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Adv Mater ; 34(30): e2202072, 2022 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-35580350


Surface oxygen vacancies have been widely discussed to be crucial for tailoring the activity of various chemical reactions from CO, NO, to water oxidation by using oxide-supported catalysts. However, the real role and potential function of surface oxygen vacancies in the reaction remains unclear because of their very short lifetime. Here, it is reported that surface oxygen vacancies can be well confined electrostatically for a polarization screening near the perimeter interface between Pt {111} nanocrystals and the negative polar surface (001) of ferroelectric PbTiO3. Strikingly, such a catalyst demonstrates a tunable catalytic CO oxidation kinetics from 200 °C to near room temperature by increasing the O2 gas pressure, accompanied by the conversion curve from a hysteresis-free loop to one with hysteresis. The combination of reaction kinetics, electronic energy loss spectroscopy (EELS) analysis, and density functional theory (DFT) calculations, indicates that the oxygen vacancies stabilized by the negative polar surface are the active sites for O2 adsorption as a rate-determining step, and then dissociated O moves to the surface of the Pt nanocrystals for oxidizing adsorbed CO. The results open a new pathway for tunable catalytic activity of CO oxidation.

Angew Chem Int Ed Engl ; 60(41): 22339-22344, 2021 Oct 04.
Artigo em Inglês | MEDLINE | ID: mdl-34352928


The strong metal-support interaction (SMSI) is widely used in supported metal catalysts and extensive studies have been performed to understand it. Although considerable progress has been achieved, the surface structure of the support, as an important influencing factor, is usually ignored. We report a facet-dependent SMSI of Pd-TiO2 in oxygen by using in situ atmospheric pressure TEM. Pd NPs supported on TiO2 (101) and (100) surfaces showed encapsulation. In contrast, no such cover layer was observed in Pd-TiO2 (001) catalyst under the same conditions. This facet-dependent SMSI, which originates from the variable surface structure of the support, was demonstrated in a probe reaction of methane combustion catalyzed by Pd-TiO2 . Our discovery of the oxidative facet-dependent SMSI gives direct evidence of the important role of the support surface structure in SMSI and provides a new way to tune the interaction between metal NPs and the support as well as catalytic activity.

Nano Lett ; 21(17): 7309-7316, 2021 Sep 08.
Artigo em Inglês | MEDLINE | ID: mdl-34410724


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 × 2) surface. The protruded Snδ+ of this surface could act as the active sites for activating O2 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.