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Effect of oxygen vacancy and highly dispersed MnO_x on soot combustion in cerium manganese catalyst.

ABSTRACT: Cerium manganese bimetallic catalysts have become the focus of current research because of their excellent catalytic performance for soot combustion. Two series of cerium manganese catalysts (Na-free catalysts and Na-containing catalysts) were prepared by coprecipitation method and characterized using XRD, N₂ adsorption-desorption, SEM, Raman, XPS, H₂-TPR, O₂-TPD, Soot-TPR-MS and in situ IR. The effects of abundant oxygen vacancies and surface highly dispersed MnO_x on soot catalytic combustion of cerium manganese catalysts prepared by different precipitants were analyzed. The activity test results show that the active oxygen species released by a large number of oxygen vacancies in the cerium manganese catalyst are more favorable to the soot catalytic combustion than MnO_x which is highly dispersed on the surface of the catalyst and has good redox performance at low temperature. Because the catalytic effect of MnO_x on the surface of Na-free catalysts is more dependent on the contact condition between the catalyst and the soot, this phenomenon can be observed more easily under the loose contact condition than under the tight contact condition. The activity cycle test results show that these two series of catalysts show good stability and repeated use will hardly cause any deactivation of the catalysts.

SUBMITTER: Zhu Y

PROVIDER: S-EPMC9975190 | biostudies-literature | 2023 Feb

REPOSITORIES: biostudies-literature

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Effect of oxygen vacancy and highly dispersed MnOx on soot combustion in cerium manganese catalyst.

Zhu Yi Y Chen Zhen Z Li Hongmei H Wang Quan Q Liu Xingyu X Hu You Y Su Cuimei C Duan Rui R Chen Shanhu S Lan Li L

Scientific reports 20230228 1

Cerium manganese bimetallic catalysts have become the focus of current research because of their excellent catalytic performance for soot combustion. Two series of cerium manganese catalysts (Na-free catalysts and Na-containing catalysts) were prepared by coprecipitation method and characterized using XRD, N2 adsorption-desorption, SEM, Raman, XPS, H2-TPR, O2-TPD, Soot-TPR-MS and in situ IR. The effects of abundant oxygen vacancies and surface highly dispersed Mn ...[more]

PMID: 36854804

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Project description:Soot combustion experiments with 5%O2/He were conducted using model soot, and four distinct compositions of CexPr1-xO2-δ oxides of varying nominal cerium compositions (x = 0, 0.2, 0.3, and 1) were prepared. The catalyst samples were comprehensively characterized using techniques such as XRD, Raman spectroscopy, HR-TEM, N2 adsorption at -196 °C, XPS, O2-TPD, H2-TPR, and work function measurements. The Pr-rich compositions, ranging from Ce0.3Pr0.7O2-δ to PrO2-δ, resulted in a significant increase in the total evolved O2 amounts and enhanced catalyst reducibility. However, a decrease in the textural properties of the catalysts was noted, which was particularly important for the pure praseodymia under the synthesis route conducted. The catalytic activity was investigated under the two following contact modes of mixing between soot and catalyst: loose and tight. The results revealed that the catalytic performance is associated with the surface contact in tight contact mode and with the combination of surface/subsurface/bulk oxygen mobility and the BET surface area in loose contact mode. Notably, the temperatures estimated at 10% and 50% of the conversion (T10 and T50) parameters were achieved at much lower temperatures than the uncatalyzed soot combustion, even under loose contact conditions. Specifically, the 50% conversion was achieved at 511 °C and 538 °C for Ce0.3Pr0.7O2 and Ce0.2Pr0.8O2, respectively. While no direct correlation between catalytic activity and work function was observed, a significant relationship emerges between work function values and the formation of oxygen vacancies, whatever the conditions used for these measurements. On the other hand, the ability to generate a high population of oxygen vacancies at low temperatures, rather than the direct activation of gas-phase O2, influences the catalytic performance of Pr-doped ceria catalysts, highlighting the importance of surface/subsurface oxygen vacancy generation, which was the parameter that showed a better correlation with the catalytic activity, whatever the soot conversion value or the mode of contact considered.

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Effect of oxygen vacancy and highly dispersed MnO_x on soot combustion in cerium manganese catalyst.

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Effect of oxygen vacancy and highly dispersed MnO<sub>x</sub> on soot combustion in cerium manganese catalyst.

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