Fourier transform Raman spectra of methyl red adsorbed on untreated and pretreated ${gamma}$-alumina and silicaalumina calcined at 900 $^{circ}C$ under 1 atm steam flowing were recorded. Spectral analysis shows that the active species adsorbed on ${gamma}$-alumina was to be deprotonated methyl red, and on silica-alumina to be di-protonated. This indicates that ${gamma}$-alumina adapted in this work holds Bronsted basicity, and silica-alumina Bronsted acidity. Raman intensities of methyl red on pretreated ${gamma}$-alumina are about three times stronger than on untreated ${gamma}$-alumina, while spectral features are unchanged. For silica-alumina, spectral features show modified vibrational characteristics upon surface hydroxylations generated from pretreatment. Consequently, the acidity loss for silica-alumina and the basicity gain for ${gamma}$-alumina were observed by increasing the surface hydroxyl groups on the catalysts through pretreatment of the steam calcination.