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

Direct Prelithiation of Silicon-Based Composite Electrodes via Island-like Thermal Evaporation

Journal Article · · Energy & Fuels

Irreversible losses of Li during solid electrolyte interface (SEI) conditioning in batteries are a key contributor to the lower specific capacities observed in silicon-containing Li-ion batteries. Herein, thermal evaporation of between 1 and 20 μm of Li onto Si-based composite anodes has been investigated as a prelithiation method to compensate for such losses. Additionally, to account for mechanical strain caused by Li–Si alloying and electrode expansion during the deposition, a stainless-steel mesh is applied to the electrodes before prelithiation to form “island-like” deposition on the electrode surface. Here, the open circuit potential was also found to decrease as a function of increased Li evaporation, consistent with the potentials of electrochemically prepared LixSi alloys. Prelithiating to compensate for irreversible Li losses to SEI formation resulted in full cells with a 15.8% increase in initial Coulombic efficiency and a 47.8% reduction in irreversible capacity loss after SEI formation cycling. Subsequent C/3 cycling showed up to a 62.9% increase in the specific capacity in prelithiated cells. X-ray photoelectron spectroscopy (XPS) revealed differences in the SEI composition that was formed by electrochemical cycling and reactively formed in prelithiated cells upon exposure to the Gen2 + 3% FEC electrolyte. The reactively formed SEI from the spontaneous reaction with lithiated silicon was carbonate-rich, while the electrochemical SEI formation showed significantly more LiPFx species, which could play a role in overall cycling performance.

Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO); German Ministry of Education and Science (BMBF)
Grant/Contract Number:
AC05-00OR22725
OSTI ID:
2586935
Alternate ID(s):
OSTI ID: 2587179
Journal Information:
Energy & Fuels, Journal Name: Energy & Fuels Journal Issue: 10 Vol. 39; ISSN 1520-5029; ISSN 0887-0624
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English

References (94)

