A proton exchange membrane fuel cell system (PEMFCS) operated electroytically at its limiting current was proposed previously as a technology to separate H 2 and He through the electrochemical oxidation of H 2 . In this work the fraction of H 2 remaining in the effluent of two different sized PEMFCs with different flow field designs was studied at several operating conditions which included different: system temperatures, inlet relative humidity (R.H.), and system pressures to determine the most efficient operating condition. Experiments were performed at a fixed dry gas flow rate with an inlet H 2 dry gas fraction of 10 %. System performance was found to depend significantly on operating conditions with optimum performance attained at 60 ºC and 100 % R.H. for both system sizes. To assist in the performance modeling of each system a differential chemical reactor model was used to determine H 2 mass transport coefficients at each operating condition.