Novel Roles of Catalysts in Producing High‐purity High‐pressure Hydrogen from Sodium Borohydride

Abstract Hydrogen has received enormous attention as a clean fuel with its high specific energy (HHV=142 MJ kg −1 ). To apply hydrogen as a practically available energy vector, the direct production of high‐pressure hydrogen with high purity is pivotal as it allows for circumventing the mechanical compression process. Recently, the concept of utilizing sodium borohydride (SBH) dehydrogenation as a chemical compressor that can generate high‐pressure hydrogen gas was demonstrated by adopting formic acid as an acid catalyst. However, the presence of impurities (e.g., CO, CO 2 ) in the final gas product requires an alternative method to enhance the use of SBH as a chemical compressor. Here, we highlighted the feasibility of producing high‐purity, high‐pressure hydrogen gas from the SBH dehydrogenation with and without Co‐based catalysts. The scrutiny behind the thermodynamics and kinetics of the SBH dehydrogenation was conducted under the elevated pressure condition. As a result, the dual roles of the catalysts as proton collectors and heat sources were revealed, both of which are essential for improving hydrogen production efficiency. We hope that our research stimulates subsequent research that pave the way to exploit hydrogen as an energy vector and achieve a more sustainable future society.