Publications

Showing 15 results for Author: Luke A. Heroux

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Dec, 2023

Journal

Understanding the Solution Dynamics and Binding of a PVDF Binder with Silicon, Graphite, and NMC Materials and the Influence on Cycling Performance

The impact of the binding, solution structure, and solution dynamics of poly(vinylidene fluoride) (PVDF) with silicon on its performance as compared to traditional graphite and Li1.05Ni0.33Mn0.33Co0.33O2 (NMC) electrode materials was explored. Through refractive index (RI) measurements, the concentration of the binder adsorbed on the surface of electrode materials during e…
Dec, 2023

Journal

Understanding the Solution Dynamics and Binding of a PVDF Binder with Silicon, Graphite, and NMC Materials and the Influence on Cycling Performance

The impact of the binding, solution structure, and solution dynamics of poly(vinylidene fluoride) (PVDF) with silicon on its performance as compared to traditional graphite and Li1.05Ni0.33Mn0.33Co0.33O2 (NMC) electrode materials was explored. Through refractive index (RI) measurements, the concentration of the binder adsorbed on the surface of electrode materials during e…
Nov, 2023

Journal

The suite of small-angle neutron scattering instruments at Oak Ridge National Laboratory

Oak Ridge National Laboratory is home to the High Flux Isotope Reactor (HFIR), a high-flux research reactor, and the Spallation Neutron Source (SNS), the world's most intense source of pulsed neutron beams. The unique co-localization of these two sources provided an opportunity to develop a suite of complementary small-angle neutron scattering instruments for studies of la…
Nov, 2023

Journal

AGES: Automated Gas Environment System for in situ neutron powder diffraction

High fluxes available at modern neutron and synchrotron sources have opened up a wide variety of in situ and operando studies of real processes using scattering techniques. This has allowed the user community to follow chemistry in the beam, which often requires high temperatures, gas flow, etc. In this paper, we describe an integrated gas handling system for the general-p…
Nov, 2023

Journal

Understanding Binder–Silicon Interactions during Slurry Processing

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 s…
Nov, 2023

Journal

Role of low molecular weight polymers on the dynamics of silicon anodes during casting

This work probes the slurry architecture of a high silicon content electrode slurry with and without low molecular weight polymeric dispersants as a function of shear rate to mimic electrode casting conditions for poly(acrylic acid) (PAA) and lithium neutralized poly(acrylic acid) (LiPAA) based electrodes. Rheology coupled ultra-small angle neutron scattering (rheo-USANS)…
Nov, 2023

Journal

A Unified User-Friendly Instrument Control and Data Acquisition System for the ORNL SANS Instrument Suite

In an effort to upgrade and provide a unified and improved instrument control and data acquisition system for the Oak Ridge National Laboratory (ORNL) small-angle neutron scattering (SANS) instrument suite—biological small-angle neutron scattering instrument (Bio-SANS), the extended q-range small-angle neutron scattering diffractometer (EQ-SANS), the general-purpose small-…
Nov, 2023

Journal

Probing Clustering Dynamics between Silicon and PAA or LiPAA Slurries under Processing Conditions

This work explores the complex interplay between slurry aggregation, agglomeration, and conformation (i.e., shape) of poly(acrylic acid) (PAA)- and lithiated PAA-based silicon slurries as a function of the shear rate and the resulting slurry homogeneity. These values were measured by small-angle neutron scattering (SANS) and rheology-coupled ultra-SANS at conditions releva…
Nov, 2023

Journal

Competitive adsorption within electrode slurries and impact on cell fabrication and performance

Why do battery researchers use 10–20 wt% binder in research cells when commercial chemistries use much less? This report seeks to explore this question by understanding the ordering and structure of polyimide binder with a silicon/pitch-carbon black electrode system. Correlating the effect of binder concentration on electrode architecture and electrochemical properties is…
Nov, 2023

Journal

Structure and dynamics of small polyimide oligomers with silicon as a function of aging

The effect of UV curing and shearing on the structure and behavior of a polyimide (PI) binder as it disperses silicon particles in a battery electrode slurry was investigated. PI dispersant effectiveness increases with UV curing time, which controls the overall binder molecular weight. The shear force during electrode casting causes higher molecular weight PI to agglomerat…
Sep, 2023

Journal

Origin of rate limitations in solid-state polymer batteries from constrained segmental dynamics within the cathode

Currently, one of the key challenges preventing the wide commercialization of polymer-based solid-state batteries is achieving high-rate capabilities. This work unravels chain structure and segmental dynamics in a polymer-based composite cathode consisting of LiFePO4 (LFP), carbon, and poly(ethylene oxide) (PEO) with lithium bis(trifluoromethanesulfonyl)imide. Small-angle…
Feb, 2022

Journal

Controlling the Morphology of PEDOT:PSS Blend Films with Pre-Deposition Solution Composition and Deposition Technique

Understanding the relationships between morphology, fabrication processes, and thermoelectric performance in conducting polymers is essential to the development of high- efficiency organic thermoelectrics as an alternative to commonly used rare metals. Altering the film fabrication process of poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS) with the add…

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Publications

Understanding the Solution Dynamics and Binding of a PVDF Binder with Silicon, Graphite, and NMC Materials and the Influence on Cycling Performance

Understanding the Solution Dynamics and Binding of a PVDF Binder with Silicon, Graphite, and NMC Materials and the Influence on Cycling Performance

The suite of small-angle neutron scattering instruments at Oak Ridge National Laboratory

AGES: Automated Gas Environment System for in situ neutron powder diffraction

Understanding Binder–Silicon Interactions during Slurry Processing

Role of low molecular weight polymers on the dynamics of silicon anodes during casting

A Unified User-Friendly Instrument Control and Data Acquisition System for the ORNL SANS Instrument Suite

Probing Clustering Dynamics between Silicon and PAA or LiPAA Slurries under Processing Conditions

Competitive adsorption within electrode slurries and impact on cell fabrication and performance

Structure and dynamics of small polyimide oligomers with silicon as a function of aging

Origin of rate limitations in solid-state polymer batteries from constrained segmental dynamics within the cathode

Controlling the Morphology of PEDOT:PSS Blend Films with Pre-Deposition Solution Composition and Deposition Technique