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

Evaluating the Effect of Electrolyte Additive Functionalities on NMC622/Si Cell Performance

Journal Article · · Journal of the Electrochemical Society

Unstable electrode/electrolyte interface is the major cause of degradation for silicon (Si)-based anodes for lithium (Li)-ion batteries. Development of functional electrolyte additives can provide a viable path toward stabilizing the dynamic Si/electrolyte interface, which will benefit the development of high energy density Li-ion batteries. Here, we evaluate polymerizable electrolyte additives with varying functional groups (fluorocarbon, thiophosphate, and fluorophosphazene). The additives are examined using LiNi0.6Mn0.2Co0.2O2/Si full cells where the cycle performance and impedance are measured. Electrochemical tests show that the fluorine-containing additives provide better passivation at the Si electrode, leading to enhanced full cell performance. Here, among the three additives examined, best electrochemical performance is observed from the fluorocarbon-containing compound, followed by fluorophosphazene- and thiophosphate-containing compounds. Characterization of the solid electrolyte interphase (SEI) on cycled electrodes using Auger electron spectroscopy (AES), X-ray photoelectron spectroscopy (XPS), and attenuated total reflectance Fourier transform infrared spectroscopy (ATR-FTIR) reveal that higher concentration of fluorine and lithium oxide, and lower concentration of carbonate and organic species correlate with enhanced electrochemical performance.

Research Organization:
National Renewable Energy Laboratory (NREL), Golden, CO (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office
Grant/Contract Number:
AC36-08GO28308; SC0021392
OSTI ID:
1876016
Alternate ID(s):
OSTI ID: 1988742
Report Number(s):
NREL/JA-5K00-82464; MainId:83237; UUID:10ad23e4-5ab1-4dc0-82d4-ee021d5d06e5; MainAdminID:64825
Journal Information:
Journal of the Electrochemical Society, Journal Name: Journal of the Electrochemical Society Journal Issue: 7 Vol. 169; ISSN 0013-4651
Publisher:
IOP PublishingCopyright Statement
Country of Publication:
United States
Language:
English

References (53)

