HCl oxidation for sustainable Cl2 recycle over the CexZr1- xO2 catalysts: Effects of Ce/Zr ratio on activity and stability

Zhaoyang Fei; Xingxing Xie; Yong Dai; Haoyue Liu; Xian Chen; Jihai Tang; Mifen Cui; Xu Qiao

doi:10.1021/ie503297k

HCl oxidation for sustainable Cl₂ recycle over the Ce_xZr_{1- x}O₂ catalysts: Effects of Ce/Zr ratio on activity and stability

Zhaoyang Fei, Xingxing Xie, Yong Dai, Haoyue Liu, Xian Chen, Jihai Tang, Mifen Cui, Xu Qiao

College of Chemical Engineering

Nanjing Tech University

Research output: Contribution to journal › Article › peer-review

39 Scopus citations

Abstract

Ce_xZr_1-xO₂ oxides prepared by a soft reactive grinding (SRG) procedure have been investigated as the catalysts for HCl oxidation. The results show that the catalytic activities and stabilities of Ce_xZr_1-xO₂ oxides are remarkably dependent on the Ce/Zr ratio. A correlation between the physicochemical properties and catalytic performances of these samples reveals that the cubic phase in Ce_xZr_1-xO₂ with higher oxygen storage capacity (OSC) is more active for HCl oxidation, but the tetragonal phase is crucial to the stability of the catalysts. The Ce_0.5Zr_0.5O₂ catalyst with mixed phases and the highest OSC (80 μmol_O2·g_cat^-1) exhibits an excellent activity (1.89 g_Cl2·g_cat^-1·h^-1 at 430 °C) and stability (300 h) in the target reaction. Kinetic studies show that both O₂ and HCl competed for the active sites rendering desorption of surface Cl as the rate-determining step. Accelerating the replacement of surface Cl by O₂ is essential for improving the activity of Ce_0.5Zr_0.5O₂.

Original language	English
Pages (from-to)	19438-19445
Number of pages	8
Journal	Industrial and Engineering Chemistry Research
Volume	53
Issue number	50
DOIs	https://doi.org/10.1021/ie503297k
State	Published - 17 Dec 2014

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title = "HCl oxidation for sustainable Cl2 recycle over the CexZr1- xO2 catalysts: Effects of Ce/Zr ratio on activity and stability",

abstract = "CexZr1-xO2 oxides prepared by a soft reactive grinding (SRG) procedure have been investigated as the catalysts for HCl oxidation. The results show that the catalytic activities and stabilities of CexZr1-xO2 oxides are remarkably dependent on the Ce/Zr ratio. A correlation between the physicochemical properties and catalytic performances of these samples reveals that the cubic phase in CexZr1-xO2 with higher oxygen storage capacity (OSC) is more active for HCl oxidation, but the tetragonal phase is crucial to the stability of the catalysts. The Ce0.5Zr0.5O2 catalyst with mixed phases and the highest OSC (80 μmolO2·gcat-1) exhibits an excellent activity (1.89 gCl2·gcat-1·h-1 at 430 °C) and stability (300 h) in the target reaction. Kinetic studies show that both O2 and HCl competed for the active sites rendering desorption of surface Cl as the rate-determining step. Accelerating the replacement of surface Cl by O2 is essential for improving the activity of Ce0.5Zr0.5O2.",

author = "Zhaoyang Fei and Xingxing Xie and Yong Dai and Haoyue Liu and Xian Chen and Jihai Tang and Mifen Cui and Xu Qiao",

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T1 - HCl oxidation for sustainable Cl2 recycle over the CexZr1- xO2 catalysts

T2 - Effects of Ce/Zr ratio on activity and stability

AU - Fei, Zhaoyang

AU - Xie, Xingxing

AU - Dai, Yong

AU - Liu, Haoyue

AU - Chen, Xian

AU - Tang, Jihai

AU - Cui, Mifen

AU - Qiao, Xu

PY - 2014/12/17

Y1 - 2014/12/17

N2 - CexZr1-xO2 oxides prepared by a soft reactive grinding (SRG) procedure have been investigated as the catalysts for HCl oxidation. The results show that the catalytic activities and stabilities of CexZr1-xO2 oxides are remarkably dependent on the Ce/Zr ratio. A correlation between the physicochemical properties and catalytic performances of these samples reveals that the cubic phase in CexZr1-xO2 with higher oxygen storage capacity (OSC) is more active for HCl oxidation, but the tetragonal phase is crucial to the stability of the catalysts. The Ce0.5Zr0.5O2 catalyst with mixed phases and the highest OSC (80 μmolO2·gcat-1) exhibits an excellent activity (1.89 gCl2·gcat-1·h-1 at 430 °C) and stability (300 h) in the target reaction. Kinetic studies show that both O2 and HCl competed for the active sites rendering desorption of surface Cl as the rate-determining step. Accelerating the replacement of surface Cl by O2 is essential for improving the activity of Ce0.5Zr0.5O2.

AB - CexZr1-xO2 oxides prepared by a soft reactive grinding (SRG) procedure have been investigated as the catalysts for HCl oxidation. The results show that the catalytic activities and stabilities of CexZr1-xO2 oxides are remarkably dependent on the Ce/Zr ratio. A correlation between the physicochemical properties and catalytic performances of these samples reveals that the cubic phase in CexZr1-xO2 with higher oxygen storage capacity (OSC) is more active for HCl oxidation, but the tetragonal phase is crucial to the stability of the catalysts. The Ce0.5Zr0.5O2 catalyst with mixed phases and the highest OSC (80 μmolO2·gcat-1) exhibits an excellent activity (1.89 gCl2·gcat-1·h-1 at 430 °C) and stability (300 h) in the target reaction. Kinetic studies show that both O2 and HCl competed for the active sites rendering desorption of surface Cl as the rate-determining step. Accelerating the replacement of surface Cl by O2 is essential for improving the activity of Ce0.5Zr0.5O2.

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HCl oxidation for sustainable Cl₂ recycle over the Ce_xZr_{1- x}O₂ catalysts: Effects of Ce/Zr ratio on activity and stability

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