Mg(NH2)2–2LiH is an attractive system because of its high reversible hydrogen capacity (∼5.6 wt%) and suitable thermodynamic parameters that allow operation below 100 °C. However, a relatively high kinetic barrier in the hydrogen desorption blocks its application at low temperature. In this work, a small amount of additive, triphenyl phosphate (TPP), was introduced and its effects on hydrogen desorption/absorption in the Mg(NH2)2–2LiH system were studied. Experimental results showed that TPP can prevent aggregation/crystallization during the cycling tests and thus achieve an enhanced kinetic performance. Complete dehydrogenation and hydrogenation can be successfully carried out at temperatures below 150 °C. Moreover, a significant reduction of the entropy change of hydrogen desorption (ΔSdes) was found in the TPP-doped system compared with the pristine Mg(NH2)2–2LiH system, thought to be due to the persistence of amorphous Mg(NH2)2 in the TPP-doped sample during dehydrogenation and hydrogenation cycling, thereby greatly affecting the equilibrium hydrogen pressure.
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