Carbon-Based Anodes for Lithium Sulfur Full Cells with High Cycle Stability journal August 2013
Achieving Desirable Initial Coulombic Efficiencies and Full Capacity Utilization of Li‐Ion Batteries by Chemical Prelithiation of Graphite Anode journal April 2021
Pre‐Lithiation of Silicon Anodes by Thermal Evaporation of Lithium for Boosting the Energy Density of Lithium Ion Cells journal March 2022
Engineering Prelithiation of Polyacrylic Acid Binder: A Universal Strategy to Boost Initial Coulombic Efficiency for High‐Areal‐Capacity Si‐Based Anodes journal July 2022
Electrolyte Design Enabling a High‐Safety and High‐Performance Si Anode with a Tailored Electrode–Electrolyte Interphase journal August 2021
Unblocked Electron Channels Enable Efficient Contact Prelithiation for Lithium‐Ion Batteries journal March 2022
Interfacing Si‐Based Electrodes: Impact of Liquid Electrolyte and Its Components journal January 2022
Surface and Interface Engineering of Silicon-Based Anode Materials for Lithium-Ion Batteries journal July 2017
Mechanistic Insights into the Pre‐Lithiation of Silicon/Graphite Negative Electrodes in “Dry State” and After Electrolyte Addition Using Passivated Lithium Metal Powder journal May 2021
Revisiting the Preparation Progress of Nano‐Structured Si Anodes toward Industrial Application from the Perspective of Cost and Scalability journal January 2022
On the Practical Applicability of the Li Metal‐Based Thermal Evaporation Prelithiation Technique on Si Anodes for Lithium Ion Batteries journal November 2022
Elucidating the Role of Prelithiation in Si‐based Anodes for Interface Stabilization journal June 2023
A Thorough Analysis of Two Different Pre‐Lithiation Techniques for Silicon/Carbon Negative Electrodes in Lithium Ion Batteries journal March 2021
Precisely Prelithiated Polyacrylic Acid Binder Improving Electrochemical Performance of Micron‐Sized Silicon Anodes for Lithium‐Ion Batteries journal June 2024
Research Progress on Coating Structure of Silicon Anode Materials for Lithium‐Ion Batteries journal October 2021
Chemically Prelithiated Hard‐Carbon Anode for High Power and High Capacity Li‐Ion Batteries journal January 2020
The Vital Role of Electrolyte Reduction Potential in Forming a Stable SEI in Phosphorus‐Based Anodes journal March 2023
Benchmarking the Effect of Particle Size on Silicon Anode Materials for Lithium‐Ion Batteries journal June 2023
Regulating the Solvation Structure of Li+ Enables Chemical Prelithiation of Silicon-Based Anodes Toward High-Energy Lithium-Ion Batteries journal April 2023
Carbon-coated SiOx anode materials via PVD and pyrolyzed fuel oil to achieve lithium-ion batteries with high cycling stability journal January 2022
Impedance of porous electrodes journal November 1995
Milled flake graphite/plasma nano-silicon@carbon composite with void sandwich structure for high performance as lithium ion battery anode at high temperature journal April 2018
Advanced electrolyte/additive for lithium-ion batteries with silicon anode journal August 2016
Prelithiation of silicon/graphite composite anodes: Benefits and mechanisms for long-lasting Li-Ion batteries journal August 2020
Prelithiation strategies for silicon-based anode in high energy density lithium-ion battery journal October 2023
Prelithiated rigid polymer with high ionic conductivity as silicon-based anode binder for lithium-ion battery journal November 2023
Impedance of porous electrodes in the presence of electroactive species and solution resistance journal December 2023
Effect of electrode structure on performance of Si anode in Li-ion batteries: Si particle size and conductive additive journal January 2005
Li-doping process for LixSiO-negative active material synthesized by chemical method for lithium-ion cells journal August 2005
Electrochemical behaviors of silicon based anode material journal February 2006
A prelithiated carbon anode for lithium-ion battery applications journal November 2006
Deciphering the multi-step degradation mechanisms of carbonate-based electrolyte in Li batteries journal March 2008
Scalable process for application of stabilized lithium metal powder in Li-ion batteries journal March 2016
Connecting the irreversible capacity loss in Li-ion batteries with the electronic insulating properties of solid electrolyte interphase (SEI) components journal March 2016
Mechanism of the carbonate-based-electrolyte degradation and its effects on the electrochemical performance of Li 1+x (Ni a Co b Mn 1-a-b ) 1-x O 2 cells journal December 2016
Improved electrochemical performance of micro-sized SiO-based composite anode by prelithiation of stabilized lithium metal powder journal April 2017
Understanding the influence of electrolyte additives on the electrochemical performance and morphology evolution of silicon nanowire based lithium-ion battery anodes journal August 2017
Understanding of pre-lithiation of poly(acrylic acid) binder: Striking the balances between the cycling performance and slurry stability for silicon-graphite composite electrodes in Li-ion batteries journal March 2019
Improving the cyclability of silicon anodes for lithium-ion batteries using a simple pre-lithiation method journal May 2020
An electrode-level prelithiation of SiO anodes with organolithium compounds for lithium-ion batteries journal December 2020
Competitive adsorption within electrode slurries and impact on cell fabrication and performance journal February 2022
Quantification of lithium inventory loss in micro silicon anode via titration-gas chromatography journal May 2022
Improved stability of nano-Sn electrode with high-quality nano-SEI formation for lithium ion battery journal March 2015
Designing nanostructured Si anodes for high energy lithium ion batteries journal October 2012
Differential cross-section measurements for the 7Li(p,p0)7Li, 7Li(p,p1)7Li, 7Li(p,α0)4He, 19F(p,p0)19F, 19F(p,α0)16O and 19F(p,α1,2)16O reactions journal October 2012
MATBOX: An Open-source Microstructure Analysis Toolbox for microstructure generation, segmentation, characterization, visualization, correlation, and meshing journal January 2022
A highly effective and controllable chemical prelithiation of Silicon/Carbon/Graphite composite anodes for lithium-ion batteries journal December 2023
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
