


Towards high energy density lithium battery anodes: silicon and lithium
journal, January 2019


Composite lithium electrode with mesoscale skeleton via simple mechanical deformation
journal, March 2019


Fluorinated solid electrolyte interphase enables highly reversible solid-state Li metal battery
journal, December 2018


Concentrated LiODFB Electrolyte for Lithium Metal Batteries
journal, July 2019


Lithiophilic Silver Coating on Lithium Metal Surface for Inhibiting Lithium Dendrites
journal, February 2020