Research Projects

The shift toward a hydrogen-powered energy system demands the creation of reliable, safe, and sustainable methods for hydrogen storage and release. Traditional approaches, such as high-pressure tanks or complex cryogenic setups, are costly and pose significant safety risks when scaled up. Liquid Organic Hydrogen Carriers (LOHCs) offer a promising alternative, as they can reversibly bind hydrogen and be transported as liquids under normal conditions, utilizing the existing fuel distribution infrastructure. Within this class of materials, N-heterocyclic compounds stand out due to their high hydrogen storage capacity, adaptable thermodynamic profiles, and structural versatility. This project outlines a sustainable approach for hydrogen release from hydrogen-rich N-heterocyclic Liquid Organic Hydrogen Carriers (LOHCs) through acceptorless dehydrogenation (AD), utilizing electrochemical and photochemical methods without the need for preexisting unsaturation. Conventional thermal dehydrogenation typically depends on high operating temperatures and expensive noble metal catalysts, which hinder both cost-effectiveness and environmental sustainability. In contrast, this work focuses on leveraging low-potential electrooxidation and visible-light-induced photocatalysis to enable hydrogen release under mild conditions with reduced energy requirements. This strategy targets the oxidative dehydrogenation of fully saturated N-heterocycles, including compounds like 2,5-dimethylpiperazine, N-alkyl dodecahydrocarbazole, N-alkyl octahydroindole along with their analogues. These molecules possess moderate dehydrogenation enthalpies (ranging from 30 to 55 kJ/mol of H₂), making them favorable candidates for low-energy hydrogen release. The research emphasizes the development of catalytic systems—either photoactive or electroactive—that enable sequential hydrogen extraction without the need for external hydrogen acceptors, thereby enhancing atom efficiency and promoting sustainability. This project encompasses the following key objectives: • Designing high-performance, reusable photo- and electro-catalysts utilizing earth-abundant transition metals or organic semiconductor materials. • Gaining mechanistic insights by identifying intermediates via spectroscopy and electrochemistry. • Exploring the relationship between the molecular structure of N-heterocyclic LOHCs and their hydrogen release properties to enhance both kinetics and thermodynamics. • Evaluating the feasibility and repeatability of hydrogen release and uptake cycles in practical, integrated systems. The overarching goal is to establish a foundation for advanced LOHC technologies powered by renewable electricity and solar energy. By avoiding the use of high temperatures, precious metal catalysts, or sacrificial oxidants, this approach supports the global transition to clean hydrogen production, circular carbon systems, and sustainable energy solutions.