Revisiting Prussian Blue Analogues with Solid‐State MAS NMR Spectroscopy: Spin Density and Local Structure in [Cd3{Fe(CN)6}2]⋅15 H2O

No legendary Prussian order! The distribution of vacancies in Prussian blue analogues is not random, and the spin density on the Cd(2+) ion varies depending on the number of paramagnetic ions in its surroundings. This conclusion follows from (113)Cd solid-state magic-angle spinning NMR studies of [Cd(3){Fe/Co(CN)(6)}(2)] x 15 H(2)O, where the presence of small but significant spin density on the observed (113)Cd nucleus leads to improved spectral resolution.