DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Nanoscale Mapping of Extrinsic Interfaces in Hybrid Solid Electrolytes

Journal Article · · Joule

Inorganic-organic hybrid solid electrolytes are promising material systems for all solid-state batteries (ASSBs). These electrolytes contain numerous solidsolid interfaces that govern transport pathways, electrodeelectrolyte compatibility, and durability. This paper evaluates the role that electrodeelectrolyte interfaces and electrolyte structure have on electrochemical performance. Atomic force microscopy techniques reveal how mechanical, adhesion, and morphological properties transform in a series of model hybrid solid electrolytes. These measurements are mapped to sub-surface microstructural features using synchrotron nano-tomography. Hybrid solid electrolytes with shorter polymer chains demonstrate a higher adhesion (100 nN), Young’s Modulus (6.4 GPa), capacity (114.6 mAh/g), and capacity retention (92.9%) than hybrid electrolytes with longer polymer chains (i.e., higher molecular weight). Extrinsic interfacial properties largely dictate electrochemical performance in ASSBs. Finally, microstructural control over inorganic constituents may provide a means for tailoring interfacial properties in hybrid solid electrolytes.

Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS); Energy Frontier Research Centers (EFRC) (United States). Fluid Interface Reactions, Structures and Transport Center (FIRST); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Organization:
National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Grant/Contract Number:
AC02-06CH11357; AC05-00OR22725
OSTI ID:
1608206
Journal Information:
Joule, Journal Name: Joule Journal Issue: 1 Vol. 4; ISSN 2542-4351
Publisher:
Elsevier - Cell PressCopyright Statement
Country of Publication:
United States
Language:
English

References (51)

