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首页> 外文期刊>ChemCatChem >Selective Catalytic Reduction of NOx with Ammonia over Copper Ion Exchanged SAPO-47 Zeolites in a Wide Temperature Range
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Selective Catalytic Reduction of NOx with Ammonia over Copper Ion Exchanged SAPO-47 Zeolites in a Wide Temperature Range

机译:在宽温度范围内使用铜离子交换SAPO-47沸石的氨的选择性催化还原NOx

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摘要

Copper-exchanged H-SAPO-47 zeolites were synthesized by an aqueous solution ion exchange method and applied in the selective catalytic reduction of NO with NH3 (SCR). The microporous chabazite (CHA) structure of the catalysts was characterized and confirmed using synchrotron X-ray diffraction and nitrogen adsorption-desorption experiments. The synthesized Cu-x-SAPO-47 catalysts exhibited excellent SCR activity and nearly 100% N-2 selectivity in a wide temperature range. The Cu-0.1-SAPO-47 sample exhibited higher activity than the other samples below 250 degrees C. The weak Lewis acid sites originating from the introduction of Cu2+ were more active than the BrOnsted acid sites of the zeolites framework at low temperature. Two types of isolated Cu2+ species with different coordination surroundings were found, namely, Cu2+ cations bonded with the six-membered rings and those bonded in the CHA cages. The former species exhibited good stability and activity at high temperature, whereas the latter ones were more active at low temperature. The Cu-0.1-SAPO-47 catalyst provided a considerable amount of isolated Cu2+ bonded in the CHA cages. These results indicated that active Lewis acid sites and isolated Cu2+ species are responsible for their excellent SCR activity.
机译:通过水溶液离子交换法合成铜交换的H-SAPO-47沸石,并在NH 3(SCR)中的选择性催化还原中施加。使用同步辐射X射线衍射和氮吸附 - 解吸实验表征并确认催化剂的微孔曲谱(CHA)结构。合成的Cu-X-SAPO-47催化剂在宽温度范围内表现出优异的SCR活性和近100%N-2选择性。 Cu-0.1-Sapo-47样品表现出比低于250℃的其他样品更高的活性。源自Cu2 +的弱路易斯酸性位于低温下沸石框架的刚性酸位点更有效。发现了两种孤立的Cu2 +种类,即具有不同的协调周围环境,即与六元环粘合的Cu2 +阳离子和在CHA笼中粘合的阳离子。前一种物种在高温下表现出良好的稳定性和活性,而后者在低温下更活跃。 Cu-0.1-Sapo-47催化剂提供了大量的分离的Cu 2 +在CHA笼中键合。这些结果表明,活性路易斯酸部位和分离的Cu2 +物种是它们优异的SCR活性的原因。

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