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

Understanding Binder–Silicon Interactions during Slurry Processing

Journal Article · · Journal of Physical Chemistry. C
The conformation of poly(acrylic acid) (PAA) as a function of shear during slurry processing to construct silicon-based anodes is elucidated via rheology-coupled ultra-small-angle neutron scattering (rheo-USANS). Rheo-USANS shows that PAA with encapsulated silicon exists as discrete aggregates that do not interact with one another. As a result, a well-connected matrix of silicon and carbon black dispersed in PAA does not exist; thus, the electrode is inhomogeneous. Raman mapping and X-ray photoelectron spectroscopy were used to confirm the electrode heterogeneity and further understand the cycling properties. These results are correlated to silicon surface chemistry to provide a pathway to making better electrodes.
Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office
Grant/Contract Number:
AC05-00OR22725
OSTI ID:
1649398
Journal Information:
Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Journal Issue: 24 Vol. 124; ISSN 1932-7447
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English

References (126)

FTIR studies of conformational energies of poly(acrylic acid) in cast films journal February 1997
Silicon Composite Electrodes with Dynamic Ionic Bonding journal May 2017
Molecular rheology of polymer solutions: Interpretation and utility journal January 1975
A Highly Cross-Linked Polymeric Binder for High-Performance Silicon Negative Electrodes in Lithium Ion Batteries journal July 2012
Hildebrand and Hansen solubility parameters from Molecular Dynamics with applications to electronic nose polymer sensors journal January 2004
Rheological investigations of suspensions of talc, calcium carbonate, and their mixtures in a polystyrene melt journal November 1999
Osmotic deswelling of weakly charged poly(acrylic acid) solutions and gels journal November 1995
Solvation characteristics of a model water-soluble polymer journal January 2006
A Quadruple-Hydrogen-Bonded Supramolecular Binder for High-Performance Silicon Anodes in Lithium-Ion Batteries journal June 2018
Shear rate-dependent structure of polymer-stabilized TiO2 dispersions journal March 2013
Si-Based Anode Materials for Li-Ion Batteries: A Mini Review journal September 2014
Electronic structure of strained polymers: 3. Scaled Hessians for polyethylene journal January 1993
Concentration and shear rate dependence of viscosity in random coil polysaccharide solutions journal September 1981
XPS studies on SiOx thin films journal June 1993
Particle size and zeta potential of carbon black in liquid media journal November 2007
Ultra-small-angle scattering studies of complex fluids journal June 2005
Reversible conformational behavior of poly(acrylic acid) LB film with changes in pH, ionic strength and time journal February 2006
Dispersion mechanisms in aqueous alumina suspensions at high solids loadings journal February 2006
Effect of nonionic and ionic surfactants on zeta potential and dispersion properties of carbon black powders journal June 2009
On the binding mechanism of CMC in Si negative electrodes for Li-ion batteries journal December 2007
Self-healing strategy for Si nanoparticles towards practical application as anode materials for Li-ion batteries journal February 2018
Lithium polyacrylate as a binder for tin–cobalt–carbon negative electrodes in lithium-ion batteries journal March 2010
Cyclability study of silicon–carbon composite anodes for lithium-ion batteries using electrochemical impedance spectroscopy journal April 2011
Effect of binder properties on electrochemical performance for silicon-graphite anode: Method and application of binder screening journal August 2014
A Facile 3D Binding Approach for High Si Loading Anodes journal September 2016
A comparative study of polyacrylic acid (PAA) and carboxymethyl cellulose (CMC) binders for Si-based electrodes journal December 2017
