The high energy planetary milling process was applied successfully to improve the ionic conductivity of cesium hydrogen sulfate (CsHSO4). Electrochemical impedance spectroscopy measurements indicate that 3 h of mechanochemical pulverization by ballmilling quadrupled the ionic conductivity of CsHSO4. It was found via electrolytic splitting of (100%) hydrogen sulfide content feed gas at 150 degrees C that the exchange current density improved by over 70% using modified CsHSO4 when compared to the unmodified CsHSO4. As a result, mechanochemical pulverization shows good promise in minimizing activation barriers frequently encountered in an electrolytic synthesis that uses CsHSO4-based membranes.