skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Understanding the Effect of Interlayers at the Thiophosphate Solid Electrolyte/Lithium Interface for All-Solid-State Li Batteries

Journal Article · · Chemistry of Materials
 [1];  [1];  [2]; ORCiD logo [3];  [3]; ORCiD logo [1]; ORCiD logo [3]; ORCiD logo [2];  [4]; ORCiD logo [1]
  1. Univ. of Illinois at Urbana-Champaign, Urbana, IL (United States)
  2. Northwestern Univ., Evanston, IL (United States)
  3. Argonne National Lab. (ANL), Lemont, IL (United States)
  4. Univ. of Illinois at Urbana-Champaign, Urbana, IL (United States); KTH Royal Institute of Technology, Stockholm (Sweden)
+ Show Author Affiliations

All-solid-state Li-ion batteries afford possibilities to enhance battery safety while improving their energy and power densities. Current challenges for achieving high-performance all-solid-state batteries with long cycle life include shorting resulting predominantly from Li dendrite formation and infiltration through the solid electrolyte (SE) and increases in cell impedance induced by SE decomposition at the SE/electrode interface. In this work, we evaluate the electrochemical properties of two interlayer materials, Si and LixAl(2-x/3)O3 (LiAlO), at the Li7P3S11 (LPS)/Li interface. Compared to the Li/LPS/Li symmetric cells in absence of interlayers, the presence of Si and LiAlO both significantly enhance the cycle number and total charge passing through the interface before failures resulting from cell shorting. In both cases, the noted improvements were accompanied by cell impedances that had increased substantially. The data reveal that both interlayers prevent the direct exposure of LPS to the metallic Li and therefore eliminate the intrinsic LPS decomposition that occurs at Li surfaces before electrochemical cycling. After cycling, a reduction of LPS to Li2S occurs at the interface when a Si interlayer is present; LiAlO, which functions to drop the potential between Li and LPS, suppresses LPS decomposition processes. The relative propensities toward SE decomposition follows from the electrochemical potentials at the interface, which are dictated by the identities of the interlayer materials. As a result, this work provides new insights into the phase dynamics associated with specific choices for SE/electrode interlayer materials and the requirements they impose for realizing high efficiency, long lasting all-solid-state batteries.

Research Organization:
Energy Frontier Research Centers (EFRC) (United States). Center for Electrical Energy Storage (CEES); Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
1500114
Journal Information:
Chemistry of Materials, Vol. 30, Issue 24; ISSN 0897-4756
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 60 works
Citation information provided by
Web of Science

References (48)

