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Defect‐rich ultrathin ZnAl‐layered double hydroxide nanosheets are successfully prepared. Under UV–vis irradiation, these nanosheets are superior efficient catalysts for the photoreduction of CO2 to CO with water. The formed oxygen vacancies lead to the formation of coordinatively unsaturated Zn+ centers within the nanosheets, responsible for the very high photocatalytic activities.
Catalysts with coordinatively unsaturated Znd+ (d < 2) centers have recently attracted attention for the photocatalytic dehydrogenation of methane. On page 7824, T. Zhang and co‐workers report that Zn+–Vo complexes are introduced by synthesizing ultrathin ZnAl‐layer double hydroxide nanosheets, which exhibit extraordinarily high activity for the photoreduction of CO2 to CO with water.
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