There are economic incentives to extend service of CANDU nuclear reactors in Ontario because of their reputation for safety and reliability. Pressure tubes made of zirconium alloys are vulnerable to failure by Delayed Hydride Cracking (DHC), which limits the amount of hydrogen, stress, temperature, and service life. Recreating reactor end-of-life conditions for testing purposes requires a method of adding hydrogen quantitatively into zirconium alloys without modifying irradiation damage.The thesis demonstrates a promising mechanical hydriding technique that is suitable for adding hydrogen beyond the conventional solubility limit into zirconium alloys at 200 °C within hours, with 99 % accuracy and 3 % precision based on massbalance. The technique can be used to map the Zirconium-Hydride phase system. Results attributed to the delta ( -ZrHx) solvus have been measured and agree with reported values. Confidence in the model is reinforced by the determination of hydrogen solubility in a copper barrier, which was found to agree with theoretical predictions. 5.2.