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Li–N–H materials, particularly lithium amide and lithium imide, have been explored for use in a variety of energy storage applications in recent years. Compositional variation within the parent lithium imide, anti-fluorite crystal structure has been related to both its facile storage of hydrogen and impressive catalytic performance for the decomposition of ammonia. Here, we explore the controlled solid-state synthesis of Li–N–H solid-solution anti-fluorite structures ranging from amide-dominated (Li 4/3 (NH 2 ) 2/3 (NH) 1/3  or Li 1.333 NH 1.667 ) through lithium imide to majority incorporation of lithium nitride–hydride (Li 3.167 (NH) 0.416 N 0.584 H 0.584  or Li 3.167 NH). Formation of these solid solutions is demonstrated to cause significant changes to the thermal stability and ammonia reactivity of the samples, highlighting the potential use of compositional variation to control the properties of the material in gas storage and catalytic applications.

Compositional flexibility in Li–N–H materials: implications for ammonia catalysis and hydrogen storage