Efficient selective oxidation of propylene by dioxygen on mesoporous-silica-nanoparticle-supported nanosized copper

Lai, Nien-Chu; Tsai, Ming‐Hsiu; Liu, Chun-Hsia; Chen, Ching-Shiun; Yang, C. S.

doi:10.1016/j.jcat.2018.07.014

Cited by 20 publications

(4 citation statements)

References 56 publications

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“…These observations demonstrate that cobalt-catalyzed propylene aerobic epoxidation is a site-specific reaction. The Arrhenius plots of propylene epoxidation give an apparent activation energy of 64 kJ/mol for PO formation over Co@Y (Figure S16), which is a relatively low value in aerobic epoxidation. − To our knowledge, Co@Y is the first example of an industrial-relevant catalyst for propylene epoxidation with O 2 , showing high propylene conversion at reasonable PO selectivity. The direct comparison of various epoxidation catalysts is summarized in Figure c and Table S2.…”

Section: Resultsmentioning

confidence: 99%

Direct Propylene Epoxidation with Molecular Oxygen over Cobalt-Containing Zeolites

et al. 2022

J. Am. Chem. Soc.

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Direct propylene epoxidation with molecular oxygen is a dream reaction with 100% atom economy, but aerobic epoxidation is challenging because of the undesired over-oxidation and isomerization of epoxide products. Herein, we report the construction of uniform cobalt ions confined in faujasite zeolite, namely, Co@Y, which exhibits unprecedented catalytic performance in the aerobic epoxidation of propylene. Propylene conversion of 24.6% is achieved at propylene oxide selectivity of 57% at 773 K, giving a state-of-the-art propylene oxide production rate of 4.7 mmol/gcat/h. The catalytic performance of Co@Y is very stable, and no activity loss can be observed for over 200 h. Spectroscopic analyses reveal the details of molecular oxygen activation on isolated cobalt ions, followed by interaction with propylene to produce epoxide, in which the Co2+–Coδ+–Co2+ (2 < δ < 3) redox cycle is involved. The reaction pathway of propylene oxide and byproduct acrolein formation from propylene epoxidation is investigated by density functional theory calculations, and the unique catalytic performance of Co@Y is interpreted. This work presents an explicit example of constructing specific transition-metal ions within the zeolite matrix toward selective catalytic oxidations.

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Section: Resultsmentioning

confidence: 99%

Direct Propylene Epoxidation with Molecular Oxygen over Cobalt-Containing Zeolites

et al. 2022

J. Am. Chem. Soc.

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“…To estimate the surface area, particle size, and dispersion of metallic copper properties, a hydrogen TPR reaction combined with nitrous oxide oxidation was performed in a U-shaped quartz reactor at atmospheric pressure (Gervasini and Bennici, 2005;Lai et al, 2018). Fresh CuTMS (200 mg) was loaded on 40 mesh silica bed with a steam rate of 60 ml/min (5% H 2 balance with Ar) and heated at 10 • C/min to reach the first H 2 -TPR result.…”

Section: Hydrogen Temperature-programmed Reduction (H 2 -Tpr)mentioning

confidence: 99%

High-performance and long-term stability of mesoporous Cu-doped TiO2 microsphere for catalytic CO oxidation

Yang

Lin

Montini

et al. 2021

Journal of Hazardous Materials

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“…In addition, the copper nanoparticles can be stabilized using zeolites. The latter facilitates the adsorption of the reagents, thus improving the catalytic activity [50]. Titanium oxide is less thermally stable; however, it provides the chemical stability of the copper catalysts towards poisoning [51][52][53].…”

Section: Introductionmentioning

confidence: 99%

Sol-Gel Synthesis and Characterization of the Cu-Mg-O System for Chemical Looping Application

et al. 2022

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A sol-gel technique was applied to prepare the two-component oxide system Cu-Mg-O, where MgO plays the role of oxide matrix, and CuO is an active chemical looping component. The prepared samples were characterized by scanning electron microscopy, low-temperature nitrogen adsorption, and X-ray diffraction analysis. The reduction behavior of the Cu-Mg-O system was examined in nine consecutive reduction/oxidation cycles. The presence of the MgO matrix was shown to affect the ability of CuO towards reduction and re-oxidation significantly. During the first reduction/oxidation cycle, the main characteristics of the oxide system (particle size, crystallization degree, etc.) undergo noticeable changes. Starting from the third cycle, the system exhibits a stable operation, providing the uptake of similar hydrogen amounts within the same temperature range. Based on the obtained results, the two-component Cu-Mg-O system can be considered as a prospective chemical looping agent.

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Efficient selective oxidation of propylene by dioxygen on mesoporous-silica-nanoparticle-supported nanosized copper

Cited by 20 publications

References 56 publications

Direct Propylene Epoxidation with Molecular Oxygen over Cobalt-Containing Zeolites

Direct Propylene Epoxidation with Molecular Oxygen over Cobalt-Containing Zeolites

High-performance and long-term stability of mesoporous Cu-doped TiO2 microsphere for catalytic CO oxidation

Sol-Gel Synthesis and Characterization of the Cu-Mg-O System for Chemical Looping Application

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