We demonstrate that non-stoichiometric lithium imide is a highly active catalyst for the production of high-purity hydrogen from ammonia, with superior ammonia decomposition activity to a number of other catalyst materials. Neutron powder diffraction measurements reveal that the catalyst deviates from pure imide stoichiometry under ammonia flow, with active catalytic behaviour observed across a range of stoichiometry values near the imide. These measurements also show that hydrogen from the ammonia is exchanged with, and incorporated into, the bulk catalyst material, in a significant departure from existing ammonia decomposition catalysts. The efficacy of the lithium imide–amide system not only represents a more promising catalyst system, but also broadens the range of candidates for amide-based ammonia decomposition to include those that form imides.
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