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Silica alumina supported Mo@Pt overlayer catalysts were prepared via the directed deposition technique and evaluated for hydrodeoxygenation (HDO) of guaiacol and anisole. As predicted computationally, Mo@Pt overlayers showed reduced heats of hydrogen and carbon monoxide adsorption via chemisorption. The decreased activity of Mo@Pt overlayer catalysts for the ethylene hydrogenation descriptor reaction also suggested decreased hydrogen adsorption strength compared to a Pt only catalyst. H2-TPR results demonstrated the close interaction between Pt and Mo species for Mo@Pt overlayer catalysts and the enhanced reducibility of the molybdenum oxides via deposition of Pt to Mo. Mo@Pt overlayer catalysts showed significantly improved guaiacol and …