Abstract
Kinetic analysis is a powerful and effective strategy to reveal the physical-chemical nature of the promotion effect of heteroatoms to nanocarbon catalysts. The present work reported the mechanistic and kinetic analysis of ethylbenzene oxidative dehydrogenation (ODH) reactions on heteroatom (N or B) doped and undoped carbon nanotube (CNT) catalysts via active site titration, kinetic isotope effect and single reactant surface reaction experiments etc. The physical-chemical meanings behind the elementary step rate and equilibrium constants were revealed and applied for interpretations of the promotion effect of heteroatoms at molecular level. Nitrogen doped CNT exhibited both higher rate and equilibrium constants for C–H bond dissociation and O2 adsorption than undoped one via facilitating the electron transfer process. The evolution of the active sites could be quantitatively described with rate equation via the theory of most abundant surface intermediates, which provides in depth understandings on the mechanism and structure-function relations in carbon catalyzed redox reactions.
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