Effect of SO2 on the soot oxidation activity of flame spray pyrolysis-made manganese oxide catalyst in gasoline model exhaust

IF 1.7 4区 化学 Q4 CHEMISTRY, PHYSICAL
Markus Werther, Christian Singer, Alexander Gross, Sven Kureti, Juan Carlos Martínez-Munuera, Avelina García-García
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Abstract

This study deals with the effect of SO2 on the soot oxidation activity of flame spray pyrolysis-prepared manganese oxide in gasoline model exhaust. The catalyst was exposed to 15 and 30 ppm SO2 at 250 °C and was characterized by N2 physisorption, SO2-TPD, O2-TPD, DRIFTS, XPS and PXRD. It was shown that the SO2 adsorption results in the formation of surface sulfate, while the uptake increased from 26 to 45 μmol/g with growing sulfur content of the model exhaust. The sulfur adsorption reduces the mobility and availability of oxygen on the catalyst thus inhibiting the oxygen transport from gas phase over the catalyst to the contact points of the soot. Consequently, the soot oxidation activity, investigated with tight contact blends of catalyst and soot, decreases with inclining amount of sulfate. Finally, the sulfate species were mostly removed by thermal treatment at 705 °C, which additionally provoked catalyst sintering. As a result, the catalytic performance of the de-sulfated catalyst was slightly lower compared to the sulfated sample.

二氧化硫对火焰喷射热解制造的氧化锰催化剂在汽油模型废气中烟尘氧化活性的影响
摘要 本研究探讨了二氧化硫对火焰喷射热解制备的氧化锰在汽油模型废气中烟尘氧化活性的影响。催化剂在 250 °C 下分别暴露于 15 和 30 ppm SO2,并通过 N2 物理吸附、SO2-TPD、O2-TPD、DRIFTS、XPS 和 PXRD 对其进行了表征。结果表明,二氧化硫的吸附导致表面硫酸盐的形成,而随着模型废气中硫含量的增加,吸附量从 26 μmol/g 增加到 45 μmol/g。硫的吸附降低了氧在催化剂上的流动性和可用性,从而抑制了氧从催化剂上的气相向烟尘接触点的传输。因此,在催化剂和烟尘紧密接触的情况下,烟尘氧化活性随着硫酸盐含量的增加而降低。最后,在 705 °C 的热处理过程中,大部分硫酸盐物质都被除去了,热处理还导致催化剂烧结。因此,脱硫催化剂的催化性能略低于硫酸盐样品。
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来源期刊
CiteScore
3.30
自引率
5.60%
发文量
201
审稿时长
2.8 months
期刊介绍: Reaction Kinetics, Mechanisms and Catalysis is a medium for original contributions in the following fields: -kinetics of homogeneous reactions in gas, liquid and solid phase; -Homogeneous catalysis; -Heterogeneous catalysis; -Adsorption in heterogeneous catalysis; -Transport processes related to reaction kinetics and catalysis; -Preparation and study of catalysts; -Reactors and apparatus. Reaction Kinetics, Mechanisms and Catalysis was formerly published under the title Reaction Kinetics and Catalysis Letters.
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