High-power all-solid-state batteries using sulfide superionic conductors journal March 2016
Promises, Challenges, and Recent Progress of Inorganic Solid-State Electrolytes for All-Solid-State Lithium Batteries journal February 2018
A lithium superionic conductor journal July 2011
New, Highly Ion-Conductive Crystals Precipitated from Li2S-P2S5 Glasses journal April 2005
A sulphide lithium super ion conductor is superior to liquid ion conductors for use in rechargeable batteries journal January 2014
Air-stable, high-conduction solid electrolytes of arsenic-substituted Li 4 SnS 4 journal January 2014
A synthesis of crystalline Li7P3S11 solid electrolyte from 1,2-dimethoxyethane solvent journal December 2014
Atomic Layer Deposition of the Solid Electrolyte LiPON journal July 2015
Anomalous High Ionic Conductivity of Nanoporous β-Li3PS4 journal January 2013
Inorganic Solid-State Electrolytes for Lithium Batteries: Mechanisms and Properties Governing Ion Conduction journal December 2015
The Effect of Interfacial Deformation on Electrodeposition Kinetics journal January 2004
The Impact of Elastic Deformation on Deposition Kinetics at Lithium/Polymer Interfaces journal January 2005
Mechanism of Lithium Metal Penetration through Inorganic Solid Electrolytes journal July 2017
Modeling of internal mechanical failure of all-solid-state batteries during electrochemical cycling, and implications for battery design journal January 2017
Characterizing the Li–Li7La3Zr2O12 interface stability and kinetics as a function of temperature and current density journal January 2016
Interface Stability in Solid-State Batteries journal December 2015
Direct Observation of the Interfacial Instability of the Fast Ionic Conductor Li 10 GeP 2 S 12 at the Lithium Metal Anode journal March 2016
Interphase formation and degradation of charge transfer kinetics between a lithium metal anode and highly crystalline Li7P3S11 solid electrolyte journal March 2016
Evolution at the Solid Electrolyte/Gold Electrode Interface during Lithium Deposition and Stripping journal March 2017
Toward garnet electrolyte–based Li metal batteries: An ultrathin, highly effective, artificial solid-state electrolyte/metallic Li interface journal April 2017
Negating interfacial impedance in garnet-based solid-state Li metal batteries journal December 2016
Garnet Solid Electrolyte Protected Li-Metal Batteries journal May 2017
Transition from Superlithiophobicity to Superlithiophilicity of Garnet Solid-State Electrolyte journal September 2016
Interface Re-Engineering of Li 10 GeP 2 S 12 Electrolyte and Lithium anode for All-Solid-State Lithium Batteries with Ultralong Cycle Life journal January 2018
Stabilizing Li 10 SnP 2 S 12 /Li Interface via an in Situ Formed Solid Electrolyte Interphase Layer journal July 2018
XPS and SEM analysis between Li/Li3PS4 interface with Au thin film for all-solid-state lithium batteries journal September 2018
Lithium metal protected by atomic layer deposition metal oxide for high performance anodes journal January 2017
Ultrathin Lithium-Ion Conducting Coatings for Increased Interfacial Stability in High Voltage Lithium-Ion Batteries journal May 2014
Inductive Loop in the Impedance Response of Perovskite Solar Cells Explained by Surface Polarization Model journal March 2017
The effect of atomic hydrogen on the anodic dissolution of iron in a sulfate electrolyte studied with impedance spectroscopy journal November 2008
Impedance Spectra of Energy-Storage Electrodes Obtained with Commercial Three-Electrode Cells: Some Sources of Measurement Artefacts journal December 2014
Myth and Reality about the Origin of Inductive Loops in Impedance Spectra of Lithium-Ion Electrodes — A Critical Experimental Approach journal July 2016
Analysis of the structure and degree of crystallisation of 70Li 2 S–30P 2 S 5 glass ceramic journal January 2015
Single-Crystal Silicon Membranes with High Lithium Conductivity and Application in Lithium-Air Batteries journal September 2011
Redox activity of argyrodite Li6PS5Cl electrolyte in all-solid-state Li-ion battery: An XPS study journal February 2017
Interface Stability of Argyrodite Li 6 PS 5 Cl toward LiCoO 2 , LiNi 1/3 Co 1/3 Mn 1/3 O 2 , and LiMn 2 O 4 in Bulk All-Solid-State Batteries journal April 2017
Redox-active cathode interphases in solid-state batteries journal January 2017
Structural and electronic features of binary Li2S-P2S5 glasses journal February 2016
Instantaneous preparation of high lithium-ion conducting sulfide solid electrolyte Li 7 P 3 S 11 by a liquid phase process journal January 2017
Infrared, Raman, resonance Raman spectra and lattice dynamics calculations of the solid potassium(I) nickel(II) thiophosphate compound, KNiPS4 journal June 1995
Infrared, Raman and resonance Raman spectra and lattice dynamics calculations of the solid potassium(I) palladium(II) thiophosphate compound KPdPS4 journal August 1999
Infrared, Raman and resonance Raman spectra of the solid nickel(II) thiophosphate compound (PPh4)3 [(NiPS4)3] and force constants in the trinickel [Ni3P3S12]3− cyclic anion journal December 1999
Ionic conductivity of and phase transition in lithium thiophosphate Li3PS4 journal November 1984
Darstellung, Schwingungsspektrum und Normalkoordinatenanalyse des Gold-ortho-Thiophosphates, AuPS4 journal June 1986
Lithium ion conducting solid electrolytes prepared from Li2S, elemental P and S journal October 2006
A structural, spectroscopic and electrochemical study of a lithium ion conducting Li10GeP2S12 solid electrolyte journal May 2013
Palladium Chemistry in Molten Alkali Metal Polychalcophosphate Fluxes. Synthesis and Characterization of K 4 Pd(PS 4 ) 2 , Cs 4 Pd(PSe 4 ) 2 , Cs 10 Pd(PSe 4 ) 4 , KPdPS 4 , K 2 PdP 2 S 6 , and Cs 2 PdP 2 Se 6 journal December 1997
(PPh3-C3H6-PPh3)0.5[NiPS4] and (PPh3-C2H2-PPh3)0.5[NiPS4]: Two new compounds containing [NiPS4]? chains journal January 2003

Cited By (5)

Sulfide‐Based Solid‐State Electrolytes: Synthesis, Stability, and Potential for All‐Solid‐State Batteries journal August 2019
Incorporating Solvate and Solid Electrolytes for All‐Solid‐State Li 2 S Batteries with High Capacity and Long Cycle Life journal May 2019
Unraveling the Intra and Intercycle Interfacial Evolution of Li 6 PS 5 Cl‐Based All‐Solid‐State Lithium Batteries journal December 2019
Understanding interface stability in solid-state batteries journal December 2019
Cyclic utilisation of waste tires as nanostructured anode materials for Li-ion batteries journal January 2020

Similar Records

Related Subjects

25 ENERGY STORAGE