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Selective catalytic reduction of NO by methane over Co,H-SSZ-13 catalysts: Types and catalytic functions of active Co sites
Journal of Catalysis ( IF 7.3 ) Pub Date : 2020-03-24 , DOI: 10.1016/j.jcat.2020.02.018
Rania Charrad , Hanna E. Solt , Attila Domján , Faouzi Ayari , Mourad Mhamdi , József Valyon , Ferenc Lónyi

Co-SSZ-13 zeolite catalysts were prepared by solid-state ion exchange with CoCl2 salt for the selective catalytic reduction of NO with methane (CH4/NO–SCR). Fresh catalysts contained hard-to-reduce lattice Co2+/[Co-OH]+ ions and showed activity proportional to the concentration of these species. The NO conversion was accompanied by steam-generating methane oxidation. Under the arising hydrothermal conditions, a fraction of Co ions transformed into Co-oxo species especially in catalysts of high Co content (Co/AlF > 0.3), resulting in boosted activity in NO2-forming catalytic NO oxidation. The increased NO2 concentration brought about higher concentration of surface cobalt nitrate species responsible for the rate-determining methane activation, so the overall rate of the NO–SCR reaction was also accelerated. Steam admixed to the feed decreased the conversion of methane more significantly than that of NO. Its observed high hydrothermal stability renders the Co-SSZ-13 catalyst a very promising candidate for the CH4/NO–SCR reaction.



中文翻译:

Co,H-SSZ-13催化剂上甲烷选择性催化还原NO的作用:活性Co位的类型和催化功能

Co-SSZ-13沸石催化剂是通过与CoCl 2盐进行固态离子交换而制备的,用于用甲烷(CH 4 / NO-SCR)选择性催化还原NO 。新鲜的催化剂包含难以还原的晶格Co 2+ / [Co-OH] +离子,并且其活性与这些物质的浓度成正比。NO转化伴随着蒸汽产生的甲烷氧化。在出现的水热条件下,一部分Co离子特别是在高Co含量(Co / Al F  > 0.3)的催化剂中转化为Co-oxo物种,从而提高了NO 2的活性,形成了催化型NO氧化。增加的NO 2甲烷浓度的增加导致决定甲烷活化速率的表面硝酸钴种类的浓度增加,因此NO-SCR反应的总速率也加快了。混合到进料中的蒸汽比NO降低了甲烷的转化率。它观察到的高水热稳定性使Co-SSZ-13催化剂成为CH 4 / NO-SCR反应的非常有希望的候选者。

更新日期:2020-04-09
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