Ion conductors comprising noncentrosymmetric frameworks have emerged as new functional materials. However, strongly correlated polarity functionality and ion transport have not been achieved. Herein, we report a ferroelectric proton conductor, KMnN(CN)·HO (), exhibiting the strong correlation between its polar skeleton and conductive ions that generate anomalous ferroelectricity via the proton-bias phenomenon. The application of an electric field of ±1 kV/cm (0.1 Hz) on at 298 K produced the ferroelectricity (polarization = 1.5 × 10 μC/cm), which was enhanced by the ferroelectric-skeleton-trapped conductive protons. Furthermore, the strong polarity-proton transport coupling of induced a proton-rectification-like directional ion-conductive behavior that could be adjusted by the magnitude and direction of DC electric fields. Moreover, exhibited reversible polarity switching between the polar and its dehydrated form, , with a centrosymmetric structure comprising an order-disorder-type transition of the nitrido-bridged chains.
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