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High voltage electrolytes for lithium-ion batteries with micro-sized silicon anodes

Journal Article · · Nature Communications

Abstract

Micro-sized silicon anodes can significantly increase the energy density of lithium-ion batteries with low cost. However, the large silicon volume changes during cycling cause cracks for both organic-inorganic interphases and silicon particles. The liquid electrolytes further penetrate the cracked silicon particles and reform the interphases, resulting in huge electrode swelling and quick capacity decay. Here we resolve these challenges by designing a high-voltage electrolyte that forms silicon-phobic interphases with weak bonding to lithium-silicon alloys. The designed electrolyte enables micro-sized silicon anodes (5 µm, 4.1 mAh cm −2 ) to achieve a Coulombic efficiency of 99.8% and capacity of 2175 mAh g −1 for >250 cycles and enable 100 mAh LiNi 0.8 Co 0.15 Al 0.05 O 2 pouch full cells to deliver a high capacity of 172 mAh g −1 for 120 cycles with Coulombic efficiency of >99.9%. The high-voltage electrolytes that are capable of forming silicon-phobic interphases pave new ways for the commercialization of lithium-ion batteries using micro-sized silicon anodes.

Sponsoring Organization:
USDOE
Grant/Contract Number:
NONE; EE0009183; SC0012704
OSTI ID:
2293628
Alternate ID(s):
OSTI ID: 2315630
Journal Information:
Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 15; ISSN 2041-1723
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United Kingdom
Language:
English

References (59)

A Critical Size of Silicon Nano-Anodes for Lithium Rechargeable Batteries journal March 2010
Enhancing Li + Transport in NMC811||Graphite Lithium‐Ion Batteries at Low Temperatures by Using Low‐Polarity‐Solvent Electrolytes journal July 2022
Electrolyte/Electrode Interfaces in All-Solid-State Lithium Batteries: A Review journal April 2021
Systematic and collaborative approach to problem solving using X-ray photoelectron spectroscopy journal September 2021
Highly Fluorinated Interphases Enable High-Voltage Li-Metal Batteries journal January 2018
Influence of external pressure on silicon electrodes in lithium-ion cells journal July 2022
Silicon Microparticle Anodes with Self-Healing Multiple Network Binder journal May 2018
High-Energy Li Metal Battery with Lithiated Host journal March 2019
Enabling electrolyte compositions for columnar silicon anodes in high energy secondary batteries journal September 2017
A carbonate-free, sulfone-based electrolyte for high-voltage Li-ion batteries journal May 2018
Interface Stability in Solid-State Batteries journal December 2015
Solvate Structures and Computational/Spectroscopic Characterization of LiPF 6 Electrolytes journal April 2015
Insights into the Structure and Transport of the Lithium, Sodium, Magnesium, and Zinc Bis(trifluoromethansulfonyl)imide Salts in Ionic Liquids journal August 2018
Nonvolatile and Nonflammable Sulfolane-Based Electrolyte Achieving Effective and Safe Operation of the Li–O2 Battery in Open O2 Environment journal January 2022
Nanoscale Chemical Evolution of Silicon Negative Electrodes Characterized by Low-Loss STEM-EELS journal November 2016
Robust Solid/Electrolyte Interphase (SEI) Formation on Si Anodes Using Glyme-Based Electrolytes journal April 2021
Nonaqueous Liquid Electrolytes for Lithium-Based Rechargeable Batteries journal October 2004
Weakly Solvating Solution Enables Chemical Prelithiation of Graphite–SiO x Anodes for High-Energy Li-Ion Batteries journal June 2021
Quantum Chemistry and Molecular Dynamics Simulation Study of Dimethyl Carbonate: Ethylene Carbonate Electrolytes Doped with LiPF 6 journal February 2009
Viscosity of a Room Temperature Ionic Liquid: Predictions from Nonequilibrium and Equilibrium Molecular Dynamics Simulations journal March 2009
Polarizable Force Field Development and Molecular Dynamics Simulations of Ionic Liquids journal August 2009
Anisotropic Swelling and Fracture of Silicon Nanowires during Lithiation journal August 2011
Building better batteries journal February 2008
Promise and reality of post-lithium-ion batteries with high energy densities journal March 2016
Opportunities and challenges for a sustainable energy future journal August 2012
Self-healing chemistry enables the stable operation of silicon microparticle anodes for high-energy lithium-ion batteries journal November 2013
High rate and stable cycling of lithium metal anode journal February 2015
Silicon carbide-free graphene growth on silicon for lithium-ion battery with high volumetric energy density journal June 2015
High-performance lithium-ion anodes using a hierarchical bottom-up approach journal March 2010
High-performance lithium battery anodes using silicon nanowires journal December 2007
High capacity silicon anodes enabled by MXene viscous aqueous ink journal February 2019
Supremely elastic gel polymer electrolyte enables a reliable electrode structure for silicon-based anodes journal December 2019
Identifying the components of the solid–electrolyte interphase in Li-ion batteries journal August 2019
Battery revolution to evolution journal November 2019
Electrolyte design for LiF-rich solid–electrolyte interfaces to enable high-performance microsized alloy anodes for batteries journal April 2020
Calendar aging of silicon-containing batteries journal September 2021
Formation of hierarchically ordered structures in conductive polymers to enhance the performances of lithium-ion batteries journal January 2023
Non-flammable electrolyte enables Li-metal batteries with aggressive cathode chemistries journal July 2018
Aqueous Li-ion battery enabled by halogen conversion–intercalation chemistry in graphite journal May 2019
Valence electron energy-loss spectroscopy of silicon negative electrodes for lithium batteries journal January 2010
3D visualization of inhomogeneous multi-layered structure and Young's modulus of the solid electrolyte interphase (SEI) on silicon anodes for lithium ion batteries journal January 2014
High-voltage positive electrode materials for lithium-ion batteries journal January 2017
Guidelines and trends for next-generation rechargeable lithium and lithium-ion batteries journal January 2020
Silicon oxides: a promising family of anode materials for lithium-ion batteries journal January 2019
Revealing the size-dependent electrochemical Li-storage behaviors of SiO-based anodes journal January 2022
Recent developments in nanostructured anode materials for rechargeable lithium-ion batteries journal January 2011
The Nose–Hoover thermostat journal October 1985
Commentary: The Materials Project: A materials genome approach to accelerating materials innovation journal July 2013
Self-Consistent Equations Including Exchange and Correlation Effects journal November 1965
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set journal October 1996
Generalized Gradient Approximation Made Simple journal October 1996
FIT2D : a multi-purpose data reduction, analysis and visualization program journal March 2016
A Major Constituent of Brown Algae for Use in High-Capacity Li-Ion Batteries journal September 2011
Highly elastic binders integrating polyrotaxanes for silicon microparticle anodes in lithium ion batteries journal July 2017
Analysis of SiO Anodes for Lithium-Ion Batteries journal January 2005
Alloy Design for Lithium-Ion Battery Anodes journal January 2007
Dynamic Structure Discovery Applied to the Ion Transport in the Ubiquitous Lithium-ion Battery Electrolyte LP30 journal October 2022
Electrolyte Solvation and Ionic Association II. Acetonitrile-Lithium Salt Mixtures: Highly Dissociated Salts journal January 2012
Li + Transference Numbers in Liquid Electrolytes Obtained by Very-Low-Frequency Impedance Spectroscopy at Variable Electrode Distances journal January 2016

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