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Advanced Kinetic and Titration Strategies for Assessing the Intrinsic Kinetics on Oxide and Sulfide Catalysts

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Abstract

Found on the surfaces of transition metal oxides or sulfides are metal cations and oxygen or sulfur anions (Mn+-O2− or Mn+-S2−) with diverse catalytic functions as redox sites (Mn+-O2− → M-□), Brønsted acid sites (M-OH), and Lewis acid–base sites (Mδ+-O2−). These active site pairs often work together in catalyzing the chemical transformation in cascade reactions. This article describes several experimental strategies, combining kinetic and titration methods, to decouple the effects of surface site occupation on turnover rates, identify the kinetic bottlenecks, remove the effects arising from deactivation, as well as elucidate the potential participation of multiple types of active sites. Using a correlative approach in connecting the rate dependencies and titration studies, one could pinpoint the key factors that contribute to the rates and interpret the measured rates in terms of molecular events on the surfaces.

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Acknowledgements

This work was supported by Suncor Energy Inc., Imperial Oil, Canada Foundation for Innovation (CFI), and the Natural Sciences and Engineering Research Council of Canada (NSERC) through Collaborative Research and Development Grant CRDPJ543577-19 and CRDPJ476457-14. H. Cai acknowledges the financial support from the National Natural Science Foundation of China (NSFC, Grant No. 22208299). G. Cai and W. T. Broomhead acknowledge financial support from the University of Toronto Graduate Student Endowment Fund. We thank A. Rodriguez (Western University) for preparing the bulk FeMoOx catalysts and W. Tian (Western University) for preparing the VOx/TiO2 catalysts.

Funding

NSERC, CRDPJ543577-19, Ya-Huei Cathy Chin, CRDPJ476457-14, Ya-Huei Cathy Chin, National Natural Science Foundation of China, 22208299, Haiting Cai

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  1. Department of Chemical Engineering and Applied Chemistry, University of Toronto, Toronto, ON, M5S 3E5, Canada

    Guangming Cai, William T. Broomhead, Ya-Huei Cathy Chin & Haiting Cai

  2. Institute of Industrial Catalysis, State Key Laboratory of Green Chemistry Synthesis Technology, College of Chemical Engineering, Zhejiang University of Technology, Hangzhou, Zhejiang, 310014, China

    Haiting Cai

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Cai, G., Broomhead, W.T., Chin, YH.C. et al. Advanced Kinetic and Titration Strategies for Assessing the Intrinsic Kinetics on Oxide and Sulfide Catalysts. Top Catal 66, 1102–1119 (2023). https://doi.org/10.1007/s11244-023-01849-w

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