Synthesis and decomposition of Li3Na(NH2)4 and investigations of Li-Na-N-H based systems for hydrogen storage

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  • Lars H Jepsen
  • ,
  • Peikun Wang, Chinese Academy of Sciences, China
  • Guotao Wu, Chinese Academy of Sciences, China
  • Zhitao Xiong, Chinese Academy of Sciences, China
  • Flemming Besenbacher
  • Ping Chen, Chinese Academy of Sciences, China
  • Torben R Jensen

Previous studies have shown modified thermodynamics of amide-hydride composites by cation substitution, while this work systematically investigates lithium-sodium-amide, Li-Na-N-H, based systems. Li3Na(NH2)4 has been synthesized by combined ball milling and annealing of 3LiNH2-NaNH2 with LiNa2(NH2)3 as a minor by-product. Li3+xNa1-x(NH2)4 releases NaNH2 and forms non-stoichiometric Li3+xNa1-x(NH2)4 before it melts at 234 °C, as observed by in situ powder X-ray diffraction. Above 234 °C, Li3+xNa1-x(NH2)4 releases a mixture of NH3, N2 and H2 while a bi-metallic lithium sodium imide is not observed during decomposition. Hydrogen storage performances have been investigated for the composites Li3Na(NH2)4-4LiH, LiNH2-NaH and NaNH2-LiH. Li3Na(NH2)4-4LiH converts into 4LiNH2-NaH-3LiH during mechanochemical treatment and releases 4.2 wt% of H2 in multiple steps between 25 and 340 °C as revealed by Sievert's measurements. All three investigated composites have a lower peak temperature for H2 release as compared to LiNH2-LiH, possibly owing to modified kinetics and thermodynamics, due to the formation of Li3Na(NH2)4 and LiNa2(NH2)3.

Original languageEnglish
JournalPhysical Chemistry Chemical Physics
Pages (from-to)1735-1742
Number of pages8
Publication statusPublished - 2016

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