Abstract
Storage of hydrogen, particularly liquid organic hydrogen carrier (LOHC), has attracted much attention to address the problem of safe storage and transport of H2. N-heterocycles are promising hydrogen carriers for storing/releasing hydrogen through reversible catalytic hydrogenation/dehydrogenation cycles. Therefore, designing cost-effective, efficient, reusable single catalysts for both processes with high catalytic activity is currently of interest. Herein, we report the successful preparation of atomically dispersed Co/Zn single-atom catalysts on nitrogen-doped carbon by pyrolysis of bimetallic CoxZny-MOF-508@Melamine. The synthesized CoxZny-NC catalyst showed highly efficient catalytic activity for the reversible hydrogenation and dehydrogenation of quinoline derivatives in the same solvent. Catalytic reversible hydrogen storage/release was demonstrated for three consecutive cycles without losing efficiency. The main features of this work require low loading of catalysts compared to reported heterogeneous non-precious metal catalysts. A control experiment revealed that free N-H groups/N-atoms are essential for dehydrogenation/hydrogenation reactions, and a possible reaction mechanism was proposed.
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