Catalysts for selective propane oxidation in the presence of carbon monoxide: Mechanistic aspects

Swislocki, Simon; Stöwe, Klaus; Maier, Wilhelm F.

doi:10.1016/j.jcat.2014.05.008

Cited by 28 publications

(15 citation statements)

References 67 publications

(97 reference statements)

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“…Detailed peak assignments are shown in Table S1. In particular, the peaks at 1340, 1380, 1455, and 1470 cm –1 correspond to polydentate CO 3 2– , δ s (CH 3 ), v s (COO – ), and δ as (CH 3 ), respectively. − This suggests that propane reacts with the oxygen of the LaMnO 3 sample to a certain degree. The same phenomenon is observed in the spectra (in Figure b,c) of LaCo 0.2 Mn 0.8 O 3 and LaCoO 3 samples, indicating that the same adsorption behavior occurs on the LaCo x Mn 1– x O 3 catalysts.…”

Section: Resultsmentioning

confidence: 96%

Insight into the Effect of Cobalt Substitution on the Catalytic Performance of LaMnO₃ Perovskites for Total Oxidation of Propane

et al. 2020

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Cobalt-substituted LaMnO 3 perovskite catalysts synthesized by the citric acid sol−gel method have been investigated for the total oxidation of propane, as a model for emission control of hydrocarbon volatile organic compounds. Characterization studies demonstrate that a trace of cobalt substitution can enhance the specific surface area, produce abundant reactive oxygen species, and improve low-temperature reducibility, which promote the catalytic activities of La-Co x Mn 1−x O 3 catalysts remarkably. LaCo 0.2 Mn 0.8 O 3 exhibits the highest catalytic activity (T 90 = 355 °C), of which T 90 is 25 °C lower than that of LaMnO 3 . In situ DRIFTS and C 3 H 8 -TPSR results indicate that the adsorption and activation of propane will be accelerated by appropriate Co substitution and acetone and carboxylate species are considered as intermediates involved in propane oxidation. In addition, the influence of water vapor on the catalytic activity of the LaCo 0.2 Mn 0.8 O 3 catalyst for propane oxidation is greater than that of CO 2 , while LaCo 0.2 Mn 0.8 O 3 can sustain robust stability under CO 2 and water vapor atmospheres.

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Section: Resultsmentioning

confidence: 96%

Insight into the Effect of Cobalt Substitution on the Catalytic Performance of LaMnO₃ Perovskites for Total Oxidation of Propane

et al. 2020

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“…In addition, multiple bands between 1300 and 1900 cm –1 appeared. The bands at 1855, 1589, and 1457 cm –1 can be attributed to ν(C = O), ν as (COO), and ν s (COO) modes, respectively, − and both the bands at 1373 and 1392 cm –1 were assigned to δ s (CH 3 ). ,, Since the latter two bands had the same shape and intensity, isopropyl groups were concluded to form on the Ru/Al 2 O 3 - X catalysts after exposure to the feed gas. In addition, the intensity of the band observed at 1855 cm –1 for the Ru/Al 2 O 3 - X catalysts clearly increased with increasing Ru loading, as shown in Figure S10.…”

Section: Resultsmentioning

confidence: 97%

“…As shown in Figure C, when the CeO 2 support was exposed to pure propane for 30 min, in addition to the absorption band at 2967 cm –1 assigned to the absorption of gaseous propane, , an absorption band attributed to ν as (COO) was observed at 1546 cm –1 , indicating that propane reacted with the oxygen of the CeO 2 support to a certain degree. − When the feed gas was replaced with 0.5 vol % C 3 H 8 –5 vol % O 2 –94.5 vol % Ar, multiple bands appeared at 2933, 2842, 1506, 1466, 1428, 1371, 1355, and 1296 cm –1 . The bands at 2933 and 2842 cm –1 were assigned to ν(CH 2 ), ,,, and those at 1506, 1466, 1428, 1371, 1355, and 1296 cm –1 were attributed to ν as (COO), δ as (CH 3 ), ν s (COO), δ s (CH 3 ), δ s (CH 3 ), and ν(C–O), − respectively. Therefore, these results revealed that unlike in the case of the Al 2 O 3 support, propane could be partially oxidized and adsorb to the surface of the CeO 2 support.…”

Section: Resultsmentioning

confidence: 98%

Total Oxidation of Propane over a Ru/CeO₂ Catalyst at Low Temperature

Zong

Wang

Guo

et al. 2018

Environ. Sci. Technol.

