Abstract
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 (Li4/3(NH2)2/3(NH)1/3 or Li1.333NH1.667) through lithium imide to majority incorporation of lithium nitride–hydride (Li3.167(NH)0.416N0.584H0.584 or Li3.167NH). 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.
Highlights
Compositional variation, and the ability to exert synthetic control over such variation, lies at the heart of much of functional materials chemistry research, impacting a wide range of materials properties from metal alloy strength to superconductivity
We aim to provide a synthetically-accessible library of Li–N–H materials which can be further investigated for their functional properties as catalysts, catalyst supports and hydrogen stores, as well as synthetic approaches for the synthesis of other functional M–N–H solid solutions
Synchrotron powder X-ray diffraction data provides a basis for assessment of the structural variation across the Li–N–H samples and the successful formation of solid solutions
Summary
Compositional variation, and the ability to exert synthetic control over such variation, lies at the heart of much of functional materials chemistry research, impacting a wide range of materials properties from metal alloy strength to superconductivity. On either side of the stoichiometric imide, there is a wide compositional range where the diffraction data show only Fm3%m peaks, indicating a disordered (solid solution) average structure.
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