A study of the relationship between coulombic efficiency and capacity degradation of commercial lithium-ion batteries journal February 2018
Critical electrode properties and drying conditions causing component segregation in graphitic anodes for lithium-ion batteries journal August 2018
Size and pH effect on electrical and conformational behavior of poly(acrylic acid): Simulation and experiment journal May 2006
Polyvinyl alcohol grafted poly (acrylic acid) as water-soluble binder with enhanced adhesion capability and electrochemical performances for Si anode journal September 2018
Stability analysis for 5V high energy density pouch batteries of Si anode and SL/EMC electrolytes journal January 2019
Adsorption of poly(acrylic acid) onto the surface of titanium dioxide and the colloidal stability of aqueous suspension journal January 2005
Optimization of multicomponent aqueous suspensions of lithium iron phosphate (LiFePO4) nanoparticles and carbon black for lithium-ion battery cathodes journal September 2013
DLS and zeta potential – What they are and what they are not? journal August 2016
Effect of crosslinking binders on Li-storage behavior of silicon particles as anodes for lithium ion batteries journal July 2019
Role of the binder on the failure mechanism of Si nano-composite electrodes for Li-ion batteries journal August 2011
Critical roles of binders and formulation at multiscales of silicon-based composite electrodes journal April 2015
Investigation of film solidification and binder migration during drying of Li-Ion battery anodes journal June 2016
Influence of inactive electrode components on degradation phenomena in nano-Si electrodes for Li-ion batteries journal September 2016
Investigation of binder distribution in graphite anodes for lithium-ion batteries journal February 2017
What makes lithium substituted polyacrylic acid a better binder than polyacrylic acid for silicon-graphite composite anodes? journal April 2018
Quantifying gas generation from slurries used in fabrication of Si-containing electrodes for lithium-ion cells journal August 2018
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
Mantid—Data analysis and visualization package for neutron scattering and μ SR experiments
  • Arnold, O.; Bilheux, J. C.; Borreguero, J. M.
  • Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 764 https://doi.org/10.1016/j.nima.2014.07.029
journal November 2014
Role of organically modified layered silicate as an active interfacial modifier in immiscible polystyrene/polypropylene blends journal November 2004
pH-induced conformational changes of loosely grafted molecular brushes containing poly(acrylic acid) side chains journal November 2008
Dispersion and rheological properties of concentrated silicon aqueous suspension journal January 2006
Theory of polyelectrolytes in solutions and at surfaces journal November 2005
Nonlinear Behavior of Gelatin Networks Reveals a Hierarchical Structure journal December 2015
Formation and Growth Mechanisms of Solid-Electrolyte Interphase Layers in Rechargeable Batteries journal November 2015
Role of Polyacrylic Acid (PAA) Binder on the Solid Electrolyte Interphase in Silicon Anodes journal March 2019
Auger Electrons as Probes for Composite Micro- and Nanostructured Materials: Application to Solid Electrolyte Interphases in Graphite and Silicon-Graphite Electrodes journal October 2017
Improved Cycling Performance of a Si Nanoparticle Anode Utilizing Citric Acid as a Surface-Modifying Agent journal December 2016
Polydopamine Wrapping Silicon Cross-linked with Polyacrylic Acid as High-Performance Anode for Lithium-Ion Batteries journal January 2016
Cross-Linked Chitosan as an Efficient Binder for Si Anode of Li-ion Batteries journal January 2016
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
Mussel-Inspired Conductive Polymer Binder for Si-Alloy Anode in Lithium-Ion Batteries journal January 2018
Chemical Evolution in Silicon–Graphite Composite Anodes Investigated by Vibrational Spectroscopy journal May 2018
Direct Observation of Carboxymethyl Cellulose and Styrene–Butadiene Rubber Binder Distribution in Practical Graphite Anodes for Li-Ion Batteries journal October 2019