Analysis of Strain and Stress in Ceramic, Polymer and Metal Matrix Composites by Raman Spectroscopy journal August 2002
Low Resistance-Integrated All-Solid-State Battery Achieved by Li 7 La 3 Zr 2 O 12 Nanowire Upgrading Polyethylene Oxide (PEO) Composite Electrolyte and PEO Cathode Binder journal October 2018
Lithium Ion Pathway within Li 7 La 3 Zr 2 O 12 -Polyethylene Oxide Composite Electrolytes journal September 2016
Recent Progress of Hybrid Solid‐State Electrolytes for Lithium Batteries journal June 2018
Direct Observation of the Growth of Lithium Dendrites on Graphite Anodes by Operando EC-AFM journal December 2017
Effective medium theory in studies of conductivity of composite polymeric electrolytes journal October 1995
Polymer-ceramic composite electrolytes journal December 1994
Role of the ceramic fillers in enhancing the transport properties of composite polymer electrolytes journal May 2001
Modulation of solid electrolyte interphase of lithium-ion batteries by LiDFOB and LiBOB electrolyte additives journal May 2018
Screening polyethylene oxide-based composite polymer electrolytes via combining effective medium theory and Halpin-Tsai model journal March 2018
LiNbO3-coated LiCoO2 as cathode material for all solid-state lithium secondary batteries journal July 2007
Direct observation of lithium dendrites inside garnet-type lithium-ion solid electrolyte journal August 2015
Dendrite short-circuit and fuse effect on Li/polymer/Li cells journal July 2006
Solid polymer electrolytes incorporating cubic Li7La3Zr2O12 for all-solid-state lithium rechargeable batteries journal December 2017
Interfaces in Solid-State Lithium Batteries journal October 2018
Enhancement of ionic conductivity of composite membranes for all-solid-state lithium rechargeable batteries incorporating tetragonal Li7La3Zr2O12 into a polyethylene oxide matrix journal January 2015
All-solid-state lithium-ion and lithium metal batteries – paving the way to large-scale production journal April 2018
Facile and scalable fabrication of polymer-ceramic composite electrolyte with high ceramic loadings journal June 2018
Hybrid electrolytes for lithium metal batteries journal July 2018
Characterization of the morphology of primary silicon particles using synchrotron X-ray tomography journal January 2017
Composite solid electrolytes for all-solid-state lithium batteries journal April 2019
Nanoscale silicon as anode for Li-ion batteries: The fundamentals, promises, and challenges journal October 2015
PEO/garnet composite electrolytes for solid-state lithium batteries: From “ceramic-in-polymer” to “polymer-in-ceramic” journal April 2018
Comparison of nanoindentation and AFM methods for the determination of mechanical properties of polymers journal May 2013
Ion-conductivity and Young's modulus of the polymer electrolyte PEO–ammonium perchlorate journal February 2007
Microstructure and temperature dependent lithium ion transport of ceramic–polymer composite electrolyte for solid-state lithium ion batteries based on garnet-type Li7La3Zr2O12 journal August 2016
Elastic Properties of the Solid Electrolyte Li 7 La 3 Zr 2 O 12 (LLZO) journal December 2015
Lithium Ion Conducting Poly(ethylene oxide)-Based Solid Electrolytes Containing Active or Passive Ceramic Nanoparticles journal January 2017
In Situ STEM-EELS Observation of Nanoscale Interfacial Phenomena in All-Solid-State Batteries journal May 2016
In Situ AFM Imaging of Solid Electrolyte Interfaces on HOPG with Ethylene Carbonate and Fluoroethylene Carbonate-Based Electrolytes journal November 2015
Investigation of the Interaction between Nafion Ionomer and Surface Functionalized Carbon Black Using Both Ultrasmall Angle X-ray Scattering and Cryo-TEM journal February 2017
Suppression of Lithium Dendrite Formation by Using LAGP-PEO (LiTFSI) Composite Solid Electrolyte and Lithium Metal Anode Modified by PEO (LiTFSI) in All-Solid-State Lithium Batteries journal April 2017
Composite Polymer Electrolytes with Li 7 La 3 Zr 2 O 12 Garnet-Type Nanowires as Ceramic Fillers: Mechanism of Conductivity Enhancement and Role of Doping and Morphology journal June 2017
New Insights into the Compositional Dependence of Li-Ion Transport in Polymer–Ceramic Composite Electrolytes journal January 2018
Tortuosity Effects in Garnet-Type Li 7 La 3 Zr 2 O 12 Solid Electrolytes journal December 2018
Effect of Pore Connectivity on Li Dendrite Propagation within LLZO Electrolytes Observed with Synchrotron X-ray Tomography journal March 2018
Tandem Interface and Bulk Li-Ion Transport in a Hybrid Solid Electrolyte with Microsized Active Filler journal August 2019
Synergistic Coupling between Li 6.75 La 3 Zr 1.75 Ta 0.25 O 12 and Poly(vinylidene fluoride) Induces High Ionic Conductivity, Mechanical Strength, and Thermal Stability of Solid Composite Electrolytes journal September 2017
Nanocomposite polymer electrolytes for lithium batteries journal July 1998
Cryo-STEM mapping of solid–liquid interfaces and dendrites in lithium-metal batteries journal August 2018
Li-ion transport in a representative ceramic–polymer–plasticizer composite electrolyte: Li 7 La 3 Zr 2 O 12 –polyethylene oxide–tetraethylene glycol dimethyl ether journal January 2017
Understanding inks for porous-electrode formation journal January 2017
Visualizing percolation and ion transport in hybrid solid electrolytes for Li–metal batteries journal January 2019
The use of the PeakForce TM quantitative nanomechanical mapping AFM-based method for high-resolution Young's modulus measurement of polymers journal October 2011
TomoPy: a framework for the analysis of synchrotron tomographic data journal August 2014
Nanoscale 3D imaging at the Advanced Photon Source journal May 2016
Compatibility of Lithium Ion Conductive Sulfide Glass with Carbon-Lithium Electrode journal January 2003
The Impact of Elastic Deformation on Deposition Kinetics at Lithium/Polymer Interfaces journal January 2005
Resolution of the Modulus versus Adhesion Dilemma in Solid Polymer Electrolytes for Rechargeable Lithium Metal Batteries journal January 2012
Evaluating the Effects of Temperature and Pressure on Li/PEO-LiTFSI Interfacial Stability and Kinetics journal January 2018
Effects of Electrolyte Additives and Solvents on Unwanted Lithium Plating in Lithium-Ion Cells journal January 2017