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A systematic investigation on the hydrogen storage properties of Li-Mg-N-H materials with various compositions was performed. Li-Mg-N-H hydrogen storage materials were prepared by mechanically milling LiNH2/MgH2 mixtures with initial molar ratios ranging from 1.5:1 to 3: 1, followed by de/rehydriding at 200 degrees C. It was found that the hydrogen storage capacity of the system was highly dependent on the initial phase ratio of the LiNH2/MgH2 mixture. An optimum hydrogen capacity of about 5 wt% was achieved in the 2.15:1 LiNH2/MgH2 mixture. Different carbon materials, such as the single-walled carbon nanotubes (SWNTs), multi-walled carbon nanotubes, graphite and activated carbon, were used as additive to improve the hydrogen storage performance. It was found that the dehydriding kinetics of the Li-Mg-N-H material could be markedly improved by adding a small amount of SWNTs, especially in the as-prepared state. (c) 2006 International Association for Hydrogen Energy. Published by Elsevier Ltd. All rights reserved.