화학공학소재연구정보센터
Applied Catalysis A: General, Vol.557, 145-153, 2018
Combined catalytic action of supported Cu and Au in imine production from coupled benzyl alcohol and nitrobenzene reactions
The feasibility of continuous gas phase coupling of benzyl alcohol dehydrogenation with nitrobenzene hydrogenation for imine (N-benzylideneaniline) synthesis over mixtures of Cu/SiO2 and (TiO2, MgO) supported Au catalysts has been established. The catalysts were characterised in terms of specific surface area, pore volume, TPR, H-2 chemisorption, STEM, XPS and TGA-DSC analysis. Au/TiO2 prepared by deposition-precipitation exhibited a narrower particle size distribution (1-6 nm) and smaller mean (3.2 nm) than Au/MgO (1-15 nm, mean = 7.7 nm) prepared by impregnation. Dehydrogenation of benzyl alcohol (to benzaldehyde) over Cu/SiO2 delivered a (ten-fold) higher rate than supported Au and Au/TiO2 exhibited a higher H-2 chemisorption capacity and greater (by a factor of ten) nitrobenzene hydrogenation rate than Cu/SiO2 and Au/MgO. Inefficient hydrogen utilisation is demonstrated for the cross-coupling reaction over Cu/SiO2 alone and a temporal activity loss is linked to carbonaceous (benzoate) deposition (on the basis of XPS and TGA-DSC analysis). Incorporation of Au/TiO2 (and Au/MgO) with Cu/SiO2 increased the imine formation rate and H-2 utilisation efficiency. The combination of Au/TiO2 with Cu/SiO2 served to circumvent Cu/SiO2 deactivation, resulting in enhanced stability with a four-fold increase in imine production and full H-2 utilisation at Cu/Au = 10.