Effect of strongly bound copper species in copper-ceria catalyst for preferential oxidation of carbon monoxide

被引:48
作者
Du, Pei-Pei [1 ]
Wang, Wei-Wei [2 ]
Jia, Chun-Jiang [2 ]
Song, Qi-Sheng [2 ]
Huang, Yu-Ying [1 ]
Si, Rui [1 ]
机构
[1] Chinese Acad Sci, Shanghai Synchrotron Radiat Facil, Shanghai Inst Appl Phys, Shanghai, Peoples R China
[2] Shandong Univ, Key Lab Colloid & Interface Chem, Key Lab Special Aggregated Mat, Sch Chem & Chem Engn, Jinan 250100, Peoples R China
基金
美国国家科学基金会;
关键词
Copper-ceria; Preferential oxidation of carbon monoxide; Ammonium carbonate leaching; X-ray absorption fine structure; Coprecipitation; X-RAY-ABSORPTION; SELECTIVE CO OXIDATION; CUO-CEO2; CATALYSTS; OXIDE CATALYST; IN-SITU; CUO/CEO2; REDOX PROPERTIES; H-2-RICH GAS; PROX; CU;
D O I
10.1016/j.apcata.2015.10.041
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
Copper-ceria catalysts with the Cu contents up to 40 at.% were prepared by the coprecipitation method. Ammonium carbonate was used as the leaching agent on the as-calcined samples to remove the weakly bound copper species. The parent and leached catalysts were tested for the preferential oxidation of carbon monoxide (CO-PROX) reaction from 40 to 200 degrees C in 1%CO/1%O-2/50%H-2/N-2 with a space velocity of 60,000 mL h(-1) g(cat)(-1). When the Cu doping amount reached 30 at.%, the stable and constant CO-PROX reactivity, including CO conversion and 02 selectivity, was presented for both parent and ammonium carbonate leached catalysts. The fresh and used samples have been carefully characterized by various techniques such as power X-ray diffraction (XRD), X-ray absorption fine structure (XAFS), transmission electron microscopy (TEM), X-ray Photoelectron Spectroscopy (XPS) and temperature-programmed reduction by hydrogen (H-2-TPR). It was confirmed that there are two different types of copper species, i.e. weakly bound CuOx clusters and strongly bound Cu-[O-x]-Ce structure, in both parent and leached catalysts. Furthermore, we have demonstrated that the weakly bound CuOx clusters removed by ammonium carbonate can be recovered by the migration of Cu-[O-x]-Ce species under the reduction or reaction conditions. The strongly bound copper species in CeO2 have been identified to be the reservoir for the active Cu sites for CO-PROX. (C) 2015 Elsevier B.V. All rights reserved.
引用
收藏
页码:87 / 101
页数:15
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