Overcoming Barriers in Electrochemical Toluene Hydrogenation for Efficient Hydrogen Storage by Pt₃Au Alloy Catalysts

Hydrogen storage and transportation are essential for the hydrogen economy, and liquid organic hydrogen carriers (LOHCs), such as a toluene/methylcyclohexane (TOL/MCH) system, offer significant advantages in terms of safety and efficiency. However, the electrochemical reduction of TOL to MCH (TER) faces challenges from competing with the hydrogen evolution reaction (HER) and catalyst instability. In this study, Pt3Au is introduced as a highly effective catalyst for TER. Through density functional theory screening, we identified distinctive properties of Pt3Au, including enhanced binding to the TER intermediates and effective HER suppression. Experimental validation confirmed these computational predictions, with Pt3Au achieving the highest reported Faradaic efficiency (98%) in proton exchange membrane systems. Moreover, long-term testing demonstrated that Pt3Au maintained Faradaic efficiencies of >90% over 9 h, highlighting its robustness and operational stability. By integrating computational modeling and experimental evaluation, this work addresses key limitations in LOHC catalysis. Pt3Au establishes a benchmark for selective and stable TER performance, paving the way for advanced hydrogen storage technologies. These findings emphasize the critical role of rational catalyst design in overcoming the challenges associated with scalable and efficient hydrogen storage solutions.