MOF-derived Cu based materials as highly active catalysts for improving hydrogen storage performance of Mg-Ni-La-Y alloys

Higher initial (de)hydrogenation temperature and sluggish kinetics are the main bottlenecks to develop Mg-based hydrogen storage alloys with high hydrogen capacity. One of the effective methods of solving these problems is introducing additives to enhance (de)hydrogenation kinetics and decrease particle sizes to lower (de)hydrogenation temperatures. In this work, Mg85-Ni10-La4.5-Y0.5 alloy doped with Cu@C nanoparticles is prepared, which could enhance (de)hydrogenation kinetics via introducing Cu nanoparticles as a catalyst and reduce the alloy particle sizes via acting as a grinding agent to lower (de)hydrogenation temperature. The results indicate the dehydrogenation temperature of the modified Mg85-Ni10-La4.5-Y0.5 composite could be decreased to 308.5 °C, absorb 4.73 wt% H2 at 220 °C within 1 min and release 5.01 wt% H2 within 4 min at 300 °C. Moreover, the capacity retention could be maintained around 98.8% after 10 cycles at 300 °C, superior than those of Mg85-Ni10-La4.5-Y0.5 and milled-Mg85-Ni10-La4.5-Y0.5. DFT results and characterizations suggest that in-situ formed Mg2Cu could accelerate the dissociation of Mg-H bonds and the presence of amorphous carbon in Mg-Ni-La-Y-Cu system will further synergistically improve the (de)hydrogenation kinetics of Mg85-Ni10-La4.5-Y0.5. Reduced particle sizes under the aid of carbon frameworks also help introduce boundaries of the particles and shorten hydrogen diffusion pathways. MgH2 reacted with copper to generate nano MgCu2 and Mg2Cu in situ, accelerating the dissociation of hydrogen molecules and promoted the hydrogenation of the Mg phase. [Display omitted]