TiO2 nanofiber-supported copper nanoparticle catalysts for highly efficient methane conversion to C1 oxygenates under mild conditions
The selective oxidation of methane under mild conditions remains the “Holy Grail of Catalysis”. The key to activating methane and inhibiting over-oxidation of target oxygenates lies in designing active centers. Copper nanoparticles were loaded onto TiO 2 nanofibers using the photo-deposition method....
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Veröffentlicht in: | Nano research 2024-05, Vol.17 (5), p.3844-3852 |
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Hauptverfasser: | , , , , , , , , , , , |
Format: | Artikel |
Sprache: | eng |
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Zusammenfassung: | The selective oxidation of methane under mild conditions remains the “Holy Grail of Catalysis”. The key to activating methane and inhibiting over-oxidation of target oxygenates lies in designing active centers. Copper nanoparticles were loaded onto TiO
2
nanofibers using the photo-deposition method. The resulting catalysts were found to effectively convert methane into C1 oxygenated products under mild conditions. Compared with previously reported catalysts, it delivers a superior performance of up to 2510.7 mmol·g
Cu
−1
·hr
−1
productivity with a selectivity of around 100% at 80 °C for 5 min. Microstructure characterizations and density functional theory (DFT) calculations indicate that TiO
2
in the mixed phase of anatase and rutile significantly increases the Cu
+
/Cu
0
ratio of the supported Cu species, and this ratio is linearly related to the formation rate of oxygen-containing species. The Cu
1
site promotes the generation of active O species from H
2
O
2
dissociation on Cu
2
O (111). These active O species reduce the energy barrier for breaking the C–H bond of CH
4
, thus boosting the catalytic activity. The methane conversion mechanism was proposed as a methyl radical pathway to form CH
3
OH and CH
3
OOH, and then the generated CH
3
OH is further oxidized to HOCH
2
OOH. |
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ISSN: | 1998-0124 1998-0000 |
DOI: | 10.1007/s12274-023-6356-9 |