Synthesis of highly-dispersed CuO-CeO2 catalyst through a chemisorption-hydrolysis route for CO preferential oxidation in H2-rich stream

被引:48
作者
Meng, Ming [1 ]
Liu, Yaqiong [1 ]
Sun, Zhaosong [1 ]
Zhang, Lijie [1 ]
Wang, Xitao [1 ]
机构
[1] Tianjin Univ, Tianjin Key Lab Appl Catalysis Sci & Engn, Sch Chem Engn & Technol, Tianjin 300072, Peoples R China
基金
中国国家自然科学基金; 高等学校博士学科点专项科研基金;
关键词
Chemisorption-hydrolysis; Cu dispersion; CO preferential oxidation; CuO-CeO2; HYDROGEN-RICH STREAM; CU-CE-O; CARBON-MONOXIDE; SELECTIVE OXIDATION; ACTIVE-SITES; H-2; CUO/CEO2; EXCESS; COPPER; CERIA;
D O I
10.1016/j.ijhydene.2012.07.075
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
The CuO-CeO2 catalyst (CuO loading: 15 wt%) was prepared by a novel chemisorption-hydrolysis method, and employed for the preferential oxidation of CO (CO PROX) in H-2-rich stream. For comparison, several other conventional methods such as impregnation, co-precipitation and deposition-precipitation were also used to prepare the catalyst. It is found that the CuO CeO2 catalyst prepared by chemisorption-hydrolysis method exhibits the best catalytic performance, giving not only the widest temperature window (120-170 degrees C) for CO complete conversion, but also the highest oxygen to CO2 selectivity of 99.9% at 120 degrees C. The results of XRD, N2O chemisorption and in-situ FT-IR conformably indicate that this catalyst possesses the highest dispersion of Cu species, which facilitates the formation of Cu+ carbonyl species, and simultaneously prevents the adsorption and oxidation of H-2. With the increase of reaction temperature, Cu+ is gradually reduced to Cu-0, enhancing the adsorption and oxidation of H-2, as a result, the selectivity of oxygen towards CO2 is lowered obviously. The presence of CO2 and H2O exhibits negative effects on the catalytic performance, shortening the activity window to 150-170 degrees C region and decreasing the CO2 selectivity to 87% at the temperature for the initial 100% conversion of CO. Based on the above study, a potential reaction pathway for CO PROX over the CuO-CeO2 catalyst is proposed. Copyright (C) 2012, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.
引用
收藏
页码:14133 / 14142
页数:10
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