Effect of Cu deposition method on silico aluminophosphate catalysts in NH3-SCR and NH3-SCO reactions

被引:24
|
作者
Schiavoni, Marco [1 ]
Campisi, Sebastiano [1 ]
Gervasini, Antonella [1 ]
机构
[1] Univ Milan, Dipartimento Chim, Via Camillo GoIgi 19, I-20133 Milan, Italy
关键词
Silicoaluminophosphate (SAPO); Copper-chabazite catalysts; Catalyst characterization; NH3-SCR (catalytic nitrogen oxide reduction); NH3-SCO (catalytic ammonia oxidation); ELECTRON-PARAMAGNETIC-RESONANCE; COPPER-BASED CATALYSTS; SELECTIVE REDUCTION; ACTIVE-SITES; NOX; ZEOLITE; AMMONIA; OXIDATION; IONS; NH3;
D O I
10.1016/j.apcata.2017.06.034
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
In this study, a commercial silicoaluminophosphate of chabazite (CHA) structure with low addition of copper phase (ca. 2-3 wt.%) deposited from Cu-acetate, Cu-nitrate, and Cu-chloride precursors (Cu/CHA) with ionic exchange and impregnation procedures was taken into consideration thanks to its known good de-NOx activity. The Cu/CHA samples were tested in the NH3-SCR (catalytic reduction of NOx by NH3) and NH3-SCO (catalytic oxidation of NH3) reactions, in the 200-500 degrees C interval. Important differences of Cu aggregation on CHA surface were evidenced between the samples prepared by ionic-exchange and impregnation, as observed from Uv-DRS, EPR, and H-2-TPR analyses. Well-dispersed Cu-phase on the CHA surface and more aggregated CuOx clusters were formed by depositing the Cu-phase with ionic-exchange and impregnation method, respectively. All the Cu/CHA samples were active and selective in the NH3-SCR reaction in the explored temperature interval, with enhanced performances of the sample prepared by impregnation. NH3-SCO selectivity to N-2 was higher (80-95%) on the samples with lower Cu aggregation while sample with surface CuOx species was less selective (65%) but more active at lower temperatures. Temperature to obtain 50% of ammonia conversion (T-50 degrees C) was around 250 degrees C, for the sample prepared by impregnation, and in the range 355-390 degrees C for the samples prepared by ionic-exchange. The study permitted to disclose the possibility to use Cu/CHA samples in a cascade NH3-SCR and NH3-SCO reactions in a future process for zero emissions of both NOx and NH3.
引用
收藏
页码:162 / 172
页数:11
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