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Interrogative Kinetics A New Methodology for Catalyst Characterization. Theory Sergiy O. Shekhtman, Gregory S. Yablonsky, John T. Gleaves. Dpt. of Chemical.

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Presentation on theme: "Interrogative Kinetics A New Methodology for Catalyst Characterization. Theory Sergiy O. Shekhtman, Gregory S. Yablonsky, John T. Gleaves. Dpt. of Chemical."— Presentation transcript:

1 Interrogative Kinetics A New Methodology for Catalyst Characterization. Theory Sergiy O. Shekhtman, Gregory S. Yablonsky, John T. Gleaves. Dpt. of Chemical Engineering, Washington University, Campus Box 1198, One Brookings Drive, St. Louis, MO 63130, USA, fax: (314) 935-7211, e-mail: sos@wuche.che.wustl.edu CREL 2001

2 The Theory of the Interrogative Kinetics Approach State-Defining Experiment To explicitly separate diffusional transport and reaction. To identify the primary kinetic characteristics that can be independently measured in a TAP experiment. To relate the primary kinetic characteristics to detailed reaction mechanisms and distinguish them. State-Altering Experiment To create and kinetically characterize different uniform catalyst states using TAP multi-pulse experiments. To extract the catalyst state characteristics from data obtained in a multi-pulse experiment (particularly the number of active sites). To make assumptions about the reaction mechanism

3 Interrogative Kinetics A New Methodology for Catalyst Characterization. Application to Furane Oxidation over VPO Catalyst Sergiy O. Shekhtman, Gregory S. Yablonsky, John T. Gleaves, Rebecca Fushimi Dpt. of Chemical Engineering, Washington University, Campus Box 1198, One Brookings Drive, St. Louis, MO 63130, USA, fax: (314) 935-7211, e-mail: sos@wuche.che.wustl.edu CREL 2001

4 Multi-Pulse TAP Experiment Furane Oxidation over VPO Catalyst Furane Conversion. Furane/Argon mixture (9/1) was pulsed over oxidized VPO catalyst at 400˚C

5 Multi-Pulse TAP Experiment Furane Oxidation over VPO Catalyst Furane Basic Kinetic Coefficients over Oxidized and “Relaxed” Catalyst Furane/Argon mixture (9/1) was pulsed over oxidized VPO catalyst at 400˚C. After catalyst had been completely reduced, it was left under vacuum conditions for 14 hrs. The, furane was pulsed again.

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