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K-Ion Slides in Prussian Blue Analogues
John Cattermull1,2, Nikolaj Roth1,3, Simon J Cassidy1
1Inorganic Chemistry Laboratory, Department of Chemistry, University of Oxford, South Parks Road, Oxford OX1 3QR, U.K.
Abstract:
We study the phenomenology of cooperative off-centering of K+ ions in potassiated Prussian blue analogues (PBAs). The principal distortion mechanism by which this off-centering occurs is termed a "K-ion slide", and its origin is shown to lie in the interaction between local electrostatic dipoles that couple through a combination of electrostatics and elastic strain. Using synchrotron powder X-ray diffraction measurements, we determine the crystal structures of a range of low-vacancy K2M[Fe(CN)6] PBAs (M = Ni, Co, Fe, Mn, Cd) and establish an empirical link between composition, temperature, and slide-distortion magnitude. Our results reflect the common underlying physics responsible for K-ion slides and their evolution with temperature and composition. Monte Carlo simulations driven by a simple model of dipolar interactions and strain coupling reproduce the general features of the experimental phase behavior. We discuss the implications of our study for optimizing the performance of PBA K-ion battery cathode materials and also its relevance to distortions in other, conceptually related, hybrid perovskites.
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