Skip to main content
U.S. Department of Energy
Office of Scientific and Technical Information

Microscopic Observation of Solid Electrolyte Interphase Bilayer Inversion on Silicon Oxide

Journal Article · · ACS Energy Letters
Silicon has been investigated in recent years as an alloying anode material to enhance gravimetric energy density in lithium-ion batteries. Although recent developments have suggested that silicon oxides exhibit improved cycling stability over pure Si, the origin of the improved cycling performance is still poorly understood. The initial solid electrolyte interphase (SEI) formation mechanisms on Si wafers with both native oxide and chemically etched thermal oxide coatings are investigated structurally, chemically, and morphologically in the nanoscale. After one electrochemical cycle, microscopy reveals that SEI formed on native SiOx features the typical SEI bilayer structure with a carbon-rich outer SEI layer and an inorganic-rich inner SEI layer. In contrast, the SEI formed on chemically etched thermal oxide shows an inversion in the structure. This work observes distinct initial SEI formation mechanisms on the HF-etched SiO2 surface, which may be partially responsible for improved cycle life observed in SiOx-based anode materials.
Research Organization:
National Renewable Energy Laboratory (NREL), Golden, CO (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office
Grant/Contract Number:
AC36-08GO28308
OSTI ID:
1721751
Report Number(s):
NREL/JA--5K00-77261; MainId:26207; UUID:1cfcfec0-4728-40e7-9bc2-bdcb4672f139; MainAdminID:18843
Journal Information:
ACS Energy Letters, Journal Name: ACS Energy Letters Journal Issue: 12 Vol. 5; ISSN 2380-8195
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English

References (35)

In Situ Measurement of Solid Electrolyte Interphase Evolution on Silicon Anodes Using Atomic Force Microscopy journal April 2016
Electrochemical performance of thermally-grown SiO2 as diffusion barrier layer for integrated lithium-ion batteries journal April 2018
Calendar-life versus cycle-life aging of lithium-ion cells with silicon-graphite composite electrodes journal August 2018
Electrochemical behavior of SiO anode for Li secondary batteries journal October 2011
Solid Electrolyte Interphase on Native Oxide-Terminated Silicon Anodes for Li-Ion Batteries journal March 2019
A review of the electrochemical performance of alloy anodes for lithium-ion batteries journal January 2011
Quantifying capacity loss due to solid-electrolyte-interphase layer formation on silicon negative electrodes in lithium-ion batteries journal October 2012
Evolution of solid electrolyte interphase and active material in the silicon wafer model system journal January 2021
Dynamic Structure and Chemistry of the Silicon Solid-Electrolyte Interphase Visualized by Cryogenic Electron Microscopy journal November 2019
Three-dimensional electronic resistivity mapping of solid electrolyte interphase on Si anode materials journal January 2019
The Effect of Fluoroethylene Carbonate as an Additive on the Solid Electrolyte Interphase on Silicon Lithium-Ion Electrodes journal August 2015
Facile and Efficient Synthesis of a Microsized SiO x /C Core–Shell Composite as Anode Material for Lithium Ion Batteries journal July 2017
Chemistry of Electrolyte Reduction on Lithium Silicide journal May 2019
Vertical Graphene Growth on SiO Microparticles for Stable Lithium Ion Battery Anodes journal May 2017
Enhanced Interfacial Stability of Si Anodes for Li-Ion Batteries via Surface SiO 2 Coating journal August 2020
Surface SiO 2 Thickness Controls Uniform-to-Localized Transition in Lithiation of Silicon Anodes for Lithium-Ion Batteries journal May 2020
Operando Electrochemical Atomic Force Microscopy of Solid–Electrolyte Interphase Formation on Graphite Anodes: The Evolution of SEI Morphology and Mechanical Properties journal July 2020
Hard X-ray Photoelectron Spectroscopy (HAXPES) Investigation of the Silicon Solid Electrolyte Interphase (SEI) in Lithium-Ion Batteries journal August 2015
Mechanical Properties and Chemical Reactivity of Li x SiO y Thin Films journal October 2018
Beyond Doping and Coating: Prospective Strategies for Stable High-Capacity Layered Ni-Rich Cathodes journal March 2020
Emerging Opportunities for Two-Dimensional Materials in Lithium-Ion Batteries journal August 2017
25.1%-Efficient Monolithic Perovskite/Silicon Tandem Solar Cell Based on a p -type Monocrystalline Textured Silicon Wafer and High-Temperature Passivating Contacts journal March 2019
Temperature-Dependent Solubility of Solid Electrolyte Interphase on Silicon Electrodes journal October 2019
Electron-Rich Driven Electrochemical Solid-State Amorphization in Li–Si Alloys journal August 2013
Lithiation of SiO 2 in Li-Ion Batteries: In Situ Transmission Electron Microscopy Experiments and Theoretical Studies journal November 2014
Determination of the Solid Electrolyte Interphase Structure Grown on a Silicon Electrode Using a Fluoroethylene Carbonate Additive journal July 2017
Silicon oxides: a promising family of anode materials for lithium-ion batteries journal January 2019
Silicon: toward eco-friendly reduction techniques for lithium-ion battery applications journal January 2019
Atomic structure of sensitive battery materials and interfaces revealed by cryo–electron microscopy journal October 2017
Structural Analysis of Pure and Electrochemically Lithiated SiO Using Neutron Elastic Scattering journal January 2004
Analysis of SiO Anodes for Lithium-Ion Batteries journal January 2005
Capacity Fading Mechanism and Improvement of Cycling Stability of the SiO Anode for Lithium-Ion Batteries journal January 2018
Calendar and Cycle Life of Lithium-Ion Batteries Containing Silicon Monoxide Anode journal January 2018
Correlation of Electrolyte Volume and Electrochemical Performance in Lithium-Ion Pouch Cells with Graphite Anodes and NMC532 Cathodes journal January 2017
Investigation of the irreversible reaction mechanism and the reactive trigger on SiO anode material for lithium-ion battery journal January 2011