Elucidating the Role of Carbon Conductive Additive in the Processing and Electrochemical Behavior of Surface-Modified Si Anodes journal March 2024
In Situ Prelithiation by Direct Integration of Lithium Mesh into Battery Cells journal May 2023
Ambient-Air Stable Lithiated Anode for Rechargeable Li-Ion Batteries with High Energy Density journal October 2016
Silicon-Core–Carbon-Shell Nanoparticles for Lithium-Ion Batteries: Rational Comparison between Amorphous and Graphitic Carbon Coatings journal September 2019
Prelithiation Effects in Enhancing Silicon-Based Anodes for Full-Cell Lithium-Ion Batteries Using Stabilized Lithium Metal Particles journal May 2023
Chemical Pre-lithiation of SiOx Anodes with a Weakly Solvating Solution of Polycyclic Aromatic Hydrocarbons for Lithium-Ion Batteries journal August 2023
Enabling SiO x /C Anode with High Initial Coulombic Efficiency through a Chemical Pre-Lithiation Strategy for High-Energy-Density Lithium-Ion Batteries journal May 2020
Direct-Contact Prelithiation of Si–C Anode Study as a Function of Time, Pressure, Temperature, and the Cell Ideal Time journal April 2022
Functionalized Silicon Particles for Enhanced Half- and Full-Cell Cycling of Si-Based Li-Ion Batteries journal February 2023
Impact of Electrolyte on Direct-Contact Prelithiation of Silicon-Graphite Anodes in Lithium-Ion Cells with High-Nickel Cathodes journal August 2024
Chemical Prelithiation of Negative Electrodes in Ambient Air for Advanced Lithium-Ion Batteries journal February 2019
Fast and Controllable Prelithiation of Hard Carbon Anodes for Lithium-Ion Batteries journal February 2020
Tailoring Electrolyte Solvation Chemistry toward an Inorganic-Rich Solid-Electrolyte Interphase at a Li Metal Anode journal May 2021
New Insight into the Role of Fluoro-ethylene Carbonate in Suppressing Li-Trapping for Si Anodes in Lithium-Ion Batteries journal September 2023
Effective Chemical Prelithiation Strategy for Building a Silicon/Sulfur Li-Ion Battery journal May 2019
Weakly Solvating Solution Enables Chemical Prelithiation of Graphite–SiO x Anodes for High-Energy Li-Ion Batteries journal June 2021
Solvent Decompositions and Physical Properties of Decomposition Compounds in Li-Ion Battery Electrolytes Studied by DFT Calculations and Molecular Dynamics Simulations journal February 2005
Ring-Opening Polymerization of Ethylene Carbonate and Depolymerization of Poly(ethylene oxide- c o -ethylene carbonate) journal March 2000
Anisotropic Swelling and Fracture of Silicon Nanowires during Lithiation journal August 2011
Prelithiation of Silicon–Carbon Nanotube Anodes for Lithium Ion Batteries by Stabilized Lithium Metal Powder (SLMP) journal August 2013
Prelithiated Silicon Nanowires as an Anode for Lithium Ion Batteries journal July 2011
Overcoming low initial coulombic efficiencies of Si anodes through prelithiation in all-solid-state batteries journal April 2024
Review on modeling of the anode solid electrolyte interphase (SEI) for lithium-ion batteries journal March 2018
Free-standing ultrathin lithium metal–graphene oxide host foils with controllable thickness for lithium batteries journal May 2021
Analysis of Rutherford backscattering spectra with CNN-GRU mixture density network journal July 2024
Understanding undesirable anode lithium plating issues in lithium-ion batteries journal January 2016
Lithium trapping in alloy forming electrodes and current collectors for lithium based batteries journal January 2017
Walnut-structure Si–G/C materials with high coulombic efficiency for long-life lithium ion batteries journal January 2018
Electrolytes for advanced lithium ion batteries using silicon-based anodes journal January 2019
Real-time monitoring of stress development during electrochemical cycling of electrode materials for Li-ion batteries: overview and perspectives journal January 2019
Morphology engineering of silicon nanoparticles for better performance in Li-ion battery anodes journal January 2020
Bulk boron doping and surface carbon coating enabling fast-charging and stable Si anodes: from thin film to thick Si electrodes journal January 2021
Improving the cycling stability of silicon nanowire anodes with conducting polymer coatings journal January 2012
Minimized lithium trapping by isovalent isomorphism for high initial Coulombic efficiency of silicon anodes journal November 2019
Structured Silicon Anodes for Lithium Battery Applications journal January 2003
Structural Changes in Silicon Anodes during Lithium Insertion/Extraction journal January 2004
Chemical Formation of a Solid Electrolyte Interface on the Carbon Electrode of a Li-Ion Cell journal January 1998
Examining CO 2 as an Additive for Solid Electrolyte Interphase Formation on Silicon Anodes journal March 2021
Investigation of the Direct Contact Prelithiation of Silicon-Graphite Composite Anodes for Lithium-Ion Batteries journal June 2023
Understanding the Electrolyte Chemistry Induced Enhanced Stability of Si Anodes in Li-Ion Batteries based on Physico-Chemical Changes, Impedance, and Stress Evolution during SEI Formation journal September 2023
Analysis of Degradation of Si/Carbon||LiNi 0.5 Mn 0.3 Co 0.2 O 2 Full Cells: Effect of Prelithiation journal January 2019
Performance Enhancing Electrolyte Additives for Lithium Ion Batteries with Silicon Anodes journal January 2012
Investigation of Pre-lithiation in Graphite and Hard-Carbon Anodes Using Different Lithium Source Structures journal January 2017
Understand and Mitigate Reaction Non-Uniformity in Battery Electrodes journal May 2019
Impact of Full Prelithiation of Si-Based Anodes on the Rate and Cycle Performance of Li-Ion Capacitors journal May 2022
A New High-Throughput Focused MeV Ion-Beam Analysis Setup journal February 2021

Similar Records

Direct Prelithiation of Silicon-Based Composite Electrodes via Island-like Thermal Evaporation
Journal Article · Thu Mar 13 00:00:00 EDT 2025 · Energy & Fuels · OSTI ID:2587179

Insights on the cycling behavior of a highly-prelithiated silicon–graphite electrode in lithium-ion cells
Journal Article · Mon Feb 10 23:00:00 EST 2020 · JPhys Energy · OSTI ID:1774506

Achieving SEI preformed graphite in flow cell to mitigate initial lithium loss
Journal Article · Sat May 14 00:00:00 EDT 2022 · Carbon · OSTI ID:1874579

Related Subjects