Synergistic effects of Cu species and acidity of Cu-ZSM-5 on catalytic performance for selective catalytic oxidation of n-butylamine

AbstractActivation of O2 is a critical step in heterogeneous catalytic oxidation. Here, the concept of increased electron donors induced by nitrogen vacancy is adopted to propose an efficient strategy to develop highly active and stable catalysts for molecular O2 activation. Carbon nitride with nitrogen vacancies is prepared to serve as a support as well as electron sink to construct a synergistic catalyst with Pt nanoparticles. Extensive characterizations combined with the first-principles calculations reveal that nitrogen vacancies with excess electrons could effectively stabilize metallic Pt nanoparticles by strong p-d coupling. The Pt atoms and the dangling carbon atoms surround the vacancy can synergistically donate electrons to the antibonding orbital of the adsorbed O2. This synergistic catalyst shows great enhancement of catalytic performance and durability in toluene oxidation. The introduction of electron-rich non-oxide substrate is an innovative strategy to develop active Pt-based oxidation catalysts, which could be conceivably extended to a variety of metal-based catalysts for catalytic oxidation.

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Selective Catalytic Oxidation of Toluene to Benzaldehyde: Effect of Aging Time and Calcination Temperature Using CuxZnyO Mixed Metal Oxide Nanoparticles

Catalysts ◽

10.3390/catal11030354 ◽

2021 ◽

Vol 11 (3) ◽

pp. 354

Author(s):

Khadijah H. Alharbi ◽

Ali Alsalme ◽

Ahmed Bader A. Aloumi ◽

Mohammed Rafiq H. Siddiqui

Keyword(s):

Metal Oxide ◽

Calcination Temperature ◽

Aging Time ◽

Metal Oxide Nanoparticles ◽

Catalytic Performance ◽

Molar Ratio ◽

Mixed Metal Oxide ◽

Toluene Oxidation ◽

Mixed Metal ◽

Selective Catalytic Oxidation

Oxidation is an important organic transformation, and several catalysts have been reported for this conversion. In this study, we report the synthesis of mixed metal oxide CuxZnyO, which is prepared by a coprecipitation method by varying the molar ratio of Cu and Zn in the catalytic system. The prepared mixed metal oxide CuxZnyO was evaluated for catalytic performance for toluene oxidation. Various parameters of the catalytic evaluation were studied in order to ascertain the optimum condition for the best catalytic performance. The results indicate that aging time, calcination temperature, reaction temperature, and feed rate influence catalytic performance. It was found that the catalyst interfaces apparently enhanced catalytic activity for toluene oxidation. The XRD diffractograms reveal the crystalline nature of the mixed metal oxide formed and also confirm the coexistence of hexagonal and monoclinic crystalline phases. The catalyst prepared by aging for 4 h and calcined at 450 °C was found to be the best for the conversion of toluene to benzaldehyde while the reactor temperature was maintained at 250 °C with toluene fed into the reactor at 0.01 mL/min. The catalyst was active for about 13 h.

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