Citation: XIE Xing-Xing, FEI Zhao-Yang, ZOU Chong, LI Zheng-Zhou, CHEN Xian, TANG Ji-Hai, CUI Mi-Fen, QIAO Xu. Effects of Rare-Earth Additives on Structures and Performances of CuO-CeO₂-SiO₂ Catalysts for Recycling Cl₂ from HCl Oxidation[J]. Acta Physico-Chimica Sinica, ;2015, 31(6): 1153-1161. doi: 10.3866/PKU.WHXB201504145 shu

Effects of Rare-Earth Additives on Structures and Performances of CuO-CeO₂-SiO₂ Catalysts for Recycling Cl₂ from HCl Oxidation

XIE Xing-Xing ^1,2 ,
FEI Zhao-Yang ^1,2, ,
ZOU Chong ^1,2 ,
LI Zheng-Zhou ^1,2 ,
CHEN Xian ² ,
TANG Ji-Hai ² ,
CUI Mi-Fen ² ,
QIAO Xu ^1,2,

1.
1 State Key Laboratory of Materials-Oriented Chemical Engineering, Nanjing Tech University, Nanjing 210009, P. R. China;
2 College of Chemistry and Chemical Engineering, Nanjing Tech University, Nanjing 210009, P. R. China

Received Date: 23 December 2014
Available Online: 14 April 2015
Fund Project: 国家科技支撑计划(2011BAE18B01) (2011BAE18B01) 江苏省科技支撑计划(BE2011830) (BE2011830) 江苏省高校自然科学基金面上项目(13KJB530006) (13KJB530006) 国家自然科学基金(21306089) (21306089)中国博士后基金(2013M531340)资助 (2013M531340)

CuO-CeO₂-SiO₂ and rare-earth-doped CuO-Ce_0.9M_0.1O₂-SiO₂ (M=La, Pr, Nd) catalysts for recycling Cl₂ from HCl oxidation were prepared by a template method, using activated carbon as a hard template. The catalyst structures were determined using X-ray diffraction (XRD), N₂ adsorption-desorption, transmission electron microscopy (TEM), Raman spectroscopy, X-ray photoelectron spectroscopy (XPS), and H₂ temperatureprogrammed reduction (H₂-TPR). The catalytic performances were also investigated. The results showed that La, Pr, and Nd cations were incorporated into the CeO₂ lattice and formed nanosized solid solutions; this greatly reduced the catalyst grain sizes, leading to higher surface areas. In addition, the oxygen vacancy concentrations were significantly improved. The changes in the structures and surface properties of the solid solutions significantly affected the HCl catalytic oxidation performances. The order of the activities of various catalysts was CuO-Ce_0.9La_0.1O₂-SiO₂>CuO-Ce_0.9Nd_0.1O₂-SiO₂>CuO-Ce_0.9Pr_0.1O₂-SiO₂>CuO-CeO₂-SiO₂. The oxygen vacancy concentrations of the solid solutions were strongly related to their catalytic activities. However, the structures and performances of the Ce_0.9M_0.1O₂-SiO₂ catalysts showed that an increase in the number of oxygen vacancies resulted in decreased catalytic activities of the solid solutions. Kinetic studies showed that oxygen adsorption could be the rate-determining step for rare-earth-doped catalysts; a higher oxygen vacancy concentration in the solid solution led to a slower reaction rate when the volumetric flow ratio of O₂ to HCl was 1. For the CuOCe_0.9M_0.1O₂-SiO₂ catalysts, spillover of oxygen species in the solid solution into the highly dispersed CuO interfaces was enhanced, which increased the overall reaction rate and gave high activity.
- Rare earth,
- CuO-CeO₂,
- HCl,
- Catalytic oxidation,
- Chlorine,
- Oxygen vacancy
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Effects of Rare-Earth Additives on Structures and Performances of CuO-CeO2-SiO2 Catalysts for Recycling Cl2 from HCl Oxidation

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Effects of Rare-Earth Additives on Structures and Performances of CuO-CeO₂-SiO₂ Catalysts for Recycling Cl₂ from HCl Oxidation