Highly stable superprotonic conductivity (>10 S cm) has been achieved through the unprecedented coordinative urea insertion in MOF-74 [M(dobdc), M = Ni, Mg; dobdc = 2,5-dioxido-1,4-benzenedicarboxylate] without an acidic moiety. The urea is bound to open metal sites and alters the void volume and surface functionality, which triggers a significant change in proton conductivity and diffusion mechanism. Solid-state H NMR revealed that the high conductivity was attributed to the strengthening of the hydrogen bonds between guest HO induced by hydrogen bonds in the interface between HO and the polarized coordinated urea.
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