Bridging Dehydrogenation and Hydrogenation in Heterogeneous Catalysis: A Demonstration of a Unified Catalytic Approach

Abstract

In the pursuit of enhancing the applications of hydrogen as an energy carrier, this research delved into the utilization of a singular hybrid catalyst capable of performing both dehydrogenation and hydrogenation processes for Liquid Organic Hydrogen Carriers (LOHCs). This study presents the synthesis and characterization of a hybrid catalyst, combining an organometallic pincer complex with Pd‐Ru heterostructures supported on γ‐alumina. Unlike conventional transition and noble metal nanoparticles, the use of a pincer complex offers exceptional thermal stability due to its aryl backbone, which is advantageous for various endothermic dehydrogenation reactions of hydrocarbons in LOHCs. This pioneering hybrid catalyst is a novel approach, demonstrating a proof of concept. In this study, we utilized the hybrid catalyst to investigate the dehydrogenation and hydrogenation of a lower enthalpic system, specifically the cyclooctane‐cyclooctene system. The dehydrogenation of cyclooctane was conducted at 443 K using tertiary butyl ethylene as a sacrificial hydrogen acceptor, while the hydrogenation of cyclooctene reaction catalyzed by Pd‐Ru nanostructures occurred at 298 K and 1 atm H2. The results showed successful tandem dehydrogenation‐hydrogenation reactions. However, challenges were noted in terms of catalytic activity and recyclability, providing valuable insights for further refinement and optimization.