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This research is supported by the AMPM CCF fund (FCC/1/1972-43-01) to Y.H. from King Abdullah University of Science and Technology and the research grant to F.L. from the National Natural Science Foundation of China (No. 61971201).

Ultrathin ceria nanosheets with exposed reactive {110} facets are synthesized to evaluate the influence of its unique nanostructure on the low-temperature redox behavior. Via a systematic comparison of the ceria nanosheets with nanorods and nanoparticles, we demonstrate that the nanosheets show the enhanced redox reaction activity and the reduced reduction temperature. Through in situ XAFS experiments, we disclose that the ultrathin nanosheets intrinsically decrease the coordination number of Ce atoms and increase the disorder of ceria face-centered cubic fluorite structure, ultimately enhance the oxygen reactivity as well as mobility. Remarkably, the nanosheets exhibit the temperature-independent reducibility between 150 and 250 °C. Through in situ DRIFTS experiments, we demonstrate that the unidentate carbonates are probably the most active surface carbonates species on the redox reaction. The bidentate carbonates are speculated to be the main carbonate species as CO molecules adsorb and diffuse on the ...