Superior Dehydrogenation Performance of α‐AlH3 Catalyzed by Li3N: Realizing 8.0 wt.% Capacity at 100 °C

The high dehydrogenation temperature of aluminum hydride (AlH3) has always been an obstacle to its application as a portable hydrogen source. To solve this problem, lithium nitride is introduced into the aluminum hydride system as a catalyst to optimize the dehydrogenation drastically, which reduces the initial dehydrogenation temperature from 140.0 to 66.8 °C, and provides a stable hydrogen capacity of 8.24, 6.18, and 5.75 wt.% at 100, 90, and 80 °C within 120 min by adjusting the mass fraction of lithium nitride. Approximately 8.0 wt.% hydrogen can be released within 15 min at 100 °C for the sample of 10 wt.% doping. Moderate dehydrogenation temperature slows down the inevitable self‐dehydrogenation process during the ball‐milling process, and the enhanced kinetics at lower temperature shows the possibility of application in the fuel cell. The addition of lithium nitride (Li3N) causes the occurrence of surface reaction on aluminum hydride (AlH3) particles during ball milling. The newly formed amorphous Li3AlN2 weakens the AlH bond energy and promotes the release of hydrogen. Lithium nitride additive and nanocrystallization via ball milling synergistically decrease the dehydrogenation temperature and enhance the kinetics of aluminum hydride.