The Study of the Binder Poly(acrylic acid) and Its Role in Concomitant Solid–Electrolyte Interphase Formation on Si Anodes journal January 2020
Revealing the Role of Poly(vinylidene fluoride) Binder in Si/Graphite Composite Anode for Li-Ion Batteries journal September 2018
Toward Efficient Binders for Li-Ion Battery Si-Based Anodes: Polyacrylic Acid journal October 2010
Toward Silicon Anodes for Next-Generation Lithium Ion Batteries: A Comparative Performance Study of Various Polymer Binders and Silicon Nanopowders journal July 2013
Multifunctional Molecular Design as an Efficient Polymeric Binder for Silicon Anodes in Lithium-Ion Batteries journal October 2014
Role of Surface Oxides in the Formation of Solid–Electrolyte Interphases at Silicon Electrodes for Lithium-Ion Batteries journal November 2014
The Isoelectric Points of Solid Oxides, Solid Hydroxides, and Aqueous Hydroxo Complex Systems journal April 1965
Measurement of the interaction between adsorbed polyelectrolytes: gelatin on mica surfaces journal May 1990
The Flow of Cream through Narrow Glass Tubes. journal July 1939
Intrinsic Viscosities of Polyelectrolytes. Poly-(acrylic Acid) journal August 1954
General Method of Manipulating Formation, Composition, and Morphology of Solid-Electrolyte Interphases for Stable Li-Alloy Anodes journal November 2017
Differential Charging in SiO 2 /Si System As Determined by XPS journal December 2003
Study on Polymer Binders for High-Capacity SiO Negative Electrode of Li-Ion Batteries journal June 2011
Examining Solid Electrolyte Interphase Formation on Crystalline Silicon Electrodes: Influence of Electrochemical Preparation and Ambient Exposure Conditions journal September 2012
Silicon Solid Electrolyte Interphase (SEI) of Lithium Ion Battery Characterized by Microscopy and Spectroscopy journal June 2013
Chemical Preinsertion of Lithium: An Approach to Improve the Intrinsic Capacity Retention of Bulk Si Anodes for Li-ion Batteries journal November 2012
In Situ FTIR-ATR Examination of Poly(acrylic acid) Adsorbed onto Hematite at Low pH journal July 2003
Optimization of LiFePO 4 Nanoparticle Suspensions with Polyethyleneimine for Aqueous Processing journal February 2012
Brownian Dynamics Simulations of Colloidal Suspensions Containing Polymers as Precursors of Composite Electrodes for Lithium Batteries journal July 2012
The Structures of Salicylate Surfactants with Long Alkyl Chains in Non-Aqueous Media journal November 2013
Monomer Functionality and Polymer Network Formation journal June 2001
Phase Behavior of Highly Immiscible Polymer Blends Stabilized by a Balanced Block Copolymer Surfactant journal August 2003
Insight into Clustering in Poly(ethylene oxide) Solutions journal September 2004
Behavior of Surface-Anchored Poly(acrylic acid) Brushes with Grafting Density Gradients on Solid Substrates  2. Theory journal November 2007
pH-Responsive Poly(acrylic acid) Core Cross-Linked Star Polymers: Morphology Transitions in Solution and Multilayer Thin Films journal April 2008
Film Thickness Dependence of the Surface Structure of Immiscible Polystyrene/Poly(methyl methacrylate) Blends journal January 1996
Phase Behavior of Blends of Linear and Branched Polyethylenes on Micron Length Scales via Ultra-Small-Angle Neutron Scattering journal April 1999
Polyelectrolyte Charge Effects on Solution Viscosity of Poly(acrylic acid) journal April 1999
Hyperbranched β-Cyclodextrin Polymer as an Effective Multidimensional Binder for Silicon Anodes in Lithium Rechargeable Batteries journal January 2014
Stable Li-ion battery anodes by in-situ polymerization of conducting hydrogel to conformally coat silicon nanoparticles journal June 2013
Breathing silicon anodes for durable high-power operations journal September 2015
Nanostructured silicon for high capacity lithium battery anodes journal January 2011
A coordinatively cross-linked polymeric network as a functional binder for high-performance silicon submicro-particle anodes in lithium-ion batteries journal January 2014
