Ultrafast hydrogenation of magnesium enabled by tetragonal ZrO<inf>2</inf> hierarchical nanoparticles

Elsevier BV
Publication Type:
Journal Article
Materials Today Nano, 2022, 18, pp. 100200
Issue Date:
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Transition metal catalysts are particularly effective in improving the reaction kinetics of light metal hydrides for reversible hydrogen storage. Herein, tetragonal ZrO2 hierarchical nanoparticles (nano-ZrO2) composed of primary particles of ∼4 nm in diameter are successfully synthesized by a facile one-pot solvothermal process. The unique hierarchical structure features homogeneous distributions of in situ formed multivalent Zr-based species, which allow superior catalytic activity for hydrogen storage in MgH2. The MgH2+10 wt% nano-ZrO2 starts releasing H2 at 163 °C after one activation, which is 107 °C lower than additive-free MgH2, and 50 °C lower than that of bulk ZrO2-doped MgH2. At 230 °C, 5.9 wt% of H is rapidly liberated within 20 min from the nano-ZrO2-containing MgH2. More importantly, the material shows superior hydrogenation kinetics compared with all reported catalyst-modified MgH2. The nano-ZrO2-containing Mg took up 4.0 wt% of H in only 12 s at 100 °C under 50 bar H2, 400 times faster than the bulk-ZrO2-modified sample. Even at 50 °C, approximately 1.8 wt% H was absorbed within 1 min. Our findings provide useful insights into the design and development of high-performance catalysts toward solid-state hydrogen storage materials.
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