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Robust Solid/Electrolyte Interphase (SEI) formation on Si Anodes Using Glyme-based Electrolytes

Journal Article · · ACS Energy Letters
 [1];  [2];  [3];  [1];  [1];  [4];  [5];  [2];  [6];  [2];  [7];  [1];  [1]
  1. Oak Ridge National Laboratory
  2. National Renewable Energy Laboratory
  3. University of Tennessee
  4. Idaho National Laboratory
  5. BATTELLE (PACIFIC NW LAB)
  6. National Energy Technology Laboratory
  7. Argonne National Laboratory

Silicon (Si) is the most naturally abundant element possessing 10-fold theoretical capacity than graphitebased anodes. The practicality of implementing Si anodes is, however limited by the unstable solidelectrolyte interphase (SEI) and anode fracturing during continuous lithiation/delithiation. We demonstrate that glyme-based electrolytes (GlyEls) assure a conformal SEI on Si and keep the Si ‘fracture-free’. Benchmarking against the optimal, commonly-used carbonate electrolyte with the fluoroethylene carbonate (FEC) additive, Si anode cycled in a GlyEl exhibits reduced early parasitic current (by 62.5%) and interfacial resistance (by 72.8%), while the cell capacity retention is promoted by >7% over a course of 110 cycles. The mechanistic investigation by X-ray photoelectron spectroscopy (XPS) and energy-dispersive X-ray spectroscopy (EDX) indicates GlyEl enriches Si SEI with elastic polyether but diminishes its carbonate species. Glyme-based electrolytes prove viable in stabilizing the SEI on silicon for future high energy density lithium-ion batteries.

Research Organization:
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Sponsoring Organization:
USDOE
DOE Contract Number:
AC05-76RL01830
OSTI ID:
1810098
Report Number(s):
PNNL-SA-160822
Journal Information:
ACS Energy Letters, Journal Name: ACS Energy Letters Journal Issue: 5 Vol. 6
Country of Publication:
United States
Language:
English

References (52)

