Reversible Dehydrogenation–Hydrogenation of Cyclohexanol–Cyclohexanone Pair Over Ru/Hierarchical Zeolite Catalyst

We report a reversible dehydrogenation–hydrogenation of cyclohexanol–cyclohexanone pair over Ru supported on Hierarchical Zeolite (Ru/HZ4A) under neat conditions. The catalyst Ru/HZ4A demonstrated high activity for both dehydrogenation of cyclohexanol to cyclohexanone (at 160°C) and hydrogenation of cyclohexanone back to cyclohexanol (60°C) with appreciably high selectivity and conversion. Moreover, the catalyst Ru/HZ4A displayed high durability under bulk and recyclability experiments, achieving hydrogen productivity as high as 156 L H2 /g Ru (STY 89 mmol H2 /g Ru /h). The developed protocol was also applied to 5‐membered and 8‐membered cycloalkanol–cycloalkanone pairs with excellent selectivity for a one‐pot reversible dehydrogenation–hydrogenation cycle. These findings underscore the potential of the developed catalytic system for a reversible hydrogen storage system.