PdAg Nanoparticles within Core-Shell Structured Zeolitic Imidazolate Framework as a Dual Catalyst for Formic Acid-based Hydrogen Storage/Production

Formic acid (FA; HCOOH) is one of the most promising candidates for the storage of hydrogen (H(2)). Herein, we report a H(2) storage/production system based on the hydrogenation of CO(2) and dehydrogenation of FA, using a nanostructured heterogeneous catalyst. Pd(1)Ag(2) nanoparticles with an average size of 2.8 nm were encapsulated within a zeolitic imidazolate framework (ZIF-8) having a core-shell structure (ZIF-8@Pd(1)Ag(2)@ZIF-8). This composite displayed high activity and stability during both the hydrogenation of CO(2) to produce FA and the dehydrogenation of FA into H(2) and CO(2). This improved performance is attributed to the use of ultrafine Pd(1)Ag(2) nanoparticles as well as the spatial regulation of the nanoparticles within the reaction field. This study suggests a new strategy for controlling the spatial distribution of metal nanoparticles within MOFs so as to fine-tune the catalytic activity and selectivity of ZIF-8@metal nanoparticles@ZIF-8 catalysts.