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dc.titleChemical and kinetic study of acetophenone hydrogenation over Pt/Al2O3: Application of BTEM and other multivariate techniques to quantitative on-line FTIR measurements
dc.contributor.authorGao, F.
dc.contributor.authorAllian, A.D.
dc.contributor.authorZhang, H.
dc.contributor.authorCheng, S.
dc.contributor.authorGarland, M.
dc.identifier.citationGao, F., Allian, A.D., Zhang, H., Cheng, S., Garland, M. (2006-07-01). Chemical and kinetic study of acetophenone hydrogenation over Pt/Al2O3: Application of BTEM and other multivariate techniques to quantitative on-line FTIR measurements. Journal of Catalysis 241 (1) : 189-199. ScholarBank@NUS Repository.
dc.description.abstractThe heterogeneous catalytic hydrogenation of acetophenone (Aceph) over Pt/Al2O3 in d8-toluene/h8-toluene at 273 K was performed in semibatch mode, using a recycle configuration and on-line quantitative Fourier transform infrared (FTIR) spectroscopy measurements. Based on the d8-toluene solvent used and the multivariate analysis applied, further details of the reaction chemistry were elucidated, including the following: (i) Solvent activation occurred during reaction, leading to observable hydrogenation and H-D exchange, and (ii) 1-phenylethanol (Phel), cyclohexyl methyl ketone (CMK), and cyclohexylethanol (Che) were observable products, and little H-D exchange occurred. The on-line FTIR measurements, with sensitivity on the order of 10-5   mol / L, also lead to the following kinetic observations: (i) Water had a strong inhibiting effect on the hydrogenation rates, and (ii) very interesting short time-scale kinetic behavior occurred after some perturbations. The latter included rapid initial hydrogenations on fresh catalyst (due to the presence of spillover hydrogen) and observable adsorption-desorption of other reactants. The reaction rates obtained from the well-defined experiments in h8-toluene were fit to a number of Langmuir-Hinshelwood-Hougen-Watson (LHHW) models, in which the effects of solvent and water were included. A model involving a pairwise addition of adsorbed dissociated hydrogen to the adsorbed substrate provided the best fit of the data. The regression of the kinetic data suggested that water made a statistically significant contribution to the competitive adsorption on the catalyst surface. In more general terms, the present contribution suggests the utility of detailed on-line liquid-phase spectroscopy together with multivariate techniques for exploratory studies of heterogeneous catalytic systems. © 2006 Elsevier Inc. All rights reserved.
dc.subjectHeterogeneous catalysis
dc.subjectLHHW model
dc.subjectMultiple perturbations
dc.subjectOn-line FTIR spectroscopy
dc.subjectRecycle reactor
dc.description.sourcetitleJournal of Catalysis
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