SEI-component formation on sub 5 nm sized silicon nanoparticles in Li-ion batteries: the role of electrode preparation, FEC addition and binders journal January 2015
The pH-responsive behaviour of poly(acrylic acid) in aqueous solution is dependent on molar mass journal January 2016
Revisiting and improving the preparation of silicon-based electrodes for lithium-ion batteries: ball milling impact on poly(acrylic acid) polymer binders journal January 2019
Correlations between structure, material properties and bioproperties in self-assembled β-hairpin peptide hydrogels journal January 2008
Neutron Scattering for Moisture Detection in Foamed Asphalt journal July 2013
Radius of Gyration of Polymer Chains journal January 1962
Solutions of Long Chain Compounds journal May 1941
XPS study of SiO thin films and SiO-metal interfaces journal August 1989
Raman Scattering by Silicon and Germanium journal March 1967
Vibrational properties of amorphous Si and Ge journal March 1975
Dynamic shear modulus of a semiflexible polymer network journal August 1998
High Friction from a Stiff Polymer Using Microfiber Arrays journal August 2006
Colloidal Processing of Silicon Nitride with Poly(acrylic acid): II, Rheological Properties journal September 1998
Forces Measured between Zirconia Surfaces in Poly(acrylic acid) Solutions journal May 1999
Silicon Nitride Colloidal Probe Measurements: Interparticle Forces and the Role of Surface-Segment Interactions in Poly(acrylic acid) Adsorption from Aqueous Solution journal August 2001
The Rheology of Polyelectrolytes. I. Flow Curves of Concentrated Poly(acrylic Acid) Solutions journal March 1961
Rheological Behavior of Filled Polymeric Systems I. Yield Stress and Shear‐Thinning Effects journal October 1988
Rheological Behavior of Filled Polymeric Systems II. The Effect of a Bimodal Size Distribution of Particulates journal November 1988
Technical note: Correlation between the Hamaker constant and the flow behavior index of a concentrated suspension journal November 1990
Relating the shear‐thinning curve to the molecular weight distribution in linear polymer melts journal March 1996
A Major Constituent of Brown Algae for Use in High-Capacity Li-Ion Batteries journal September 2011
Rheological properties of concentrated aqueous solutions of anionic and cationic polyelectrolyte mixtures journal July 2008
Flory-Huggins parameters for weakly crosslinked hydrogels of poly(acrylic acid) and poly(methacrylic acid) with various degrees of ionization journal January 2015
Thermodynamics of High Polymer Solutions journal October 1951
Structural Changes in Silicon Anodes during Lithium Insertion/Extraction journal January 2004
In Situ XRD and Electrochemical Study of the Reaction of Lithium with Amorphous Silicon journal January 2004
Improvements of Dispersion Homogeneity and Cell Performance of Aqueous-Processed LiCoO[sub 2] Cathodes by Using Dispersant of PAA–NH[sub 4] journal January 2006
Alloy Design for Lithium-Ion Battery Anodes journal January 2007
Influence of Binder Coverage on Interfacial Chemistry of Thin Film LiNi 0.6 Mn 0.2 Co 0.2 O 2 Cathodes journal January 2020
Understanding Anomalous Behavior in Coulombic Efficiency Measurements on Li-Ion Batteries journal December 2014
Lithium Ion Cell Performance Enhancement Using Aqueous LiFePO 4 Cathode Dispersions and Polyethyleneimine Dispersant journal November 2012
Chemically Surface Tunable Solubility Parameter for Controllable Drug Delivery—An Example and Perspective from Hollow PAA-Coated Magnetite Nanoparticles with R6G Model Drug journal February 2018
Predicting the Flory-Huggins χ Parameter for Polymers with Stiffness Mismatch from Molecular Dynamics Simulations journal June 2016
X-ray photoelectron spectroscopy of graphitic carbon nanomaterials doped with heteroatoms journal January 2015

Similar Records

Role of Low Molecular Weight Polymers on the Dynamics of Silicon Anodes During Casting
Journal Article · Wed May 05 00:00:00 UTC 2021 · ChemPhysChem · OSTI ID:1805014