Electrochemical development of magnetic long-range correlations with Tc=128 K in a tetraoxolene-bridged Fe-based framework

The generation of the paramagnetic radical (Cl(2)An(center dot 3-)) in the framework-edge moieties of an Fe-based two-dimensional honeycomb framework with 2,5-dichloro-3,6-dihydroxy-1,4-benzoquinonate (Cl(2)An(n-)), (H3O)(2)(phz)(3)[Fe-2(Cl(2)An)(3)] (phz=phenazine), allowed the formation of long-range magnetic correlations over the network with a relative high magnetic phase transition temperature (T-c) of 128 K. The original compound is a paramagnet with a diamagnetic Cl(2)An(2-) linker that significantly separates paramagnetic Fe-II ions (S=2), where the [(H3O)(2)(phz)(3)](2+) cation is located between layered frameworks. Post-synthetic electron-doping, i.e., reduction in the solid state, using a lithium-ion battery (LIB) system, finally produced (Li+)(3)(H3O+)(2)(phz)(3)[(Fe2+)(2)(Cl(2)An(center dot 3-))(3)], which demonstrated a drastic magnetic change.