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two-dimensional nanomaterials of non-layered metal oxide is a grand challenge because
it requires long range single-crystallinity and clean high-energy surfaces. Here,
we report the synthesis of single-crystalline MgO(111) nanosheets via a
two-step process involving the formation of ultrathin Mg(OH)2
nanosheets as precursor and their selective topotactic conversion upon heating under
dynamic vacuum. The defect-rich surface displays terminal -OH groups, 3-coordinated
O2- sites, low-coordinated Mg2+ sites as well as single
electrons trapped at oxygen vacancies, that render MgO nanosheets highly reactive
as evidenced by the activation of CO molecules at low temperatures and
pressures, with formation of strongly adsorbed red-shifted CO and coupling of CO
molecules into C2 species.