期刊
APPLIED SURFACE SCIENCE
卷 556, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.apsusc.2021.149713
关键词
Spinel Co3O4; Methane oxidation; In-situ XPS; In-situ Raman; Active oxygen species
类别
资金
- National Key Research and Development Project of Research [2017YFC0212805]
- National Natural Science Foundation of China [51878292]
- Natural Science Foundation of Guangdong Province, China [2015B020236002]
The study found that the methane oxidation activity of spinel Co3O4 catalysts depends on the different exposed crystal planes, with the high catalytic activity mainly associated with the high exposure of Co3+ and surface lattice oxygen. Adsorption oxygen species play a role in generating reactive oxygen species during the transformation of Co3+ and Co2+ structures.
Identifying the activity origin of spinel Co3O4 catalysts is extremely important for fundamental research and practical application. It is reported that octahedrally coordinated Co3+ (Co-oh(3+)) is considered as active sites in spinel Co3O4, but there is still a lack of sufficient evidence to prove the effect of Co species. In this work, we synthesized accurately the three spinel Co3O4 samples with different exposed crystal planes to investigate the reaction mechanism between methane molecule and Co species. The activity results show that methane oxidation activities follow an order of Co3O4-(2 2 0) > Co3O4-(3 1 1) > Co3O4-(1 1 1). A series of in-situ characterization analyses are performed to explore the evolution process of Co species and the transform of lattice oxygen species for methane combustion. The results indicate that the high catalytic activity is assigned to the exposed state of surface lattice oxygen atoms and the mutual transformation of Co3+ oh and Co2+ 0h . Therefore, it explained that the high activity of the (2 2 0) crystal plane is mainly involved with the high exposure of Co3+ and surface lattice oxygen. Adsorption oxygen species were induced to reactive oxygen species during the transformation of Co3+ oh stable structure and Co2+ oh unstable structure.
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