Abstract
Understanding surface reconstruction of nanocrystals is of great importance to their applications, however it is still challenging due to lack of atomic-level structural information under reconstruction conditions. Herein, through in situ spherical aberration corrected scanning transmission electron microscopy (STEM), the reconstruction of nanocrystalline SnO2 (110) surface was studied. By identifying the precise arrangements of surface/subsurface Sn and O columns through both in situ bright-field and high-angle annular dark-field STEM images, an unexpected added Sn2O model was determined for SnO2 (110)-(1 x 2) surface. The protruded Sn delta+ of this surface could act as the active sites for activating O-2 molecules according to our density functional theory (DFT) calculations. On the basis of in situ observation of atomic-level reconstruction behaviors and DFT calculations, an energy-driven reconstruction process was also revealed. We anticipate this work would help to clarify the long-standing debate regarding the reconstruction of SnO2 (110) surface and its intrinsic property.