A volumetric apparatus to measure hydrogen adsorption and desorption at room temperature and up to 100 atm has been constructed and studied for accuracy, reproducibility, and stability. The design principles are presented and considerable attention to detail is given to examine the effects of diurnal temperature changes in the manifold and helium adsorption by carbon-based adsorbents during free volume measurement. A heuristic for helium correction is derived from a model with a basis in literature and verified through calculation of adsorbent density. Several materials with well-known hydrogen capacities are studied to examine reproducibility. The microporous carbon AX-21 is studied to examine the effects of pressure step size and approach to equilibrium caused by gas mixing and the Joule-Thomson effect. Hydrogen spillover on a hybrid material, Pt on templated carbon, is examined for several loadings of metal. Kinetics of both physisorption and spillover are compared via the diffusion time constant (D/R(2)) estimated by fitting models for pore and surface diffusion to time-dependent adsorption profiles. No concentration dependence was found for pore diffusion; however, the surface diffusion time constant was shown to decrease with respect to increasing hydrogen concentration.