In this paper, we report a KOH-doped Mg(NH2)2–2LiH system with low operating temperatures and good cycling stability. The Mg(NH2)2–2LiH–0.07KOH sample can reversibly desorb/absorb ∼4.92 wt% hydrogen with a starting and peak dehydrogenation temperature of ∼75 °C and ∼120 °C, respectively, the lowest in the current Mg(NH2)2–2LiH system studied. Moreover, the cycling stability of de-/hydrogenation is also remarkably improved by KOH doping as the average capacity degradation of the Mg(NH2)2–2LiH–0.07KOH system is of only 0.002 wt% per cycle within 30 cycles. Detailed structural investigations reveal that during ball milling, the doped KOH can react with Mg(NH2)2 and LiH to convert to MgO, KH and Li2K(NH2)3, which work together to provide the synergistic effects of thermodynamics and kinetics on hydrogen desorption and absorption of the Mg(NH2)2–2LiH system upon heating, consequently inducing a significant improvement in hydrogen storage properties.
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