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

doi:10.1007/s11705-014-1409-y

Front. Chem. Sci. Eng.

2014, Vol. 8

Issue (2) : 149-155 https://doi.org/10.1007/s11705-014-1409-y

RESEARCH ARTICLE

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

Pengxu YAO,Yaquan WANG(

),Teng ZHANG,Shuhai WANG,Xiaoxue WU

Key Laboratory for Green Chemical Technology of the Ministry of Education, School of Chemical Engineering & Technology, Tianjin University, Tianjin 300072, China

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Abstract

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.

Keywords extra framework Ti cyclohexanone ammoximation titanium silicalite-1 sodium ion crystal size

Corresponding Author(s): Yaquan WANG

Issue Date: 22 May 2014

Cite this article:

Pengxu YAO,Yaquan WANG,Teng ZHANG, et al. Effect of sodium ions in synthesis of titanium silicalite-1 on its catalytic performance for cyclohexanone ammoximation[J]. Front. Chem. Sci. Eng., 2014, 8(2): 149-155.

URL:

https://academic.hep.com.cn/fcse/EN/10.1007/s11705-014-1409-y
https://academic.hep.com.cn/fcse/EN/Y2014/V8/I2/149

Fig.1 XRD patterns of TS-1-x synthesized in the presence of various concentrations of Na⁺

Tab.1 Properties of TS-1-x synthesized in the presence of various concentrations of Na⁺

Fig.2 SEM images of TS-1-x synthesized in the presence of various concentrations of Na⁺

Fig.3 FT-IR spectra of TS-1 samples synthesized in the presence of various concentrations of Na⁺

Fig.4 UV-Vis spectra of TS-1 samples synthesized in the presence of various concentrations of Na⁺

Fig.5 Catalytic performances of TS-1-x in the ammoximation of cyclohexanone

Reaction conditions: 0.5 g catalyst; 349 K, 0.1 MPa, WHSV= 12.2 h^–1, 7.0 wt-% H₂O₂, 18 wt-% cyclohexanone in t-butanol

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