Ce and Ca/Nb doped Pd-mesocellular foam catalysts for gas-phase conversion of acetone to methyl isobutyl ketone

Grzelak, Kalina; Thumbayil, Rouzana Pulikkal; Kegnæs, Søren; Trejda, Maciej; Riisager, Anders

doi:10.1016/j.micromeso.2021.111169

Cited by 4 publications

(15 citation statements)

References 52 publications

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“…Hence, both of the catalysts remained highly selectivity towards MIBK but lost significant activity over time, and only the Cu/Ce‐MCF catalyst remained stable during the long‐term test. A similar loss in activity was not observed for the analogous Pd/Ce‐MCF catalyst, [33] however, the catalytic performance of the Cu/Ce‐MCF catalyst was higher than over Pd/Ce‐MCF despite the initial decrease in activity (Figure S9).…”

Section: Resultssupporting

confidence: 64%

“…The superior performance of the Cu/Ce‐MCF catalyst compared to Cu/Ca−Nb‐MCF was attributed to the presence of basic sites coming from ceria, which were necessary for the condensation of acetone to DAA, the higher Lewis acidity of the Cu 2+ species, which was required for the dehydration of DAA to MO, and the presence of Cu 0 centers, which were active for the hydrogenation of MO to MIBK. Importantly, the Cu/Ce‐MCF catalyst had better catalytic performance and similar durability during continuous operation for 24 h to a recently reported Pd/Ce‐MCF catalyst, [33] implying that Cu can efficiently replace the noble metal Pd as an active catalyst for selective acetone condensation to MIBK.…”

Section: Discussionmentioning

confidence: 58%

“…The textural properties of mesoporous Ca−Nb‐MCF and Ce‐MCF supports, as well as mesoporous aluminophosphate oxynitride (MAPN), aluminophosphate (MAP), and hydroxyapatite (HAP) were determined by nitrogen physisorption in our previous work [33] . After impregnation of the mesoporous supports with copper species, all of the resulting materials Cu/Ca–Nb‐MCF, Cu/Ce‐MCF and Cu/MAPN maintained their mesoporous character with typical nitrogen isotherms of type IVa with H1 hysteresis loops (see the Supporting Information, Figure S1).…”

Section: Resultsmentioning

confidence: 99%

“…Catalyst preparation . Syntheses procedures of the applied catalyst supports MCF, hydroxyapatite (HAP) and mesoporous aluminophosphate oxynitride (MAPN) are described elsewhere [33] . The latter two supports served as reference materials.…”

Section: Methodsmentioning

confidence: 99%

“…Recently, we reported high stability and selectivity, but moderate activity, of Pd/Ce‐MCF (mesocellular foam) catalysts for the gas‐phase reductive condensation of acetone to MIBK [33] . In this work we have extended the study by substituting the noble metal Pd with the cheaper metal Cu in Ce‐MCF catalysts to explore the possible superior catalytic properties with the combination of Cu and ceria.…”

Section: Introductionmentioning

confidence: 99%

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Copper Supported on Ceria Mesocellular Foam Silica as an Effective Catalyst for Reductive Condensation of Acetone to Methyl Isobutyl Ketone

2022

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Copper-containing materials based on Ce-and Ca-Nb-mesocellular foam (MCF) silica supports are prepared, characterized and applied as catalysts for gas-phase reductive condensation of acetone to produce methyl isobutyl ketone (MIBK). The properties of the materials, the interaction of metal species, and their role in the catalytic process are examined by nitrogen physisorption, XRD, XPS, CO 2 -TPD, H 2 -TPR, and chemisorption of NO and pyridine combined with FTIR spectroscopy. A syner-gistic interaction of Cu 2 + , Cu 0 , and CeO 2 species incorporated in the MCF support enable the Cu/Ce-MCF catalyst to yield 34 % of acetone conversion with over 90 % MIBK selectivity at 250 °C. Moreover, this high catalyst selectivity is maintained during operation for 24 h despite a decline in catalyst activity. The catalytic performance is superior to that of hydroxyapatitesupported Cu and similar previously reported Pd-containing catalysts.

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Section: Resultssupporting

confidence: 64%

Section: Discussionmentioning

confidence: 58%

Section: Resultsmentioning

confidence: 99%

Section: Methodsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Copper Supported on Ceria Mesocellular Foam Silica as an Effective Catalyst for Reductive Condensation of Acetone to Methyl Isobutyl Ketone

2022

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Atomic cerium modulated palladium nanoclusters exsolved ferrite catalysts for lean methane conversion

Yang

Wang

et al. 2022

Exploration

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The active and stable palladium (Pd) based catalysts for CH4 conversion are of great environmental and industrial significance. Herein, we employed N2 as an optimal activation agent to develop a Pd nanocluster exsolved Ce‐incorporated perovskite ferrite catalyst toward lean methane oxidation. Replacing the traditional initiator of H2, the N2 was found as an effective driving force to selectively touch off the surface exsolution of Pd nanocluster from perovskite framework without deteriorating the overall material robustness. The catalyst showed an outstanding T50 (temperature of 50% conversion) plummeting down to 350°C, outperforming the pristine and H2‐activated counterparts. Further, the combined theoretical and experimental results also deciphered the crucial role that the atomically dispersed Ce ions played in both construction of active sites and CH4 conversion. The isolated Ce located at the A‐site of perovskite framework facilitated the thermodynamic and kinetics of the Pd exsolution process, lowering its formation temperature and promoting its quantity. Moreover, the incorporation of Ce lowered the energy barrier for cleavage of C─H bond, and was dedicated to the preservation of highly reactive PdOx moieties during stability measurement. This work successfully ventures uncharted territory of in situ exsolution to provide a new design thinking for a highly performed catalytic interface.

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Gas-phase organometallic catalysis in MFM-300(Sc) provided by switchable dynamic metal sites

et al. 2023

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Ce and Ca/Nb doped Pd-mesocellular foam catalysts for gas-phase conversion of acetone to methyl isobutyl ketone

Cited by 4 publications

References 52 publications

Copper Supported on Ceria Mesocellular Foam Silica as an Effective Catalyst for Reductive Condensation of Acetone to Methyl Isobutyl Ketone

Copper Supported on Ceria Mesocellular Foam Silica as an Effective Catalyst for Reductive Condensation of Acetone to Methyl Isobutyl Ketone

Atomic cerium modulated palladium nanoclusters exsolved ferrite catalysts for lean methane conversion

Gas-phase organometallic catalysis in MFM-300(Sc) provided by switchable dynamic metal sites

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