State of active components on the surface of the PdCl2-CuCl2/γ-Al2O3 catalyst for the low-temperature oxidation of carbon monoxide

被引:0
作者
D. N. Titov
A. V. Ustyugov
O. P. Tkachenko
L. M. Kustov
Ya. V. Zubavichus
A. A. Veligzhanin
N. V. Sadovskaya
I. V. Oshanina
L. G. Bruk
O. N. Temkin
机构
[1] Moscow State Academy of Fine Chemical Technology,Zelinsky Institute of Organic Chemistry
[2] Russian Academy of Sciences,undefined
[3] Kurchatov Institute Russian Research Center,undefined
[4] Karpov Institute of Physical Chemistry,undefined
来源
Kinetics and Catalysis | 2012年 / 53卷
关键词
Palladium; Chlorine Atom; Crystal Line Phase; Camite; Pure Oxygen Environment;
D O I
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中图分类号
学科分类号
摘要
The state of the active constituents of the freshly prepared PdCl2-CuCl2/γ-Al2O3 catalyst for the low-temperature oxidation of the carbon monoxide by molecular oxygen was studied by X-ray absorption spectroscopy (XAS), powder X-ray diffraction (XRD), scanning electron microscopy (SEM), and diffuse reflectance IR Fourier transform spectroscopy (DRIFTS). It was shown that copper in the form of a crystalline phase of Cu2Cl(OH)3 with the structure of the mineral paratacamite and palladium chloride in an amorphous state occurred on the surface of γ-Al2O3. According to XAS data, the local environment of palladium consisted of four chlorine atoms, which formed a flat square with an increased distance between palladium and one of the chlorine atoms. The evolution of the local environments of copper and palladium upon a transition from the initial salts to the impregnating solutions and chlorides on the surface of γ-Al2O3 was considered. The role of γ-Al2O3 in the formation of the Cu2Cl(OH)3 phase was discussed. It was found by the DRIFTS method that linear (2114 cm−1) and bridging (1990 and 1928 cm−1) forms of coordinated carbon monoxide were formed upon the adsorption of CO on the catalyst surface. The formation of CO2 upon the interaction of coordinated CO with atmospheric oxygen was detected. Active sites including copper and palladium were absent from the surface of the freshly prepared catalyst.
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页码:262 / 273
页数:11
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