Role of oxygen transfer and surface reaction in catalytic performance of VOx-Ce1‒xZrxO2 for propane dehydrogenation

doi:10.1016/S1872-2067(23)64494-8

Abstract

Abstract:

The bulk oxygen transfer and surface reaction as important parts of the chemical looping-related process are crucial for the rational design of new redox catalysts. This paper describes an experimental study on the effect of bulk oxygen transfer and surface reaction in Ce_1‒_xZr_xO₂ supported VO_x redox catalysts for the chemical looping oxidative propane dehydrogenation reaction. It was found that the introduction of Zr dictates the reaction performance of the redox catalyst by modulating the bulk oxygen transfer and surface reaction. The kinetic study reveals that the instantaneous reduction rate of the redox catalysts is determined by the H-abstraction step in the surface reaction. The introduction of Zr can reduce the activation energy of the H-abstraction step, which leads to the enhancement of the instantaneous reduction rate. Meanwhile, the oxygen supply capacity of the cerium oxide is increased by Zr, allowing the surface reaction to proceed over longer durations. Furthermore, the reaction model derived from the kinetics study is validated using a number of (quasi) in situ techniques. This study provides fundamental insights into the role of bulk oxygen transfer and surface reaction in chemical looping or related process.

Key words: Propane dehydrogenation, Vanadia catalyst, Redox chemistry, Surface reaction, Bulk diffusion

Jiachen Sun, Sai Chen, Donglong Fu, Wei Wang, Xianhui Wang, Guodong Sun, Chunlei Pei, Zhi-Jian Zhao, Jinlong Gong. Role of oxygen transfer and surface reaction in catalytic performance of VO_x-Ce_1‒_xZr_xO₂ for propane dehydrogenation[J]. Chinese Journal of Catalysis, 2023, 52: 217-227.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(23)64494-8

https://www.cjcatal.com/EN/Y2023/V52/I9/217

Figures/Tables 5

Fig. 1. Structure characterizations of V-Ce1-xZrxO2 redox catalysts with different Zr contents. (a) XRD patterns. (b) 532 nm excited Raman specrta of the dehydrated V-Ce1-xZrxO2. (c) Vanadyl stretching region of 532 nm Raman spectra. (d) Illustration of structural for V-Ce1-xZrxO2. (e) The XPS spectra of V 2p3/2. (f) HRTEM and EDS-STEM images of V-Ce0.3Zr0.7O2.

Fig. 2. Comparisons of propane dehydrogenation over V-Ce1-xZrxO2 redox catalysts with different Zr contents. (a) Propane conversion and propylene selectivity as a function of reaction time. (b) Contribution of ODH in propylene formation. Test conditions: 600 °C, 1.4 atmospheric pressure, WHSV = 1 h-1, 0.5 g sample, C3H8/N2 = 4:21.

Fig. 3. Temperature programmed reduction and reaction of V-Ce1-xZrxO2 redox catalysts with different Zr contents. (a) H2-TPR profiles of V-Ce1-xZrxO2 (solid lines) and pure Ce1-xZrxO2 (dash lines). (b) The H2O signal of V-Ce1-xZrxO2 during C3H8-TPR.

Fig. 4. Effects of bulk oxygen transfer and surface reaction on surface oxygen coverage of V-Ce1-xZrxO2. (a) Experimental data and kinetics ftting (dashed lines) for the reduction of V-Ce1-xZrxO2 by C3H8. (b) Oxygen coverage as a function of the reaction time. (c) Dependencies of the rate constant for the first cleavage of the C-H step (k2) on the temperature. (d) Proposed reaction model over V-Ce1-xZrxO2 during dehydrogenation stage.

Fig. 5. Structural evolution of VOx over V-Ce1-xZrxO2 redox catalysts during propane dehydrogenation reaction. In situ DRIFTS spectrum of V-CeO2 (a), V-Ce0.5Zr0.5O2 (b), V-Ce0.3Zr0.7O2 (c) and V-ZrO2 (d). (e) The time profile of the normalized intensity of V=O. (f) The calculated intensity ratios of Ce3+/V=O.

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Role of oxygen transfer and surface reaction in catalytic performance of VO_x-Ce_1‒_xZr_xO₂ for propane dehydrogenation

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