Hydrogen storage in a depleted gas field is a promising solution to the seasonal storage of renewable energy, a key question in Europe’s green transition. The gas composition and pressure in the month-long storage and recovery phase can vary substantially; meanwhile, the recovered H₂ has to be pure, especially for fuel cell applications. Pressure swing adsorption can be used for the purification of the recovered gas. A lab-scale, four-bed PSA unit was built to investigate its applicability by separating different H₂-CH₄ mixtures. The feed parameters in the experiments are based on a depleted gas reservoir with a pressure range of 25–60 bar and methane contamination between 0 and 35%. The change in the feed properties is modeled by four distinct stages and the twelve-step cycle is tailored to each stage. The high pressure did not have any irreversible effects on the process. A hydrogen purity of 99.95% was achieved in all stages with the average hydrogen recovery ranging from 60 to 80%. The experiments revealed the challenges of a cycle design when the feed parameters are not constant, but an adequate separation performance was shown, which supports the applicability of the PSA in seasonal storage and confirms the need for further investigation with multicomponent contaminants and large-scale projects.

Pressure swing adsorption (PSA) is a viable method for separating hydrogen from gas mixtures, an important aspect of long-term hydrogen storage in depleted gas fields. This study explores optimizing a 12-step PSA process for recovering high-purity hydrogen from varying compositions of hydrogen–methane mixtures, simulating the conditions likely encountered during hydrogen storage and recovery. Step-time optimization was performed on four different hydrogen–methane mixtures using the toPSAil simulation package—an open-source dynamic PSA simulator developed by researchers at the Georgia Institute of Technology—integrated with a particle swarm optimization (PSO) algorithm. The goal was to develop an optimization framework that can reliably identify PSA step times for different operating scenarios and satisfy specified purity and recovery constraints under fluctuating wellhead feed conditions. The optimization converged within 25–30 iterations, even in high-contaminant, low-pressure scenarios, where PSA performance is traditionally weak. The product purity in the optimized cycles was above 99.1% with more than 80% recovery for all cases, while fuel cell quality (99.7%) hydrogen was achieved in two out of the four scenarios. The purge-to-feed ratio of the best-performing cycles was between 0.07 and 0.32. These findings show the potential of the proposed approach in overcoming the difficulty of designing PSA cycles for non-constant gas compositions and achieving a hydrogen purification process suitable for variable feed conditions. The workflow generates a large synthetic dataset that can support surrogate or hybrid modeling. The results can help advance research in other gas separation areas with non-constant conditions, like flue gas or biogas purification.