Cementitious materials, together with other materials, are being considered to seal a potential repository at Yucca Mountain. A concern with cementitious materials is the chemical and mineralogic changes that may occur as these materials age while in contact with local ground waters. A combined theoretical and experimental approach was taken to determine the ability to theoretically predict mineralogic changes. The cementitious material selected for study has a relatively low Ca:Si ratio approaching that of the mineral tobermorite. Samples were treated hydrothermally at 200°C with water similar to that obtained from the J-13 well on the Nevada Test Site. Post-test solutions were analyzed for pH as well as dissolved K, Na, Ca, Al, and Si. Solid phases formed during these experiments were characterized by scanning electron microscopy and X-ray diffraction. These findings were compared with predictions made by the geochemical modeling code EQ3NR/EQ6. It was generally found that there was good agreement between predicted and experimental results.