The present study investigates hydrogen purification from a surrogate gas using spent coffee grounds as a medium. The study was conducted using Aspen adsorption software, and the process was examined under isothermal, adiabatic, and non-adiabatic conditions. The surrogate gas mixture comprised 70% hydrogen and 30% carbon dioxide and was introduced into two stainless steel chambers containing the coffee media. The pressure was altered from 101.3 to 150 kPa as the chamber underwent the adsorption process. At an adsorption time of 60 s, all three conditions exhibited similar levels of purity and recovery, with the isothermal mode producing the highest values. Additionally, the effect of heat dissipation and column geometry on the adsorption performance was investigated by comparing the conventional isothermal column with the rectangular non-adiabatic plate column. The plate column is rectangular, with two chambers that use the heat generated during adsorption to regenerate the opposite column during the blowdown step. This effect was evaluated under different adsorption times of 30–180 s and hydrogen feed concentrations of 70–90%. The plate column had higher hydrogen purity and recovery of 99.99% and 77.41%, respectively, compared to 99.56 and 71.12% of the cylindrical column. Overall, the results indicate that spent coffee grounds can be effectively used as a medium to purify hydrogen from a surrogate gas mixture. A rectangular non-adiabatic plate column can further enhance the purification process by improving purity and recovery responses.