Alejandra Torres-Velasco , Bhagyesha S. Patil , Hongda Zhu , Yue Qi , Simon G. Podkolzin , Juan J. Bravo-Suárez
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A general method for studying reactive surface species, CT-SKAn: Charge-transfer spectrokinetic analysis
A spectrokinetic methodology was developed to determine reactive surface species by combining operando ultraviolet–visible spectroscopy and charge transfer kinetic models. The methodology consisted of three general steps: 1) concomitant measurement of reaction rates and charge transfer via ultraviolet–visible spectroscopy; 2) development of rate expressions from kinetic models involving the adsorbed species of interest. These rate expressions relate reaction rates, charge transfer, and partial pressures of gas phase species; and 3) evaluation of the goodness of fit of the rate expressions to the experimental data. The species whose rate expressions show the best fit are the more likely reactive surface species for the studied reaction. An example is presented for the determination of reactive oxygen species during ethanol oxidation over Au/TiO2. The charge transfer spectrokinetic analysis showed that surface hydroperoxyl, hydroxyl, and atomic oxygen species were reactive surface intermediates, whereas surface molecular oxygen was not.
期刊介绍:
The Journal of Catalysis publishes scholarly articles on both heterogeneous and homogeneous catalysis, covering a wide range of chemical transformations. These include various types of catalysis, such as those mediated by photons, plasmons, and electrons. The focus of the studies is to understand the relationship between catalytic function and the underlying chemical properties of surfaces and metal complexes.
The articles in the journal offer innovative concepts and explore the synthesis and kinetics of inorganic solids and homogeneous complexes. Furthermore, they discuss spectroscopic techniques for characterizing catalysts, investigate the interaction of probes and reacting species with catalysts, and employ theoretical methods.
The research presented in the journal should have direct relevance to the field of catalytic processes, addressing either fundamental aspects or applications of catalysis.