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Morphology Effect of ZrO<sub>2</sub> on Tuning the C–H Bond Activation in Propane Dehydrogenation

Yichen Yu, Yi Dai, Ruipu Wang, Yuchen Zhang, Yuchen Zhang, Lixia Bao, Yiheng Wu, Yaoyuan Zhang, Yaoyuan Zhang, Qin Wu, Daxin Shi, Kangcheng Chen, Guiyuan Jiang, Evgenii V. Kondratenko, Hansheng Li

2023ACS Catalysis24 citationsDOI

Abstract

Alternative-type bulk ZrO 2 -based catalysts for propane dehydrogenation have attracted increasing attention. Here, we studied the effects of ZrO 2 morphology on material physicochemical properties, activity, and reaction mechanism of propane dehydrogenation by combining characterization techniques, kinetic tests, and theoretical calculations. A morphology–reactivity dependence is determined and suggests that the rate of propene formation is positively related to the fraction of the (1̅11) facet, which shows the highest intrinsic activity toward propene formation. Moreover, the H-binding energy is identified as an effective descriptor to predict the intrinsic activity in PDH, and a moderate H-binding strength is required for balancing the C–H bond activation and H 2 formation rates to ensure the highest intrinsic activity. The obtained knowledge of tuning the C–H bond activation and intrinsic activity inspires the design of highly active metal oxide based catalysts for propene formation.

Topics & Concepts

DehydrogenationPropenePropaneCatalysisActivation energyChemistryOxideReactivity (psychology)Binding energyKineticsPhotochemistryPhysical chemistryOrganic chemistryMedicineAlternative medicineNuclear physicsPathologyPhysicsQuantum mechanicsCatalysis and Oxidation ReactionsCatalytic Processes in Materials ScienceZeolite Catalysis and Synthesis