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This thesis considers the modelling of two and three dimensional molecular networks with a view to being able to predict how the geometry of a network will affect the elastic constants and specifically the Poisson's ratios of the network. Materials with negative Poisson's ratios have much better engineering properties then those with positive Poisson's ratios. Theory states that a network polymer, with negative Poisson's ratios at a molecular level, would have much better properties than most materials with negative Poisson's ratios made to date. Molecular modelling has been used to examine the elastic constants of those two and three dimensional network polymers which are most likely to be synthesised in the near future. Such networks have been predicted to have either large positive or large negative Poisson's ratios depending on the molecular arrangement of the network. Poisson's ratios varying between 0.96 and -0.86 for the three dimensional cases and between -0.9 and 1.26 for the two dimensional cases have been calculated. Young's moduli in the order of 1 GPa have been observed for the three dimensional networks as compared to Young's moduli in the order of 20 - 400 kPa which have been experimentally measured for foam materials. Comparison with local density functional calculations for two 2-D networks with the molecular modelling have confirmed the negative Poisson's ratio in these networks and shown that it is not a function of the molecular modelling packages or force field used. The off-axis properties for both the two and three dimensional networks have been calculated. These show that whilst the networks with a positive Poisson's ratio in the principal axis directions always have a positive Poisson's ratio, those networks with a negative Poisson's ratio in the principal axis directions have off-axis Poisson's ratios that vary between large and positive and large and negative. In general the networks with positive Poisson's ratios are much more isotropic than those with negative Poisson's ratios. Analytical models which model the networks using simple beam theory have been produced for various two and three dimensional networks. These models can be used to predict the elastic constants of a network without the need to do time consumingmolecular modelling calculations to a first approximation. Comparison of the molecular models and analytical models has led to the development a library of force constants for two dimensional networks which can be used to more accurately predict the elastic constants of a network based on a knowledge of the geometry of the network and the constituent `sub-units' from which it is made

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Negative Linear Compressibility (NLC), where a material expands in a given direction when subjected to hydrostatic compression, is a rare elastic property that has received much attention recently, but has yet to be used in practical applications. What are the mechanisms responsible for this property in crystals and man-made structures? Are all mechanisms somehow related to the wine-rack model? Can we find an even simpler and more fundamental elucidation of NLC? Following this mechanistic approach, can we then identify “engineering” materials with NLC? To answer these questions, I have used a combination of analytical modelling based on beam theory and finite element analysis, to investigate several structures. At first, I examine in great detail the standard wine-rack in 2D and equivalents in 3D and identify the aspect ratio (close to two) at which NLC is maximum. By adding spacers I demonstrate that a cross is not a necessary condition, and that simpler angle changes in chains are sufficient to generate NLC. Looking for materials with intersecting straight chains, “zig-zag” chains or quasi-helical structures, I find that carbon fibre mats, some extruded polymers and some woods exhibit NLC. Finally, I show that elliptical voids in 2D sheets can also generate NLC in a way related to the wine-rack. This thesis improves the understanding of the mechanism(s) responsible for NLC by proving that a wine-rack is not necessary. Perhaps more importantly it suggests that the property can be exploited in several relatively common materials.

This thesis focuses on the development, parameterization and optimization of a novel meso-scale pattern used to induce auxetic behavior, i.e., negative Poisson's ratio, at the bulk scale. Currently, the majority of auxetic structures are too porous to be utilized in conventional load-bearing applications. For others, manufacturing methods have yet to realize the meso-scale pattern. Consequently, new auxetic structures must be developed in order to confer superior thermo-mechanical responses to structures at high temperature. Additionally, patterns that take into account manufacturing limitations, while maintaining the properties characteristically attached to negative Poisson's Ratio materials, are ideal in order to utilize the potential of auxetic structures. A novel auxetic pattern is developed, numerically analyzed, and optimized via design of experiments. The parameters of the meso-structure are varied, and the bulk response is studied using finite element analysis (FEA). Various attributes of the elasto-plastic responses of the bulk structure are used as objectives to guide the optimization process

The performance of peristaltic pumps is mainly governed by their tubing or hose materials. Research and development in this area is therefore very important for peristaltic pump manufacturers to keep in front of the competition and to open up new applications to enable further market penetration. Another aspect of this is of course price; performance and cost have to be in balance. As an approach to fabricate a new tube material, the field of negative Poisson's ratio (or: auxetic) materials is explored. The combined deformations of tensile, compression and shear in a peristaltic pump tube may well benefit from the specific characteristics of auxetic materials. Materials can be designed to keep their dimensions constant in directions perpendicular to an applied load. This is referred to as “auxetic balancing”. Finite element modelling shows that lowering the Poisson's ratio will rapidly decrease the maximum stresses in the cross-section of an occluded tube. Optimum values for the Poisson's ratio are found to be between −0.1 and +0.1, preferentially being 0. The re-entrant honeycomb structure is selected for initial trials, but manufacturing of this structure at the desired dimension proved to be too difficult at this time. Instead, electrospun nanofibre membranes are selected as the reinforcement structure. A liquid silicone elastomer is used as the matrix material. Key characteristics for the new material are derived from baseline test results on existing tubing. Laminates are manufactured from electrospun nylon6 nanofibre membranes coated with a liquid silicone rubber. Compression moulding is used to cure the nylon6-silicone rubber laminate, to give two effects: it ensures impregnation of the membrane and the compression deforms the nanofibre structure in such a way that it will become auxetic through-the-thickness. Flat sheet laminates of 2 mm thickness are manufactured with 14 layers of reinforcement. A reinforcing effect and substantial lowering of the through-the-thickness Poisson's ratio is observed for the laminates at low strains. At higher strains (>50%) the effect of the reinforcement diminishes and the Poisson's ratio of the laminate and pure silicone rubber equalises. Finally, tubular laminates are manufactured and the resulting tubes are tested in a peristaltic pump with some promising results (>1 million occlusions before failure). Tube performance is not yet at the required level, but with further optimisation of the laminating process, mould design and (post-)curing large steps forward can be made.

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