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• W3083515118 endingPage "121725" @default.
• W3083515118 startingPage "121725" @default.
• W3083515118 abstract "• Dipole coupling is critical for understanding IR spectra of adsorbed CO on Cu. • Surface protrusions dominate the IR contribution from the Cu surface. • The C-O frequency in CO on supported Cu is determined by the underlying support. • Support dependent charging of the Cu surface can explain the C-O frequency shifts. • Cu surface charging regulates the adsorbate population that the surface can sustain. Infrared spectroscopy on CO chemisorbed on Raney Cu and materials with Cu dispersed as nanoparticles on oxide supports was used to evaluate support effects on the Cu surface properties. The C-O frequency (ν C-O ) is sensitive to the charge on the adsorption site with ν C-O being high on Cu + , intermediate on Cu 0 , and low on Cu − , whereby this method can probe the charging state of the Cu surface. The Raney Cu reference demonstrates the complex analysis of the IR band intensity, which can be susceptible to dipole coupling. This means that the most intense IR bands may be higher frequency bands strengthened by such coupling effects rather than the bands arising from the most abundant sites. The ν C-O of the major band attributable to CO adsorbed on the metallic surface follows the order: Cu/SiO 2 > Raney Cu > Cu/Al 2 O 3 > Cu/TiO 2 . Given the charge-frequency relationship these support-dependent frequency shifts are attributed to changes in the charging of the Cu surface caused by support effects. The Cu surface is more electron deficient for Cu/SiO 2 and electron enriched for Cu/TiO 2 . For the Cu/ZnO(/Al 2 O 3 ) samples, which are important as industrial methanol synthesis catalysts, band assignments are complicated by a low ν C-O on Cu + sites connected to the ZnO matrix. However, Cu/ZnO(/Al 2 O 3 ) has a spectral feature at 2065-68 cm −1 , which is a lower frequency than observed in the Cu single crystal studies in the literature and thus indicative of a negative charging of the Cu surface in such systems. Experiments with co-adsorption of CO and electron-withdrawing formate on Cu/ZnO and Cu/SiO 2 show that ν C-O in the adsorbed CO shifts upwards with increasing HCOO coverage. This illustrates that the surface charge is donated to the electron-withdrawing formate adsorbate, and as a result co-adsorbed CO experiences a more charge depleted Cu surface that yields higher ν C-O . The support-dependent surface charging may thus affect the interaction with adsorbates on the metal surface and thereby impact the catalytic properties of the Cu surface. Dilution of the samples in KBr, which has been used in many studies in the literature, had pronounced effects on the spectra. The presence of KBr leads to an increase in ν C-O indicative of an electron depleted surface attributed to transfer of electron-withdrawing bromine species from KBr to the sample." @default.
• W3083515118 created "2020-09-11" @default.
• W3083515118 creator A5026735838 @default.
• W3083515118 creator A5027682734 @default.
• W3083515118 creator A5050803413 @default.
• W3083515118 creator A5054120979 @default.
• W3083515118 creator A5078066679 @default.
• W3083515118 date "2021-01-01" @default.
• W3083515118 modified "2023-10-03" @default.
• W3083515118 title "Characterization of oxide-supported Cu by infrared measurements on adsorbed CO" @default.
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