Recent Advances in Silicon‐Based Electrodes: From Fundamental Research toward Practical Applications journal March 2021
Revisiting the Preparation Progress of Nano‐Structured Si Anodes toward Industrial Application from the Perspective of Cost and Scalability journal January 2022
Clarification of Decomposition Pathways in a State‐of‐the‐Art Lithium Ion Battery Electrolyte through 13 C‐Labeling of Electrolyte Components journal February 2020
Confronting the Challenges of Next‐Generation Silicon Anode‐Based Lithium‐Ion Batteries: Role of Designer Electrolyte Additives and Polymeric Binders journal May 2019
Deposition and XPS and FTIR Analysis of Plasma Polymer Coatings Containing Phosphorus: XPS & FTIR Analysis of P Containing pp journal January 2014
XPS investigation on the reactivity of surface imine groups with TFAA journal January 2019
Evaluating temperature dependent degradation mechanisms of silicon-graphite electrodes and the effect of fluoroethylene carbonate electrolyte additive journal October 2021
Diverting Exploration of Silicon Anode into Practical Way: A Review Focused on Silicon-Graphite Composite for Lithium Ion Batteries journal March 2021
A high-flux P84 polyimide mixed matrix membranes incorporated with cadmium-based metal organic frameworks for enhanced simultaneous dyes removal: Response surface methodology journal April 2020
Generation and Evolution of the Solid Electrolyte Interphase of Lithium-Ion Batteries journal October 2019
Comparative study of trimethyl phosphite and trimethyl phosphate as electrolyte additives in lithium ion batteries journal June 2005
Effect of fluoroethylene carbonate additive on interfacial properties of silicon thin-film electrode journal October 2006
Fluorinated phosphazene co-solvents for improved thermal and safety performance in lithium-ion battery electrolytes journal October 2014
Aging investigations of a lithium-ion battery electrolyte from a field-tested hybrid electric vehicle journal January 2015
Study of triallyl phosphate as an electrolyte additive for high voltage lithium-ion cells journal November 2015
Failure progression in the solid electrolyte interphase (SEI) on silicon electrodes journal February 2020
FTIR features of lithium-iron phosphates as electrode materials for rechargeable lithium batteries journal December 2006
The Chemistry of Electrolyte Reduction on Silicon Electrodes Revealed by in Situ ATR-FTIR Spectroscopy journal June 2017
Decomposition Reactions of Anode Solid Electrolyte Interphase (SEI) Components with LiPF 6 journal October 2017
In Situ Observation of Lithiation and Delithiation Reactions of a Silicon Thin Film Electrode for All-Solid-State Lithium-Ion Batteries by X-ray Photoelectron Spectroscopy journal July 2020
SiO 2 Is Wasted Space in Single-Nanometer-Scale Silicon Nanoparticle-Based Composite Anodes for Li-Ion Electrochemical Energy Storage journal November 2020
Hydrophobic versus Hydrophilic Interfacial Coatings on Silicon Nanoparticles Teach Us How to Design the Solid Electrolyte Interphase in Silicon-Based Li-Ion Battery Anodes journal February 2021
XPS on Li-Battery-Related Compounds: Analysis of Inorganic SEI Phases and a Methodology for Charge Correction journal August 2018
Tailoring the Surface of Silicon Nanoparticles for Enhanced Chemical and Electrochemical Stability for Li-Ion Batteries journal August 2019
Nonpassivated Silicon Anode Surface journal May 2020
Electrochemical Reactivity and Passivation of Silicon Thin-Film Electrodes in Organic Carbonate Electrolytes journal August 2020
Probing the Reactivity of the Active Material of a Li-Ion Silicon Anode with Common Battery Solvents journal June 2021
Highly Adhesive and Soluble Copolyimide Binder: Improving the Long-Term Cycle Life of Silicon Anodes in Lithium-Ion Batteries journal June 2015
Hard X-ray Photoelectron Spectroscopy (HAXPES) Investigation of the Silicon Solid Electrolyte Interphase (SEI) in Lithium-Ion Batteries journal August 2015
Systematic Investigation of Binders for Silicon Anodes: Interactions of Binder with Silicon Particles and Electrolytes and Effects of Binders on Solid Electrolyte Interphase Formation journal May 2016
Functionality Selection Principle for High Voltage Lithium-ion Battery Electrolyte Additives journal August 2017
Electrolyte-Additive-Driven Interfacial Engineering for High-Capacity Electrodes in Lithium-Ion Batteries: Promise and Challenges journal April 2020
Understanding Fluoroethylene Carbonate and Vinylene Carbonate Based Electrolytes for Si Anodes in Lithium Ion Batteries with NMR Spectroscopy journal July 2018
Spectroscopic Compositional Analysis of Electrolyte during Initial SEI Layer Formation journal July 2014
A cyclic phosphate-based battery electrolyte for high voltage and safe operation journal March 2020
Calendar aging of silicon-containing batteries journal September 2021
Sulfur double locked by a macro-structural cathode and a solid polymer electrolyte for lithium–sulfur batteries journal January 2015
Surface characterization and degradation behavior of polyimide films induced by coupling irradiation treatment journal January 2018
Designing superior solid electrolyte interfaces on silicon anodes for high-performance lithium-ion batteries journal January 2019
Intrinsic chemical reactivity of solid-electrolyte interphase components in silicon–lithium alloy anode batteries probed by FTIR spectroscopy journal January 2020
Facile synthesis of mesoporous carbon nitrides using the incipient wetness method and the application as hydrogen adsorbent journal January 2011
Si powders and electrodes for high-energy lithium-ion cells journal June 2020
Failure Modes of Silicon Powder Negative Electrode in Lithium Secondary Batteries journal January 2004
Reversible Cycling of Crystalline Silicon Powder journal January 2007
Perspective—Structure and Stability of the Solid Electrolyte Interphase on Silicon Anodes of Lithium-ion Batteries journal March 2021
Design of a Scavenging Pyrrole Additive for High Voltage Lithium-Ion Batteries journal April 2022
Mechanical Damage of Surface Films and Failure of Nano-Sized Silicon Electrodes in Lithium Ion Batteries journal October 2016
Citric Acid Based Pre-SEI for Improvement of Silicon Electrodes in Lithium Ion Batteries journal January 2018
Electrode Behavior RE-Visited: Monitoring Potential Windows, Capacity Loss, and Impedance Changes in Li 1.03 (Ni 0.5 Co 0.2 Mn 0.3 ) 0.97 O 2 /Silicon-Graphite Full Cells journal January 2016
Comparative Study of Fluoroethylene Carbonate and Vinylene Carbonate for Silicon Anodes in Lithium Ion Batteries journal January 2014
Review—SEI: Past, Present and Future journal January 2017
Binding Energy Referencing for XPS in Alkali Metal-Based Battery Materials Research (II): Application to Complex Composite Electrodes journal August 2018
Preparation of Superhydrophobic Polymeric Film on Aluminum Plates by Electrochemical Polymerization journal November 2009

Similar Records

Direct Prelithiation of Silicon-Based Composite Electrodes via Island-like Thermal Evaporation
Journal Article · Thu Feb 27 23:00:00 EST 2025 · Energy & Fuels · OSTI ID:2586935

The Impact of Different Substituents in Fluorinated Cyclic Carbonates in the Performance of High Voltage Lithium-Ion Battery Electrolyte
Journal Article · Wed Jan 06 23:00:00 EST 2021 · Journal of the Electrochemical Society (Online) · OSTI ID:1797972

Cycling behavior of NCM523/graphite lithium-ion cells in the 3–4.4 V range: Diagnostic studies of full cells and harvested electrodes
Journal Article · Thu Sep 22 00:00:00 EDT 2016 · Journal of the Electrochemical Society · OSTI ID:1337947