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This thesis systematically investigates the properties of the aluminium adherend which influence the fracture toughness of aluminium-epoxy adhesive joints in humid environments. The fracture energy of the adhesive joint exposed to a humid environment in comparison with the fracture energy in a dry environment provides a measure of the joint durability. A 500C and 95% relative humidity environment is used to simulate aging of an adhesive joint over several years under normal service conditions. Initially, surface roughness is found to have a significant influence on the fracture toughness of the adhesive joint in humid conditions. A direct correlation between the bond durability and the angle of deliberately machined micro-roughness in the aluminium surface is determined. Consequently a model is developed which initially has the capacity to describe the bond durability performance. The preparation of aluminium surfaces involves the use of a novel ultramilling tool to produce well defined and controlled surface topography. This work represents the first time surface angles of features in the 1????m to 10????m range have been systematically varied and a direct relationship with bond durability has been determined. The use of surface analytical tools aids in elucidating mechanisms involved in the failure of the adhesive joint and contributes to the development of the stress based diffusion model. Examination of the aluminium oxide hydration level reveals this property has a negligible effect on the fracture toughness of the aluminium-epoxy joints exposed to humid environments. This information confirms the dominant role of the physical properties of the aluminium surface in determining the adhesive joint durability. This is the first occasion that planer oxide films grown in an RF plasma have had their hydration state adjusted in a controlled manner and their properties subsequently assessed in terms of bond durability properties. Further alteration of the aluminium surface chemistry is achieved through the application of an organo-silane coupling agent and a series of novel organo-phosphonate compounds. This work further develops the stress based diffusion model developed in conjunction with the micro-machining studies. The components of surface roughness and the ability of interfacial bonds to co-operatively share load are essential for the maintenance of fracture toughness of adhesive joints exposed to humid conditions. The ability of the silane coupling agent to share load through a chemically cross-linked film is a significant property which provides the superior fracture toughness in comparison with the phosphonate treated joints. Although the organo-phosphonate treated aluminium provides hydrolytically more stable bonds than the silane coupling agent, the film is not cross-linked via primary chemical bonds and the reduced load sharing capacity of interfacial bonds increases the bond degradation rate. The stress based diffusion model evolving from the initial work in the thesis can be used to predict the performance of more complex systems based on a thorough characterisation of the aluminium surface chemistry and topography. The stress based diffusion model essentially describes the concept of the production of micro-cavities at the epoxy-aluminium interface under mode 1 load, as a result of the distribution of strong and weak adhesive bonds. Alternatively, micro-cavities may result from an inhomogeneous stress distribution. In areas where the adhesive bonds are weak, or the local stresses are high, the interfacial load produces larger micro-cavities which provide a path of low resistance for water to diffuse along the bond-line. The water then degrades the adhesive bond either through the displacement of interfacial epoxy bonds or the hydration of the oxide to form a weak barrier layer through which fracture can occur. Alternatively, the water can hydrolyse the adhesive in the interfacial region, leading to cohesive failure of the epoxy resin. The bond durability performance of a series of complex hydrated oxide films used to pre-treat the aluminium adherend provides support for the stress based diffusion model. Whilst surface area is an important property of the aluminium adherend in producing durable bonding, the best durability achievable, between an epoxy adhesive and aluminium substrate, requires a component of surface roughness which enhances the load sharing capability in the interfacial bonding region. This component of durability performance is predicted by the model. In more specific terms, a boiling water treatment of the aluminium adherend indicates a direct correlation between bond durability, surface area and topography. The characterisation of film properties indicates that the film chemistry does not change as a function of treatment conditions, however, the film topography and surface area does. The overall bond durability performance is linked to both of these properties. The detailed examination of the hydrated oxide film, produced by the boiling water treatment of aluminium, is the first time the bond durability performance has been related to the film topography. It is also the first occasion that the mechanism of film growth has been examined over such a large treatment time. The combination of surface analysis and bond durability measurements is invaluable in confirming the properties, predicted by the stress based diffusion model, which are responsible in forming fracture resistant adhesive bonds in humid conditions. The bond durability of high surface area and low surface area hydrated oxide films indicates that surface area is an important property. However, this study confirms that the absence of the preferred surface topography limits the ultimate bond durability performance attainable. The fracture toughness measurements performed on aluminium adherends pre-treated with a low surface area film also supports the mechanism of load sharing of interfacial adhesive bonds and its contribution to the overall bond durability. The role performed by the individual molecules and particles in an oxide film is similar to the load sharing performed by the silane coupling agent molecules. Further support for the stress based diffusion model is provided by films produced on aluminium immersed in nickel salt solutions. The topography of these film alters as a function of treatment time and this is directly related to fracture toughness in humid environments. This work provides the first instance where such films have been characterised in detail and their properties related to bond durability performance. The study is also the first time that the growth mechanism of the film produced on the aluminium substrate has been examined in detail. The film growth mechanism supports the film growth model proposed for the hydrated oxide film produced by the boiling water treatment. The major findings presented in this thesis are summarised as the direct correlation between surface profile angle, the importance of co-operative load sharing of interfacial adhesive bonds and the relative insignificance of surface oxide hydration in the formation of durable aluminium-epoxy adhesion. This information is used to develop a stress based diffusion model which has the capacity to describe the fracture toughness of a range of aluminium-epoxy adhesive joint systems in humid environments. The stress based diffusion model is also capable of predicting the relative performance of the bond systems examined in the final chapters of the thesis, where complex interfacial oxide films are involved in the formation of adhesive bonds.

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