The influence of FEC on the solvation structure and reduction reaction of LiPF6/EC electrolytes and its implication for solid electrolyte interphase formation journal October 2019
Failure progression in the solid electrolyte interphase (SEI) on silicon electrodes journal February 2020
Electrochemically induced fractures in crystalline silicon anodes journal June 2019
Intrinsic Properties of Individual Inorganic Silicon–Electrolyte Interphase Constituents journal November 2019
Review on modeling of the anode solid electrolyte interphase (SEI) for lithium-ion batteries journal March 2018
XPS-Surface Analysis of SEI Layers on Li-Ion Cathodes: Part I. Investigation of Initial Surface Chemistry journal January 2018
Diffusion-Induced Stress, Interfacial Charge Transfer, and Criteria for Avoiding Crack Initiation of Electrode Particles journal January 2010
Role of 1,3-Dioxolane and LiNO 3 Addition on the Long Term Stability of Nanostructured Silicon/Carbon Anodes for Rechargeable Lithium Batteries journal January 2016
Studies of Lithium Intercalation into Carbons Using Nonaqueous Electrochemical Cells journal January 1990
Mechanical Damage of Surface Films and Failure of Nano-Sized Silicon Electrodes in Lithium Ion Batteries journal October 2016
Rational Design of a Multifunctional Binder for High-Capacity Silicon-Based Anodes journal April 2019
Effect of fluoroethylene carbonate additive on interfacial properties of silicon thin-film electrode journal October 2006
Challenges for Rechargeable Li Batteries journal February 2010
Elucidating electrolyte decomposition under electron-rich environments at the lithium-metal anode journal January 2017
Improved Performance of the Silicon Anode for Li-Ion Batteries: Understanding the Surface Modification Mechanism of Fluoroethylene Carbonate as an Effective Electrolyte Additive journal March 2015
Localized High-Concentration Sulfone Electrolytes for High-Efficiency Lithium-Metal Batteries journal August 2018
Ultrathin conformal polycyclosiloxane films to improve silicon cycling stability journal July 2019
XPS study of diethyl carbonate adsorption on LiCoO2 thin films journal January 2013
Investigations of Si Thin Films as Anode of Lithium-Ion Batteries journal January 2018
Amorphous silicon anode for lithium-ion rechargeable batteries journal April 2003
A Highly Reversible Lithium Metal Anode journal January 2014
The intrinsic behavior of lithium fluoride in solid electrolyte interphases on lithium journal December 2019
Enabling High-Voltage Lithium-Metal Batteries under Practical Conditions journal July 2019
Synthesis and Characterization of Cobalt Hydroxide, Cobalt Oxyhydroxide, and Cobalt Oxide Nanodiscs journal November 2009
Connecting the irreversible capacity loss in Li-ion batteries with the electronic insulating properties of solid electrolyte interphase (SEI) components journal March 2016
Lithium Salt Effects on Silicon Electrode Performance and Solid Electrolyte Interphase (SEI) Structure, Role of Solution Structure on SEI Formation journal January 2017
Three-dimensional electronic resistivity mapping of solid electrolyte interphase on Si anode materials journal January 2019
Silicon as a potential anode material for Li-ion batteries: where size, geometry and structure matter journal January 2016
Tailored crosslinking of Poly(ethylene oxide) enables mechanical robustness and improved sodium-ion conductivity journal September 2019
Distilling nanoscale heterogeneity of amorphous silicon using tip-enhanced Raman spectroscopy (TERS) via multiresolution manifold learning journal January 2021
Stable cycling of high-voltage lithium metal batteries in ether electrolytes journal July 2018
XPS-Surface Analysis of SEI Layers on Li-Ion Cathodes: Part II. SEI-Composition and Formation inside Composite Electrodes journal January 2018
Exceptional Electrochemical Performance of Si-Nanowires in 1,3-Dioxolane Solutions: A Surface Chemical Investigation journal March 2012
Effects of High and Low Salt Concentration in Electrolytes at Lithium–Metal Anode Surfaces journal December 2016
The Role of Carbonate and Sulfite Additives in Propylene Carbonate-Based Electrolytes on the Formation of SEI Layers at Graphitic Li-Ion Battery Anodes journal January 2014
Nonaqueous Liquid Electrolytes for Lithium-Based Rechargeable Batteries journal October 2004
The state of understanding of the lithium-ion-battery graphite solid electrolyte interphase (SEI) and its relationship to formation cycling journal August 2016
Nonpassivated Silicon Anode Surface journal May 2020
Understanding Fluoroethylene Carbonate and Vinylene Carbonate Based Electrolytes for Si Anodes in Lithium Ion Batteries with NMR Spectroscopy journal July 2018
Electrochemical Charge Transfer Reaction Kinetics at the Silicon-Liquid Electrolyte Interface journal January 2015
Component-/structure-dependent elasticity of solid electrolyte interphase layer in Li-ion batteries: Experimental and computational studies journal March 2015
The Critical Role of Fluoroethylene Carbonate in the Gassing of Silicon Anodes for Lithium-Ion Batteries journal September 2017
Crack Pattern Formation in Thin Film Lithium-Ion Battery Electrodes journal January 2011
High rate and stable cycling of lithium metal anode journal February 2015
Identifying the Structural Basis for the Increased Stability of the Solid Electrolyte Interphase Formed on Silicon with the Additive Fluoroethylene Carbonate journal October 2017
Enabling electrolyte compositions for columnar silicon anodes in high energy secondary batteries journal September 2017
Structural Changes in Silicon Anodes during Lithium Insertion/Extraction journal January 2004
Fluoroethylene Carbonate and Vinylene Carbonate Reduction: Understanding Lithium-Ion Battery Electrolyte Additives and Solid Electrolyte Interphase Formation journal November 2016
Control and Optimization of the Electrochemical and Mechanical Properties of the Solid Electrolyte Interphase on Silicon Electrodes in Lithium Ion Batteries journal February 2016
Cracking mechanisms in lithiated silicon thin film electrodes journal November 2014
Artificial Solid Electrolyte Interphase To Address the Electrochemical Degradation of Silicon Electrodes journal June 2014
Formation and Growth Mechanisms of Solid-Electrolyte Interphase Layers in Rechargeable Batteries journal November 2015

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