催化作用
化学
沸石
水溶液
选择性催化还原
氮氧化物
催化剂中毒
一氧化碳中毒
金属
无机化学
碱金属
柴油
金属中毒
柴油机排气
氮氧化物
氧合物
中和
核化学
氨
作者
Tao Zhang,Jianning Zhang,Feng Yu,Dong Qi,Jian Liu,Junhua Li,Evgenii V. Kondratenko
标识
DOI:10.1021/acs.est.6c07432
摘要
Cu/SSZ-13 is a benchmark catalyst for the selective catalytic reduction (SCR) of NOx with NH3 in diesel exhaust aftertreatment, but its activity can be severely impaired by alkali and alkaline-earth metal poisoning. Conventional impregnation of catalysts with such poisons involves introducing metal species prior to catalytic testing. This means that any poisoning that develops concurrently with catalyst operation is not captured. Here, we develop an aerosol-assisted, reaction-coupled poisoning platform that continuously delivers metal-containing aqueous aerosols to SCR catalysts under hydrated NH3-SCR conditions. At nearly identical K loadings, aerosol-assisted poisoning caused substantially greater deactivation of Cu/SSZ-13 than conventional impregnation of the catalyst, with a more pronounced activity loss after poisoning at 400 °C than at 200 °C. The enhanced deactivation was accompanied by a more spatially extensive K distribution, stronger perturbations of the zeolite framework, preferential alteration of 8-membered-ring-associated [Cu(OH)]+-Z species, spectroscopic signatures consistent with CuOx aggregation, and partial neutralization of Brønsted acid sites. Similar pathway- and temperature-dependent deactivation trends were observed for Na-, Mg-, and Ca-poisoned Cu/SSZ-13 and for K-poisoned V2O5-WO3/TiO2. These results establish aerosol-assisted poisoning as a controlled, accelerated approach for evaluating metal-induced deactivation of SCR catalysts under hydrated reaction conditions.
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