摘要
Nanoscaled catalysts have attracted much more attention due to their more abundant active sites and better dispersion than their bulky counterparts.In this work,VH_(x) nanoparticles smaller than 10 nm in average size are successfully synthesized by a simple solid-state ball milling coupled with THF washing process,which are proved to be highly effective in enhancing the hydrogen absorption/desorption kinetics of MgH_(2) at moderate temperatures.The nano-VH_(x)-modified MgH_(2) releases hydrogen from 182℃,which is 88℃ lower than additive-free MgH_(2).The release of hydrogen amounts to 6.3 wt%H within 10 min at 230℃ and 5.6 wt%H after 30 min at 215℃ with initial vacuum.More importantly,the dehydro-genated MgH_(2)+10 wt.%nano-VH_(x) rapidly absorbs 5.2 wt%H within 3 min at 50℃ under 50 bar H_(2).It even takes up 4.3 wt%H within 30 min at room temperature(25℃)under 10 bar H_(2),exhibiting supe-rior hydrogenation kinetics to most of the previous reports.Mechanistic analyzes disclose the reversible transformation between V and V-H species during the hydrogen desorption-absorption process.The ho-mogeneously distributed V-based species is believed to act as hydrogen pump and nucleation sites for MgH_(2) and Mg,respectively,thus triggering fast hydrogenation/dehydrogenation kinetics.
基金
supported by the National Out-standing Youth Foundation of China (No.52125104)
the Natural Science Foundation of Zhejiang Province (No.LD21E010002)
the National Natural Science Foundation of China (No.52001277)
the Fundamental Research Funds for the Central Universities (No.2021FZZX001-09)
the National Youth Top-Notch Talent Support Program.