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Title: Solubility-mediated sustained release enabling nitrate additive in carbonate electrolytes for stable lithium metal anode

Journal Article · · Nature Communications

Here, the physiochemical properties of the solid-electrolyte interphase, primarily governed by electrolyte composition, have a profound impact on the electrochemical cycling of metallic lithium. Herein, we discover that the effect of nitrate anions on regulating lithium deposition previously known in ether-based electrolytes can be extended to carbonate-based systems, which dramatically alters the nuclei from dendritic to spherical, albeit extremely limited solubility. This is attributed to the preferential reduction of nitrate during solid-electrolyte interphase formation, and the mechanisms behind which are investigated based on the structure, ion-transport properties, and charge transfer kinetics of the modified interfacial environment. To overcome the solubility barrier, a solubility-mediated sustained-release methodology is introduced, in which nitrate nanoparticles are encapsulated in porous polymer gel and can be steadily dissolved during battery operation to maintain a high concentration at the electroplating front. As such, effective dendrite suppression and remarkably enhanced cycling stability are achieved in corrosive carbonate electrolytes.

Research Organization:
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Sponsoring Organization:
USDOE
Grant/Contract Number:
AC02-76SF00515
OSTI ID:
1475484
Journal Information:
Nature Communications, Vol. 9, Issue 1; ISSN 2041-1723
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 267 works
Citation information provided by
Web of Science

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A Molecular‐Cage Strategy Enabling Efficient Chemisorption–Electrocatalytic Interface in Nanostructured Li 2 S Cathode for Li Metal‐Free Rechargeable Cells with High Energy journal September 2019
Horizontal Growth of Lithium on Parallelly Aligned MXene Layers towards Dendrite‐Free Metallic Lithium Anodes journal June 2019
A Concentrated Ternary‐Salts Electrolyte for High Reversible Li Metal Battery with Slight Excess Li journal December 2018
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
Artificial Solid‐Electrolyte Interphase Enabled High‐Capacity and Stable Cycling Potassium Metal Batteries journal September 2019
A Sustainable Solid Electrolyte Interphase for High‐Energy‐Density Lithium Metal Batteries Under Practical Conditions journal January 2020
Enabling High‐Voltage Lithium Metal Batteries by Manipulating Solvation Structure in Ester Electrolyte journal January 2020
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A compact inorganic layer for robust anode protection in lithium‐sulfur batteries journal November 2019
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In situ fluorinated solid electrolyte interphase towards long-life lithium metal anodes journal January 2020
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Biomacromolecules enabled dendrite-free lithium metal battery and its origin revealed by cryo-electron microscopy journal January 2020
Challenges and opportunities towards fast-charging battery materials journal June 2019
3D hollow reduced graphene oxide foam as a stable host for high-capacity lithium metal anodes journal January 2019
Uniform lithium deposition on N-doped carbon-coated current collectors journal January 2019
Polar polymer–solvent interaction derived favorable interphase for stable lithium metal batteries journal January 2019
Film-forming electrolyte additives for rechargeable lithium-ion batteries: progress and outlook journal January 2019
A dual-phase Li–Ca alloy with a patternable and lithiophilic 3D framework for improving lithium anode performance journal January 2019
Separator-free and concentrated LiNO 3 electrolyte cells enable uniform lithium electrodeposition journal January 2020
A Versatile Halide Ester Enabling Li-Anode Stability and a High Rate Capability in Lithium-Oxygen Batteries journal January 2019
Enabling High‐Voltage Lithium Metal Batteries by Manipulating Solvation Structure in Ester Electrolyte journal January 2020
Innenrücktitelbild: A Sustainable Solid Electrolyte Interphase for High‐Energy‐Density Lithium Metal Batteries Under Practical Conditions (Angew. Chem. 8/2020) journal January 2020
Inside Back Cover: A Sustainable Solid Electrolyte Interphase for High‐Energy‐Density Lithium Metal Batteries Under Practical Conditions (Angew. Chem. Int. Ed. 8/2020) journal February 2020
Cation−Solvent, Cation−Anion, and Solvent−Solvent Interactions with Electrolyte Solvation in Lithium batteries journal January 2019
Nonflammable Lithium Metal Full Cells with Ultra-high Energy Density Based on Coordinated Carbonate Electrolytes journal February 2020
An ultrastable lithium metal anode enabled by designed metal fluoride spansules journal March 2020