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Facet-Dependent Photocatalytic Behaviors of ZnS-Decorated Cu <sub/>2</sub> O Polyhedra Arising from Tunable Interfacial Band Alignment
摘要： ZnS particles were grown over Cu2O cubes, octahedra, and rhombic dodecahedra for examination of their facet-dependent photocatalytic behaviors. After ZnS growth, Cu2O cubes stay photocatalytically inactive. ZnS-decorated Cu2O octahedra show enhanced photocatalytic activity resulting from better charge carrier separation upon photoexcitation. Surprisingly, Cu2O rhombic dodecahedra give greatly suppressed photocatalytic activity after ZnS deposition. Electron paramagnetic resonance (EPR) spectra agree with these experimental observations. Time-resolved photoluminescence (TRPL) profiles provide charge transfer insights. The decrease in the photocatalytic activity is attributed to an unfavorable band alignment caused by significant band bending within the Cu2O (110)/ZnS (200) plane interface. A modified Cu2O–ZnS band diagram is presented. Density functional theory (DFT) calculations generating plane-specific band energy diagrams of Cu2O and ZnS match well with the experimental results, showing charge transfer across the Cu2O (110)/ZnS (200) plane interface would not happen. This example further illustrates that the actual photocatalysis outcome for semiconductor heterojunctions cannot be assumed because interfacial charge transfer is strongly facet-dependent.
关键词： interfacial charge transfer,zinc sulfide,cuprous oxide,facet-dependent properties,heterojunctions,band alignment
更新于2025-09-23 15:23:52
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Facet-Dependent Optical Properties of Semiconductor Nanocrystals
摘要： Recent observations of facet-dependent electrical conductivity and photocatalytic activity of various semiconductor crystals are presented. Then, the discovery of facet-dependent surface plasmon resonance absorption of metal–Cu2O core–shell nanocrystals with tunable sizes and shapes is discussed. The Cu2O shells also exhibit a facet-specific optical absorption feature. The facet-dependent electrical conductivity, photocatalytic activity, and optical properties are related phenomena, resulting from the presence of an ultrathin surface layer with different band structures and thus varying degrees of band bending for the {100}, {110}, and {111} faces of Cu2O to absorb light of somewhat different wavelengths. Recently, it is shown that the light absorption and photoluminescence properties of pure Cu2O cubes, octahedra, and rhombic dodecahedra also display size and facet effects because of their tunable band gaps. A modified band diagram of Cu2O can be constructed to incorporate these optical effects. Literature also provides examples of facet-dependent optical behaviors of semiconductor nanostructures, indicating that optical properties of nanoscale semiconductor materials are intrinsically facet-dependent. Some applications of semiconductor optical size and facet effects are considered.
关键词： surface band bending,semiconductors,facet-dependent properties,cuprous oxide,nanocrystals
更新于2025-09-19 17:15:36