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Title: Continuous plating/stripping behavior of solid-state lithium metal anode in a 3D ion-conductive framework

Journal Article · · Proceedings of the National Academy of Sciences of the United States of America
 [1];  [1];  [2];  [2];  [2];  [2];  [2];  [2];  [2];  [2];  [2]
  1. Univ. of Maryland, College Park, MD (United States); The Pennsylvania State Univ., University Park, PA (United States)
  2. Univ. of Maryland, College Park, MD (United States)

The increasing demands for efficient and clean energy-storage systems have spurred the development of Li metal batteries, which possess attractively high energy densities. For practical application of Li metal batteries, it is vital to resolve the intrinsic problems of Li metal anodes, i.e., the formation of Li dendrites, interfacial instability, and huge volume changes during cycling. Utilization of solid-state electrolytes for Li metal anodes is a promising approach to address those issues. In this study, we use a 3D garnet-type ion-conductive framework as a host for the Li metal anode and study the plating and stripping behaviors of the Li metal anode within the solid ion-conductive host. We show that with a solid-state ion-conductive framework and a planar current collector at the bottom, Li is plated from the bottom and rises during deposition, away from the separator layer and free from electrolyte penetration and short circuit. Owing to the solid-state deposition property, Li grows smoothly in the pores of the garnet host without forming Li dendrites. The dendrite-free deposition and continuous rise/fall of Li metal during plating/stripping in the 3D ion-conductive host promise a safe and durable Li metal anode. Here, the solid-state Li anode shows stable cycling at 0.5 mA cm–2 for 300 h with a small overpotential, showing a significant improvement compared with reported Li anodes with ceramic electrolytes. By fundamentally eliminating the dendrite issue, the solid Li metal anode shows a great potential to build safe and reliable Li metal batteries.

Research Organization:
Univ. of Maryland, College Park, MD (United States)
Sponsoring Organization:
USDOE Advanced Research Projects Agency - Energy (ARPA-E)
Grant/Contract Number:
AR0000384; EE0006860
OSTI ID:
1429586
Alternate ID(s):
OSTI ID: 1540277
Journal Information:
Proceedings of the National Academy of Sciences of the United States of America, Vol. 115, Issue 15; ISSN 0027-8424
Publisher:
National Academy of SciencesCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 221 works
Citation information provided by
Web of Science

References (40)

Negating interfacial impedance in garnet-based solid-state Li metal batteries journal December 2016
Interface-Engineered All-Solid-State Li-Ion Batteries Based on Garnet-Type Fast Li + Conductors journal July 2016
Solid-State Lithium Metal Batteries Promoted by Nanotechnology: Progress and Prospects journal May 2017
Origin of Outstanding Stability in the Lithium Solid Electrolyte Materials: Insights from Thermodynamic Analyses Based on First-Principles Calculations journal October 2015
Three-dimensional stable lithium metal anode with nanoscale lithium islands embedded in ionically conductive solid matrix journal April 2017
A solid future for battery development journal September 2016
Li 7 La 3 Zr 2 O 12 Interface Modification for Li Dendrite Prevention journal April 2016
An Artificial Solid Electrolyte Interphase Layer for Stable Lithium Metal Anodes journal December 2015
Reviving the lithium metal anode for high-energy batteries journal March 2017
Composite lithium metal anode by melt infusion of lithium into a 3D conducting scaffold with lithiophilic coating journal February 2016
Next-Generation Lithium Metal Anode Engineering via Atomic Layer Deposition journal May 2015
Mastering the interface for advanced all-solid-state lithium rechargeable batteries journal November 2016
Conformal, Nanoscale ZnO Surface Modification of Garnet-Based Solid-State Electrolyte for Lithium Metal Anodes journal December 2016
Accommodating lithium into 3D current collectors with a submicron skeleton towards long-life lithium metal anodes journal August 2015
Poly(dimethylsiloxane) Thin Film as a Stable Interfacial Layer for High-Performance Lithium-Metal Battery Anodes journal October 2016
Three-dimensional bilayer garnet solid electrolyte based high energy density lithium metal–sulfur batteries journal January 2017
Metallic anodes for next generation secondary batteries journal January 2013
Dendrite-Free Lithium Deposition via Self-Healing Electrostatic Shield Mechanism journal March 2013
Transition from Superlithiophobicity to Superlithiophilicity of Garnet Solid-State Electrolyte journal September 2016
Protected Lithium-Metal Anodes in Batteries: From Liquid to Solid journal July 2017
Toward Safe Lithium Metal Anode in Rechargeable Batteries: A Review journal July 2017
Garnet-type solid-state fast Li ion conductors for Li batteries: critical review journal January 2014
Lithium Metal Anodes: Toward an Improved Understanding of Coupled Morphological, Electrochemical, and Mechanical Behavior journal February 2017
A new class of Solvent-in-Salt electrolyte for high-energy rechargeable metallic lithium batteries journal February 2013
Interface Stability in Solid-State Batteries journal December 2015
Surface Chemistry Mechanism of Ultra-Low Interfacial Resistance in the Solid-State Electrolyte Li 7 La 3 Zr 2 O 12 journal September 2017
Li–O2 and Li–S batteries with high energy storage journal January 2012
Lithium metal anodes for rechargeable batteries journal January 2014
Advanced Micro/Nanostructures for Lithium Metal Anodes journal February 2017
Interconnected hollow carbon nanospheres for stable lithium metal anodes journal July 2014
Direct observation of lithium dendrites inside garnet-type lithium-ion solid electrolyte journal August 2015
A Review of Solid Electrolyte Interphases on Lithium Metal Anode journal November 2015
Lithium battery chemistries enabled by solid-state electrolytes journal February 2017
Toward garnet electrolyte–based Li metal batteries: An ultrathin, highly effective, artificial solid-state electrolyte/metallic Li interface journal April 2017
Stable lithium electrodeposition in liquid and nanoporous solid electrolytes journal August 2014
Plating a Dendrite-Free Lithium Anode with a Polymer/Ceramic/Polymer Sandwich Electrolyte journal July 2016
Interface behavior between garnet-type lithium-conducting solid electrolyte and lithium metal journal September 2014
Fast Lithium Ion Conduction in Garnet-Type Li7La3Zr2O12 journal October 2007
Fast Lithium Ion Conduction in Garnet-Type Li7La3Zr2O12. journal December 2007
Stable Lithium Electrodeposition in Liquid and Nanoporous Solid Electrolytes text January 2014

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Expanded-graphite embedded in lithium metal as dendrite-free anode of lithium metal batteries journal January 2019
Nano-Cu-embedded carbon for dendrite-free lithium metal anodes journal January 2019
Design of Porous Solid Electrolytes for Rechargeable Metal Batteries journal January 2018
Building Better Batteries in the Solid State: A Review journal November 2019
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Superlithiophilic Amorphous SiO 2 –TiO 2 Distributed into Porous Carbon Skeleton Enabling Uniform Lithium Deposition for Stable Lithium Metal Batteries journal July 2019
Nanoscaled Lithium Powders with Protection of Ionic Liquid for Highly Stable Rechargeable Lithium Metal Batteries journal October 2019
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