The separation, storage and recovery of hydrogen are key requirements for the efficient development of advanced hydrogen fuel technologies. The ideal hydrogen separation membrane should have high hydrogen permeability and good mechanical properties at a range of temperatures and pressures. Tantalum is a potential candidate with highest permeability to hydrogen among pure materials for hydrogen separation membrane. Isothermal as well as isobaric PCT equilibrium studies have been done in the temperature range of 673 ? 873 K and hydrogen pressure range of 0.60 ? 1.20 atmospheres for pure Ta and its solid solution alloys with Fe in different compositions. Results are presented.