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Self-sustained combustion of CO with transient changes and reaction mechanism over CuCe0.75Zr0.25Oδ powder for honeycomb ceramic catalyst.
- Source :
-
Fuel . Mar2020, Vol. 263, pN.PAG-N.PAG. 1p. - Publication Year :
- 2020
-
Abstract
- • The powder sample is well designed and coated on the HC tube to form CuCe 0.75 Zr 0.25 O δ /HC catalyst. • The transient changes and two-dimensional temperature region are obtained for CO self-combustion via CO-TPO + FLIR. • The various intermediate species and competitive adsorption of reactants on different active sites are evidenced. • The different pathways and roles of M-K and L-H mechanisms are proposed using in situ IR. A CuCe 0.75 Zr 0.25 O δ catalyst was prepared by the sol-gel method and successfully coated on honeycomb ceramic (HC) carrier. The activity of CuCe 0.75 Zr 0.25 O δ /HC was determined by the CO-TPO + FLIR, with the results performing that the critical condition for CO self-sustained combustion is 3 vol% CO + 3 vol% O 2 /N 2 at 0.5 L/min. As the CO concentration increases from 1 vol% CO to 3 vol% CO, the induction process (<T 15) shifts toward a slower CO conversion, while the light-off process (>T 15) shifts to rapid ignition with a transient change for the CO oxidation reaction. The furnace temperature for CO self-sustained combustion decreases with increasing the CO and O 2 concentrations. Upon increasing the CO 2 concentration, however, furnace temperature is needed to increase and realize CO complete conversion. The thermal stability test combined with SEM + EDX results indicate that the CuCe 0.75 Zr 0.25 O δ /HC retains an excellent thermal stability after a 200 h, and the high-temperature region remains at 225 ± 1 °C during the CO self-combustion reaction. The activity of catalyst is reduced slightly after the 200 h test because of the carbon deposition on the catalyst surface, but such a slight deactivation can be eliminated by the air oxidation method. In situ IR results show a competitive adsorption of CO/O 2 and CO 2 on the Cu-Ce active sites, indicating that the addition of gaseous CO 2 performs an inhibition of CO oxidation. CO preferentially adsorbs linearly at Cu+ sites to form carbonyls that react with lattice oxygen to produce CO 2 to release, which can be ascribed to M-K mechanism. The L-H mechanism is less important, which involves the relatively weak reaction of adsorbed CO and adsorbed oxygen on the Cu-Ce active sites to form carbonate species. [ABSTRACT FROM AUTHOR]
Details
- Language :
- English
- ISSN :
- 00162361
- Volume :
- 263
- Database :
- Academic Search Index
- Journal :
- Fuel
- Publication Type :
- Academic Journal
- Accession number :
- 140467026
- Full Text :
- https://doi.org/10.1016/j.fuel.2019.116637