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Influence of Na

Rumin YANG, Fanhui MENG, Xiao WANG, Yaquan WANG

《化学科学与工程前沿（英文）》 2011年第5卷第4期页码 401-408 doi: 10.1007/s11705-011-1129-5

摘要： Silicalite-1 was hydrothermally synthesized in the presence of different concentrations of Na using tetrapropylammonium hydroxide (TPAOH) as a template. The synthesis was followed by a base treatment. The silicalite-1samples were characterized using X-ray diffraction, scanning electron microscopy, N adsorption, X-ray photoelectron spectroscopy, Fourier transform infrared spectroscopy and NH temperature-programmed desorption. The samples were used as catalysts for the vapor phase Beckmann rearrangement of cyclohexanone oxime. During the synthesis, the sodium ions were incorporated onto the silicalite-1 crystals, but were then removed by the base treatment. All the catalysts exhibited nearly complete conversion of cyclohexanone oxime to ?-caprolactam with selectivities grater than 95%. Addition of less than 2.5 mol-% Na (relative to TPAOH) did not influence the catalytic properties. However, for Na concentrations≥5 mol-%, the particle sizes of silicalite-1 increased and the catalytic activities decreased, which can be attributed to carbon deposition. The results in this work are of great importance for the polymer industry.

关键词： silicalite-1 cyclohexanone oxime vapor phase Beckmann rearrangement ?-caprolactam

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Effect of sodium ions in synthesis of titanium silicalite-1 on its catalytic performance for cyclohexanone

Pengxu YAO,Yaquan WANG,Teng ZHANG,Shuhai WANG,Xiaoxue WU

《化学科学与工程前沿（英文）》 2014年第8卷第2期页码 149-155 doi: 10.1007/s11705-014-1409-y

摘要： Titanium silicalite-1 (TS-1) has been hydrothermally synthesized with tetrapropylammonium hydroxide (TPAOH) as the template in the presence of various amounts of Na , characterized by inductively coupled plasma, X-ray diffraction, scanning electron microscope, X-ray photoelectron spectroscopy, Fourier transform infrared spectroscopy and ultro-violet-visible spectroscopy and studied in cyclohexanone ammoximation. The characterization results show that with the increase of Na concentration in the synthesis, both the crystal sizes of TS-1and extra framework Ti increase but framework Ti decreases. The addition of Na below 3 mol-% of TPAOH in the synthesis does not influence the catalytic properties with above 98% conversion of cyclohexanone and 99.5% selectivity to cyclohexanone oxime. However, at the concentrations of Na ≥3 mol-% of TPAOH in the synthesis, the catalysts are deactivated faster with the increase of Na addition, which can be attributed to more high molecular weight byproducts deposited in the large TS-1 particles and the loss of the frame-work titanium. The results of this work are of great importance for the industry.

关键词： extra framework Ti cyclohexanone ammoximation titanium silicalite-1 sodium ion crystal size

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Ultrasound-assisted co-precipitation synthesis of mesoporous Co3O4–CeO2 composite oxides for highly selective catalytic oxidation of cyclohexane

《化学科学与工程前沿（英文）》 2022年第16卷第8期页码 1211-1223 doi: 10.1007/s11705-022-2145-3

摘要： The one-step highly selective oxidation of cyclohexane into cyclohexanone and cyclohexanol as the essential intermediates of nylon-6 and nylon-66 is considerably challenging. Therefore, an efficient and low-cost catalyst must be urgently developed to improve the efficiency of this process. In this study, a Co₃O₄–CeO₂ composite oxide catalyst was successfully prepared through ultrasound-assisted co-precipitation. This catalyst exhibited a higher selectivity to KA-oil, which was benefited from the synergistic effects between Co³⁺/Co²⁺ and Ce⁴⁺/Ce³⁺ redox pairs, than bulk CeO₂ and/or Co₃O₄. Under the optimum reaction conditions, 89.6% selectivity to KA-oil with a cyclohexane conversion of 5.8% was achieved over Co₃O₄–CeO₂. Its catalytic performance remained unchanged after five runs. Using the synergistic effects between the redox pairs of different transition metals, this study provides a feasible strategy to design high-performance catalysts for the selective oxidation of alkanes.

关键词： Co₃O₄–CeO₂ composite oxides cyclohexanone cyclohexanol ultrasonic-assisted co-precipitation selective oxidation solvent-free