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Kinetics and Mechanism of the Low-Temperature Oxidation of Carbon Monoxide with Oxygen on a PdCl2-CuCl2/γ-Al2O3 Catalyst
被引:7
|作者:
Bruk, L. G.
[1
]
Ustyugov, A. V.
[1
]
Katsman, E. A.
[1
]
Iskhakova, L. D.
[2
]
Oshanina, I. V.
[1
]
Tkachenko, O. P.
[3
]
Kustov, L. M.
[3
,4
]
Temkin, O. N.
[1
]
机构:
[1] Moscow Technol Univ, Moscow 119571, Russia
[2] Russian Acad Sci, Fiber Opt Res Ctr, Moscow 119333, Russia
[3] Russian Acad Sci, Zelinsky Inst Organ Chem, Moscow 119991, Russia
[4] Moscow MV Lomonosov State Univ, Moscow 119991, Russia
基金:
俄罗斯基础研究基金会;
俄罗斯科学基金会;
关键词:
low-temperature oxidation;
carbon monoxide;
copper;
palladium;
metal-complex catalyst;
kinetics;
mechanism;
SUPPORTED PDCL2-CUCL2 CATALYSTS;
WACKER-TYPE CATALYSTS;
CO OXIDATION;
XAFS CHARACTERIZATION;
CU CATALYSTS;
PALLADIUM;
COMPLEXES;
SURFACE;
STATE;
WATER;
D O I:
10.1134/S0023158417020033
中图分类号:
O64 [物理化学(理论化学)、化学物理学];
学科分类号:
070304 ;
081704 ;
摘要:
A systematic study of the kinetics of the low-temperature oxidation of carbon monoxide with oxygen on a PdCl2-CuCl2/gamma-Al2O3 supported catalyst was carried out over a wide range of the partial pressures of oxygen, water, and CO in order to test hypotheses on the reaction mechanism. It was shown that, as the temperature was increased from 20 to 38A degrees C, rate of formation of CO2 decreased and the apparent activation energy was about-40 kJ/mol. The hypotheses of different degrees of complexity concerning the reaction mechanism were formulated based on physicochemical data and a Langmuir-Hinshelwood model. Mechanisms in which carbon dioxide is formed on the interaction of the surface Pd(I) and Pd(II) complexes that include carbon monoxide and water with the surface complex of Cu(I) that coordinates oxygen were recognized as the most probable.
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页码:179 / 190
页数:12
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