Interaction between CeO<sub>2</sub> and ZrO<sub>2</sub> in HCl catalytic oxidation

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Interaction between CeO₂ and ZrO₂ in HCl catalytic oxidation

更新时间：2025-12-10

- Interaction between CeO₂ and ZrO₂ in HCl catalytic oxidation
- CIESC Journal Issue 12, Pages: 5081-5089(2018)
- 作者机构：
  
  1. 南京工业大学材料化学工程国家重点实验室,江苏,南京,210009
  2. 南京工业大学化工学院,江苏,南京,210009
- 作者简介：
- 基金信息：
- DOI：10.11949/j.issn.0438-1157.20180443
  CLC： Q028.8
- Online First：05 December 2018，
  
  Published：05 December 2018
- 稿件说明：
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FEI Zhaoyang, LI Lei, CHENG Chao, et al. Interaction between CeO₂ and ZrO₂ in HCl catalytic oxidation[J]. CIESC Journal, 2018, (12): 5081-5089. DOI: 10.11949/j.issn.0438-1157.20180443.
DOI：

FEI Zhaoyang, LI Lei, CHENG Chao, et al. Interaction between CeO₂ and ZrO₂ in HCl catalytic oxidation[J]. CIESC Journal, 2018, (12): 5081-5089. DOI: 10.11949/j.issn.0438-1157.20180443. DOI：

摘要

采用浸渍法制备了不同负载量的ZrO2/CeO2·（xZr/Ce）和CeO2/ZrO2·（yCe/Zr）两组催化剂。并采用XRD、Raman、N2-Sorption、TEM和H2-TPR等手段对xZr/Ce和yCe/Zr的结构和性质进行表征，并结合HCl催化氧化活性研究CeO2与ZrO2在反应体系中的相互作用。结果显示，CeO2表面掺杂适量的Zr4+可以增加xZr/Ce表面氧空位浓度，提高其HCl氧化反应活性；但当CeO2表面掺杂过量的Zr4+，Zr元素会以ZrO2的形式存在于xZr/Ce表面，覆盖氧空位，降低了xZr/Ce的反应活性。对于yCe/Zr催化剂，ZrO2表面高分散的CeO2有利于催化活性的提高，但ZrO2表层负载的CeO2对催化活性的贡献具有阈值，当CeO2负载量超过10%后，额外增加的铈物种对催化活性已无显著促进作用；对比发现xZr/Ce的氧空位主要来自于铈锆固溶体，yCe/Zr的氧空位主要来自于高分散的CeO2，由铈锆固溶体产生的氧空位对活性提升更有利；与纯组分CeO2相比，xZr/Ce与yCe/Zr两组催化剂在苛刻条件下的长期稳定性测试中均表现出高反应稳定性。

Abstract

ZrO2/CeO2 (xZr/Ce) and CeO2/ZrO2 (yCe/Zr) catalysts with different loading were prepared by wet impregnation method. XRD

Raman

N2-Sorption

TEM and H2-TPR were used to study the interaction between CeO2 and ZrO2 in the recycling of Cl2 from HCl oxidation. The results showed that the doping appropriate amount of zirconium species on the surface of CeO2 could increase the concentration of oxygen vacancy over xZr/Ce

which was in favor of enhancing the activity of HCl oxidation. When there were too many Zr4+ doping on the surface of CeO2

a part of Zr elements would be presented as ZrO2 over the surface of xZr/Ce and the oxygen vacancy was covered

which was unfavorable to the activity of HCl oxidation. For yCe/Zr catalyst

the dispersive CeO2 over ZrO2 was beneficial to the improvement of the catalytic activity

but the increase of catalytic activity would slow down when the loading of CeO2 exceed 10%. By comparing xZr/Ce with yCe/Zr catalysts

the oxygen vacancy of xZr/Ce was mainly formed by Ce-Zr solid solution

while the oxygen vacancy of yCe/Zr was formed by highly dispersive CeO2. It was found that the oxygen vacancy produced by different structure have different effects on the activity. The oxygen vacancies produced by Ce-Zr solid solution are more favorable to the activity enhancement. The ability of chlorine resistance of xZr/Ce and yCe/Zr catalysts behaved a superior stability in the long-term test compared to pure CeO2.

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