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Operando experimental evidence on the central role of oxygen vacancies during methane combustion
Journal of Catalysis ( IF 6.5 ) Pub Date : 2020-07-31 , DOI: 10.1016/j.jcat.2020.07.024
Majid D. Farahani , Moritz Wolf , Thabiso P.O. Mkhwanazi , Michael Claeys , Holger B. Friedrich

Catalytic methane combustion is an important reaction for many industries active in energy domains, since methane is a greenhouse gas and has a high H/C ratio, which makes it a suitable replacement for oil and coal. Here, operando magnetometry, unsteady state propane dehydrogenation, XPS analysis and temperature programmed desorption of oxygen species are applied to investigate the parameters affecting methane combustion in situ using inexpensive bimetallic ferrite spinels as catalysts. Also, fresh, post catalytic and operando characterizations of the catalysts showed that oxygen vacancies are a key factor for the generation of activated interfacial oxygen species, which facilitates the dehydrogenation mechanism. Here, nickel ferrite outperformed cobalt, copper, and zinc ferrite, in methane combustion, as it displays superior thermal stability and benefits from a synergy between different active sites. NiFe2O4 provides oxygen vacancies and partially reduced metal sites with dehydrogenation ability that participate in H abstraction from methane (rate determining step).



中文翻译:

Operando实验证据证明甲烷中氧空位的重要作用

对于许多活跃于能源领域的行业而言,催化甲烷燃烧是一项重要的反应,因为甲烷是一种温室气体,并且具有很高的H / C比,这使其成为石油和煤炭的合适替代品。在这里,使用操作磁力仪,非稳态丙烷脱氢,XPS分析和程序升温对氧气进行脱附来研究影响甲烷原位燃烧的参数使用廉价的双金属铁氧体尖晶石作为催化剂。而且,催化剂的新鲜,后催化和操作特性表明,氧空位是产生活化的界面氧种类的关键因素,这促进了脱氢机理。在甲烷燃烧中,镍铁氧体的性能优于钴,铜和锌铁氧体,因为它显示出优异的热稳定性,并受益于不同活性部位之间的协同作用。NiFe 2 O 4提供了氧空位和具有脱氢能力的部分还原的金属位点,这些位点参与了从甲烷中提取H(速率确定步骤)。

更新日期:2020-08-28
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