Cynthia F. Welch

The Couette configuration of the Los Alamos Neutron Science Center Neutron Rheometer for the investigation of polymers in the bulk via small-angle neutron scattering

A neutron rheometer in the Couette geometry has been built at the Los Alamos Neutron Science Center to examine the molecular steady-state and dynamic responses of entangled polymeric materials in the bulk under the application of shear stress via small-angle neutron scattering. Although similar neutron rheometers have been fabricated elsewhere, this new design operates under the extreme conditions required for measuring the structure and behavior of high molecular weight polymer melts. Specifically, the rheometer achieves high torques (200 N m) and shear rates (865 s(-1)) simultaneously, never before attainable with other neutron rheometers at temperatures up to 240 degrees C under an inert gas environment. The design of the instrument is such that relatively small sample sizes are required. The testing of the Los Alamos Neutron Science Center Neutron Rheometer in the Couette design both as a rheometer and in the small-angle neutron optical configuration on highly viscous polystyrene is presented. The observed anisotropic neutron scattering pattern of the polystyrene melt at a molecular weight above entanglement provides evidence that the conformation of the polymer chains are elongated in the direction of the melt flow, in agreement with the current theories concerning linear polymers in the bulk.

Mixed Hydrocarbon/Fluoropolymer Membrane/Ionomer MEAs for Durablity Studies

The durability of polymer electrolyte membrane (PEM) fuel cells is a major barrier to the commercialization of these systems for stationary and transportation power applications. Commercial viability depends on improving the durability of the fuel cell components to increase the system reliability. The aim of this work is to separate ionomer degradation from membrane degradation via mixed membrane / ionomer MEA experiments. The challenges of mixed MEA fabrication due to the incompatibility of the membrane and the electrode are addressed. OCV accelerated testing experiments (AST) were performed. Development of in situ diagnostics and unique experiments to characterize the performance and properties of the ionomer in the electrode as a function of time are reported. These measurements, along with extensive ex situ and post-mortem characterization, can delineate the degradation mechanisms in order to develop more durable fuel cells and fuel cell components.

Polymers in Membrane Electrode Assemblies

This chapter is devoted to polymer electrolytes for use in membrane electrode assemblies of proton exchange membrane fuel cells. This chapter starts with a discussion of structure–property relationships of polymer electrolytes used as proton exchange membranes, in terms of water uptake, conductivity, and methanol permeability. The second part discusses polymer electrolytes used as electrode ionomers, specifically the structural effects of ionomer composition, ion exchange capacity, hydrophobicity, and dispersing solvent on fuel cell performance. The issue of interfacial compatibility between membrane and electrode is also discussed.

The Los Alamos Neutron Science Center neutron rheometer in the cone and plate geometry to examine tethered polymers/polymer melt interfaces via neutron reflectivity

Although several other neutron rheometers have been built to study soft matter under nonequilibrium conditions, none of them have the ability to measure the structure and behavior of the polymeric interfacial regions in highly viscous polymer melts which require high torques/high strain rates and high temperatures. A neutron rheometer in the cone and plate geometry has been constructed at the Los Alamos Neutron Science Center to rectify this lack of experimental instrumentation. It is also the first-of-its-kind to perform neutron reflectivity studies concurrently with rheological measurements. The details of both the development and testing of the Los Alamos Neutron Science Center neutron rheometer in the cone and plate configuration are described. Proof of principle neutron reflectivity results of end-grafted polystyrene against an identical melt under shear are presented, showing qualitatively that the structural attributes of the end-grafted polymer change when exposed to shear.

Eigenvector centrality is a metric of elastomer modulus, heterogeneity, and damage

We present an application of eigenvector centrality to encode the connectivity of polymer networks resolved at the micro- and meso-scopic length scales. This method captures the relative importance of different nodes within the network structure and provides a route toward the development of a statistical mechanics model that correlates connectivity with mechanical response. This scheme may be informed by analytical and semi-analytical models for the network structure, or through direct experimental examination. It may be used to predict the reduction in mechanical performance for heterogeneous materials subjected to specific modes of damage. Here, we develop the method and demonstrate that it leads to the prediction of established trends in elastomers. We also apply the model to the case of a self-healing polymer network reported in the literature, extracting insight about the fraction of bonds broken and re-formed during strain and recovery.

Sylgard® Mixing Study

Sylgard® 184 and Sylgard® 186 silicone elastomers form Dow Corning® are used as potting agents across the Nuclear Weapons Complex. A standardized mixing procedure is required for filled versions of these products. The present study is a follow-up to a mixing study performed by MST-7 which established the best mixing procedure to use when adding filler to either 184 or 186 base resins. The most effective and consistent method of mixing resin and curing agent for three modified silicone elastomer recipes is outlined in this report. For each recipe, sample size, mixing type, and mixing time was varied over 10 separate runs. The results show that the THINKY™ Mixer gives reliable mixing over varying batch sizes and mixing times. Hand Mixing can give improved mixing, as indicated by reduced initial viscosity; however, this method is not consistent.