Hydrogen storage has long been a priority on the renewable energy research agenda. Due to its high volumetric and gravimetric hydrogen density, MgH2 is a desirable candidate for solid-state hydrogen storage. However, its practical use is constrained by high thermal stability and sluggish kinetics. Here, PdNi bilayer metallenes are reported as catalysts for hydrogen storage of bulk-MgH2 near ambient temperature. Unprecedented 422 K beginning dehydrogenation temperature and up to 6.36 wt.% reliable hydrogen storage capacity are achieved. Fast hydrogen desorption is also provided by the system (5.49 wt.% in 1 h, 523 K). The in situ generated PdNi alloy clusters with suitable d-band centers are identified as the main active sites during the de/re-hydrogenation process by aberration-corrected transmission electron microscopy and theoretical simulations, while other active species including Pd/Ni pure phase clusters and Pd/Ni single atoms obtained via metallene ball milling, also enhance the reaction. These findings present fundamental insights into active species identification and rational design of highly efficient hydrogen storage materials.
Keywords: bilayer metallene; clusters; d-band center; hydrogen storage materials; magnesium hydride; single atoms.
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