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. Advanced Materials, 2015 Schematic showing the formation of coordinatively unsaturated ZnAl-LDH nanosheets. |