Concrete is the most widely used construction material in the world. Given its relative availability, strength, economy, and versatility to fit various applications, the material has been incorporated in roadways, bridges, buildings, and a host of other infrastructure projects. Oftentimes, concrete will be exposed to several environmental conditions that ultimately affect its durability and lifespan. These conditions include repeated freezing and thawing, chloride intrusion, sulfate attack, alkali-silica reaction, and many others. Given the age and condition of American infrastructure, concrete structures throughout the country need repair or rehabilitation. Often this repair includes the removal of degraded or damaged concrete and the application of an overlay material. There are several factors affecting the bond performance of the newly formed substrate-repair concrete, such as surface roughness, overlay material, and substrate moisture condition. The work presented in this thesis is dedicated to understanding the effect of substrate moisture condition on the overlay transition zone (OTZ) of the substrate-repair concrete. The substrate moisture condition can significantly impact the microstructure characterization of the OTZ. If the substrate is too dry, then it may absorb water from the repair material, reducing the local water-to-cement (w/c) ratio in the OTZ. Conversely, if the substrate is too wet, then the w/c ratio of the OTZ will be locally increased. In both scenarios, the interfacial bond strength is expected to be modified due to the change in the local w/c ratio. To understand this effect, various test methods and degradation mechanisms were explored. Initially, substrate-repair concrete specimens were prepared utilizing three separate substrate moisture conditions: saturated surfaced dry (SSD), sub-saturated surface dry (Sub-SSD), and oven dry (OD). After allowing these samples to cure, the strength and ion penetration risk were evaluated. The bond strength of the samples was evaluated through flexural strength testing and fracture energy determined through the RILEM draft tests. The OTZ ion penetration risk was evaluated by conducting rapid chloride penetration test (RCPT) on samples prepared with the three substrate moisture conditions. Furthermore, to determine the effect of repeated freezing and thawing on the OTZ and flexural strength, additional samples were created with the three moisture conditions. After allowing these samples to cure, they were subjected to ASTM C666 and were tested to observe their flexural strength. Another important performance indicator of concrete elements is its resistance to chloride ion penetration and corrosion. Since many structural elements are designed with steel reinforcement, chloride ion penetration represents a critical parameter in projecting material performance, since chloride ions will accelerate the rate of steel corrosion. Oftentimes, a key element in projecting this performance is identifying the rate at which ions diffuse through the material. There remain many established techniques to identify this rate of diffusion and derive a chloride diffusion coefficient; however, many of them are either destructive or qualitative in nature. In recent years, transmission X-ray microscopy (TXM) has been employed to non-destructively track diffusion and develop diffusion coefficients. The work presented in this thesis surrounds the efforts of incorporating TXM experiments at Virginia Tech. This work initially utilized a SkyScan 1174 μCT, and additional work in this thesis presents the design and construction of a dental X-ray system based on the checking ion penetration (CHIP) design. This system can conduct TXM experiments utilizing a dental X-ray as the source. The research, design, and construction of the CHIP system is discussed in this thesis. Ultimately, the research in this thesis has not observed any significant relationship between substrate moisture condition and overlay bond strength. There does appear to be an increase in chloride ion resistance for drier substrates, suggesting that pre-wetting the surface increases penetrability of the interface. / Master of Science / Concrete is the most widely used construction material in the world. Given its relative availability, strength, economy, and versatility to fit various applications, the material has been incorporated in roadways, bridges, buildings, and a host of other infrastructure projects. Oftentimes, concrete will be exposed to several environmental conditions that ultimately affect its durability and lifespan. These conditions include repeated freezing and thawing, chloride intrusion, sulfate attack, alkali-silica reaction, and many others. These environmental conditions ultimately degrade the material by inducing cracks, exposing steel reinforcement, and spalling. When the concrete has experienced significant deterioration, repair and rehabilitation of the damaged section must be performed. Most often, this repair consists of the removal of damaged concrete and the application of an overlay material to prevent further deterioration. The topics discussed in this thesis evaluate the optimum substrate conditions prior to an overlay application and the implementation of techniques to evaluate deterioration mechanisms. There are several substrate conditions that will affect bonding with the overlay material, including surface roughness, moisture conditions, and overlay type. This paper focused on the moisture condition and what effect this had on bond strength and resistance to chloride intrusion. This effect was studied in laboratory conditions and under environmental conditions such as rapid freezing and thawing. Several different deterioration mechanisms may contribute to concrete degradation. The research presented in this thesis also aimed to evaluate chloride ion diffusion. To evaluate this mechanism, two systems were explored with the intent of conducting transmission X-ray microscopy (TXM). With TXM, chloride ion diffusion can be tracked to determine the rate at which ions diffuse through the concrete. The two systems explored were an X-ray computed tomography scanner and a dental X-ray system. Both systems can conduct TXM, and this paper presents the efforts dedicated to developing them for this technique at Virginia Tech. Ultimately, the research in this thesis has not observed any significant relationship between substrate moisture condition and overlay bond strength. There does appear to be an increase in chloride ion resistance for drier substrates, suggesting that pre-wetting the surface increases penetrability of the interface.