The OH groups on the Zr-based nodes of ultrastable UiO-66 can be metallated with V ions in a facile fashion to give the derivative VUiO-66. This metallated MOF exhibits high stability over a broad temperature range and displays high selectivity for benzene under low-conversion conditions in the vapor-phase oxidative dehydrogenation of cyclohexene (activation energy ∼110 kJ/mol). The integrity o...