Improved hydrogen storage properties and mechanisms of LiAlH4 doped with Ni/C nanoparticles anchored on large-size Ti3C2Tx

Abstract

Lithium aluminum hydride (LiAlH4) with a high hydrogen capacity of 10.5 wt% has become one of the most promising solid-state hydrogen storage materials for onboard hydrogen fuel cell systems. However, neither dehydrogenation kinetics nor cycling behaviors of LiAlH4 can fulfill the requirements of practical application. Here, we prepared the Ni/C nanoparticles anchored on large-size Ti3C2Tx nanosheets, firstly introduced into LiAlH4 to investigate its catalytic effect. Dehydrogenation experiments demonstrate that LiAlH4 doped with 7 wt% Ni/C@Ti3C2 starts to release hydrogen at 56.9 °C. Also, it can release about 4.3 wt% hydrogen within 50 min at 120 °C. The activation energies of LiAlH4 doped with 7 wt% Ni/C@Ti3C2 for the first and second steps are 34.5% and 53.2% lower than the as-received LiAlH4, respectively. Under 300 °C and 40 bar hydrogen, it can absorb 0.58 wt% hydrogen. It is found that in situ formed intermetallic Al2Ti during ball milling can weaken the Al-H bonds in LiAlH4 through interfacial charge transfer and the dehybridization, benefitting for the breaking of the Al-H bond in LiAlH4. In addition, Al2Ti can promote the adsorption and splitting of H2, contributing to the rehydrogenation of LiAlH4.