200

153

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Ruthenium (Ru) nanoparticles (∼3 nm) with mass loading ranging from 1.5 to 3.2 wt % are supported on a reducible substrate, cerium dioxide (CeO, the resultant sample is called Ru/CeO), for application in the catalytic combustion of propane. Because of the unique electronic configuration of CeO, a strong metal-support interaction is generated between the Ru nanoparticles and CeO to stabilize Ru nanoparticles for oxidation reactions well. In addition, the CeO host with high oxygen storage capacity can provide an abundance of active oxygen for redox reactions and thus greatly increases the rates of oxidation reactions or even modifies the redox steps. As a result of such advantages, a remarkably high performance in the total oxidation of propane at low temperature is achieved on Ru/CeO. This work exemplifies a promising strategy for developing robust supported catalysts for short-chain volatile organic compound removal.

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“…The strong bands at 1700–1200 cm –1 were associated with carboxylate species due to the oxidation of the organic molecule. Briefly, the bands at 1631 cm –1 , 1304 and 1378 cm –1 were attributed to v (CC), v (C–O), and v (C–H) groups, , respectively. Obviously, the CC double bond appears rapidly and strongly, which indicates that propane adsorbed on the catalyst is easy to dehydrogenate to form CC double bond.…”

Section: Resultsmentioning

confidence: 99%

Difference of Oxidation Mechanism between Light C3–C4 Alkane and Alkene over Mullite YMn₂O₅ Oxides’ Catalyst

et al. 2020

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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 CC 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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Catalysts for selective propane oxidation in the presence of carbon monoxide: Mechanistic aspects

Cited by 28 publications

References 67 publications

Insight into the Effect of Cobalt Substitution on the Catalytic Performance of LaMnO₃ Perovskites for Total Oxidation of Propane

Insight into the Effect of Cobalt Substitution on the Catalytic Performance of LaMnO₃ Perovskites for Total Oxidation of Propane

Total Oxidation of Propane over a Ru/CeO₂ Catalyst at Low Temperature

Difference of Oxidation Mechanism between Light C3–C4 Alkane and Alkene over Mullite YMn₂O₅ Oxides’ Catalyst

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Catalysts for selective propane oxidation in the presence of carbon monoxide: Mechanistic aspects

Cited by 28 publications

References 67 publications

Insight into the Effect of Cobalt Substitution on the Catalytic Performance of LaMnO3 Perovskites for Total Oxidation of Propane

Insight into the Effect of Cobalt Substitution on the Catalytic Performance of LaMnO3 Perovskites for Total Oxidation of Propane

Total Oxidation of Propane over a Ru/CeO2 Catalyst at Low Temperature

Difference of Oxidation Mechanism between Light C3–C4 Alkane and Alkene over Mullite YMn2O5 Oxides’ Catalyst

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Product

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Insight into the Effect of Cobalt Substitution on the Catalytic Performance of LaMnO₃ Perovskites for Total Oxidation of Propane

Insight into the Effect of Cobalt Substitution on the Catalytic Performance of LaMnO₃ Perovskites for Total Oxidation of Propane

Total Oxidation of Propane over a Ru/CeO₂ Catalyst at Low Temperature

Difference of Oxidation Mechanism between Light C3–C4 Alkane and Alkene over Mullite YMn₂O₅ Oxides’ Catalyst