期刊
MOLECULAR CATALYSIS
卷 501, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.mcat.2020.111370
关键词
Co/Hydroxyapatite; N2O catalytic decomposition; Active sites; Geometrical effects; Spacing effects
资金
- National Natural Science Foundation of China [21673132]
- Natural Science Foundation of Shanxi Province [201801D121043]
- Key Projects of Shanxi Coal-based Low Carbon Joint Fund [U1710221]
Different methods were used to prepare Co/hydroxyapatite catalysts with various Co species, and it was found that Co(II)(2+)Oh in Co(1.2)-IE prepared by ion exchange exhibited higher catalytic activity and stability, as well as stronger resistance against oxygen and water.
Different methods including ion exchange, impregnation and hydrothermal method were used to prepare Co/hydroxyapatite catalysts with various Co species. The catalytic activities for N2O decomposition were studied. It was concluded that Co(II)(2+)Oh existed in Co(1.2)-IE prepared by ion exchange is more active than Co(2+)Td, Co(3+)Oh and Co-I(2+) obtained by impregnation and hydrothermal methods, respectively. Meanwhile, Co(1.2)-IE shows better stability and stronger resistance against 2.0 vol.% O-2 or 2.3 vol.% H2O in the feed gas. The higher catalytic activity of Co(II)(2+)Oh is attributed to its octahedral coordination geometrical structure, which make Co(II)(2+)Oh tend to donate electrons to activate N2O. Furthermore, the closer spacing distance between two Co(II)(2+)Oh sites can facilitate the combination and desorption of oxygen species. The above mentioned reasons ultimately lead to the increased catalytic activity. Finally, the results of density functional theory calculations indicate that the Co(II)(2+)Oh possesses the highest d-band center, which means the excellent catalytic activity.
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