The effect of Li(3)N additive on the Li-Mg-N-H system was examined with respect to the reversible dehydrogenation performance. Screening Study with varying Li(3)N additions (5, 10, 20, and 30 mol%) demonstrates that all are effective for improving the hydrogen desorption capacity. Optimally, incorporation of 10 mol% Li(3)N improves the practical capacity from 3.9 wt% to approximately 4.7 wt% hydrogen at 200 degrees C, which drives the dehydrogenation reaction toward completion. Moreover, the capacity enhancement persists well over 10 de-/rehydrogenation cycles. Systematic x-ray diffraction examinations indicate that Li(3)N additive transforms into LiNH(2) and LiH phases and remains during hydrogen cycling. Combined structure/property investigations suggest that the LiNH(2) "seeding" should be responsible for the capacity enhancement, which reduces the kinetic barrier associated with the nucleation of intermediate LiNH(2). In addition, the concurrent incorporation of LiH is effective for mitigating the ammonia release.
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