Abstract
Mixed solid solutions have played an important role in improving the kinetics and performance of hydrogen storage materials, as reported for the Li-Mg-N-H, K-Mg-N-H, and Rb-Mg-N-H systems. Besides, the formation of a homogeneous solid solution, mostly due to partial ionic substitution, is known to be an effective approach to improve the ionic conductivity of a material, which is an important property in electrochemical applications. We have reported a series of solid solutions based on mixed amide-hydride materials of the Group 1 elements, e.g., K(NH2)xH1-x, Rb(NH2)xH1-x, and Cs(NH2)xH1-x, via the exchange of NH2-/H- anions with the change of the lattice cell of the solid solution. Extending the research in this direction, we study the M-N-H solid solution in the MNH2-MH systems (M = K, Rb, Cs, and their combinations), i.e., KNH2-RbH, RbNH2-KH, RbNH2-CsH, and CsNH2-RbH via ex situ/in situ XRD, IR, and 1H 2D solid-state NMR. The results obtained confirm the formation of mixed metal amide-hydride solid solutions associated with an exchange between both anionic (NH2- and H-) and cationic species (K+, Rb+, and Cs+). With this study, we aim to create an accessible library of M-N-H solid solutions for further studies as additives for hydrogen storage materials or ionic conductors.