On the performance of Ag/Al2O3 as a HC-SCR catalyst - influence of silver loading, morphology and nature of the reductant

被引:39
|
作者
Kannisto, Hannes [1 ]
Arve, Kalle [2 ]
Pingel, Torben [3 ]
Hellman, Anders [4 ]
Harelind, Hanna [1 ]
Eranen, Kari [2 ]
Olsson, Eva [3 ]
Skoglundh, Magnus [1 ]
Murzin, Dmitry Yu. [2 ]
机构
[1] Chalmers Univ Technol, Competence Ctr Catalysis KCK, Dept Chem & Biol Engn, SE-41296 Gothenburg, Sweden
[2] Abo Akad Univ, Lab Ind Chem & Chem Engn, Proc Chem Ctr, FIN-20500 Turku, Finland
[3] Chalmers Univ Technol, Dept Appl Phys, SE-41296 Gothenburg, Sweden
[4] Chalmers Univ Technol, Competence Ctr Catalysis KCK, Dept Appl Phys, SE-41296 Gothenburg, Sweden
基金
瑞典研究理事会;
关键词
LEAN NOX REDUCTION; SELECTIVE REDUCTION; SILVER/ALUMINA CATALYST; HIGHER HYDROCARBONS; ALUMINA CATALYSTS; BURN CONDITIONS; OXYGEN; AG/ALUMINA; HYDROGEN; OXIDE;
D O I
10.1039/c2cy20594g
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
This study focuses on the performance of Ag/Al2O3 catalysts for hydrocarbon selective catalytic reduction (HC-SCR) of NOx under lean conditions, using complex hydrocarbons as reductants. The aim is to elucidate the correlation towards the silver loading and morphology, with respect to the nature of the reductant. Ag/Al2O3 samples with either 2 or 6 wt% silver loading were prepared, using a sol-gel method including freeze-drying. The catalytic performance of the samples was evaluated by flow reactor experiments, with paraffins, olefins and aromatics of different nature as reductants. The physiochemical properties of the samples were characterized by scanning electron microscopy/energy dispersive X-ray spectroscopy, scanning transmission electron microscopy/high angle annular dark field imaging, X-ray photoelectron spectroscopy and N-2-physisorption. The 2 wt% Ag/Al2O3 sample was found to be the most active catalyst in terms of NOx reduction. However, the results from the activity studies revealed that the decisive factor for high activity at low temperatures is not only connected to the silver loading per se. There is also a strong correlation between the silver loading and morphology (i.e. the ratio between low- and high-coordinated silver atoms) and the nature of the hydrocarbon, on the activity for NOx reduction. Calculated reaction rates over the low-coordinated step and high-coordinated terrace sites showed that the morphology of silver has a significant role in the HC-SCR reaction. For applications which include complex hydrocarbons as reductants (e.g. diesel), these issues need to be considered when designing highly active catalysts.
引用
收藏
页码:644 / 653
页数:10
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