Difference of Oxidation Mechanism between Light C3–C4
Alkane and Alkene over Mullite YMn2O5 Oxides’
Catalyst
Posted on 2020-06-19 - 12:36
Revealing
the catalytic oxidation mechanism of volatile organic
compounds (VOCs) is insightful for the development of efficient catalysts.
However, because of the complicated interactions and a large number
of intermediate species during the reactions, the analysis of the
entire reaction mechanism (including the activation modes of reactant
molecules and the rate-limiting step) remains a great challenge. Herein,
the YMn2O5 mullite catalyst was proposed to
demonstrate how to distinguish the deep oxidation difference among
C3–C4 alkanes and olefins via combining experiments and theoretical
calculations. The YMn2O5 catalyst prepared via
the hydrothermal method displayed a superior catalytic behavior with
a low T90 temperature (C3H8 at 250
°C; C3H6, C4H10,
and C4H8 less than 200 °C) (1000 ppm of
C3–C4 and 10% O2 balanced with He, WHSV = 30 000
mL/g·h). The catalytic activity remained the same after continuous
reaction for 100 h at 275 °C for each reactant. Overall, the
YMn2O5 mullite catalyst exhibits excellent durability
with no activity declines for 400 h. Combined with TPD, DRIFTS, XPS,
and DFT analysis, surface oxygen species were found to be active for
the oxidation. Owing to the difference of the HOMO induced partial
charge distributions between alkanes and alkenes, the dehydrogenation
of the end-site C–H of propane is the first step prior to the
crucial conversion of acrylate over surface labile oxygen in an octahedral
ligand unit. For propene oxidation, the CC double bond is
preferentially attacked by two surface oxygen atoms belonging to the
octahedral and pyramid ligand units with the crucial step of acetate
decomposition. These findings provide insights into the oxide catalyst
design toward the complicated VOCs oxidation from a fundamental point
of view.
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Zhang, Tong; Lang, Xiuyao; Dong, Anqi; Wan, Xiang; Gao, Shan; Wang, Li; et al. (2020). Difference of Oxidation Mechanism between Light C3–C4
Alkane and Alkene over Mullite YMn2O5 Oxides’
Catalyst. ACS Publications. Collection. https://doi.org/10.1021/acscatal.0c00703
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AUTHORS (8)
TZ
Tong Zhang
XL
Xiuyao Lang
AD
Anqi Dong
XW
Xiang Wan
SG
Shan Gao
LW
Li Wang
LW
Linxia Wang
WW
Weichao Wang
KEYWORDS
propene oxidationoctahedral ligand unitoxide catalyst designVOCs oxidationTPDXPS400 hC 4 H 10surface oxygen atomsoxidation differencealkaneactivation modesOxidation Mechanismactivity declinesreaction mechanismC 4 H 8HOMOoxidation mechanismrate-limiting stepC 3 H 6C 3 H 830 000hydrothermal methodreactant moleculesT 90 temperatureDRIFTSYMn 2 O 5 mullite catalystcharge distributionsDFT analysisYMn 2 O 5 catalystacetate decompositionsurface oxygen speciespyramid ligand unitsYMn 2 O 5 mullite catalyst exhibits100 hWHSV