Computation-Based Development of Carrier Materials and Catalysts for Liquid Organic Hydrogen Carrier Systems

Liquid Organic Hydrogen Carriers (LOHCs) have emerged as a promising solution for hydrogen storage, offering high hydrogen storage capacity, reversibility, thermal stability, and compatibility with existing infrastructures. Despite their potential, LOHC systems face significant challenges, including the need for specialized carriers and catalysts for efficient hydrogen storage and release. This review emphasizes the importance of computational analysis in overcoming these challenges. We summarize the computational accuracy of estimating dehydrogenation enthalpy for the carrier materials and explore molecular tuning strategies to enhance the dehydrogenation properties. In addition, we review computational studies that have investigated the impacts of catalytic adsorption/desorption and kinetic properties on the catalytic performance as well as catalyst design methods in terms of the geometry of active metal species, second metals, promoters, heterolytic hydrogen generation, and hydrogen spillover. This review further addresses the current challenges in LOHC systems, and then suggests future computational research directions to improve their efficiency and viability.