Low-Cost Synthesis of Titanium Silicalite-1 (TS-1) with Highly Catalytic Oxidation Performance through a Controlled Hydrolysis Process

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• 作者：Xiujuan Deng ; Yuning Wang ; Lu Shen ; Haihong Wu ; Yueming Liu ; Mingyuan He
• 刊名：Industrial & Engineering Chemistry Research
• 出版年：2013
• 出版时间：January 23, 2013
• 年：2013
• 卷：52
• 期：3
• 页码：1190-1196
• 全文大小：361K
• 年卷期：v.52,no.3(January 23, 2013)
• ISSN：1520-5045

文摘

Titanium silicalite-1 (TS-1) has been successfully synthesized in ultralow molar ratio of TPAOH/SiO₂ by two-step and multistep hydrolysis process, where the molar ratio of tetrapropylammonium hydroxide/silica (TPAOH/SiO₂) could be reduced to 0.08 and 0.065, respectively. Combined characterization of X-ray diffraction (XRD), N₂ adsorption鈥揹esorption, scanning electron microcopy (SEM), Fourier transform infrared spectroscopy (FT-IR), UV鈥搗is spectroscopy, and thermal gravimetric (TG) analysis shows that currently synthesized TS-1 samples have the typical 鈥渂lackberry鈥?morphology, and the particle size is around 300鈥?00 nm, similar to that of the conventional TS-1 synthesized at a high molar ratio of TPAOH/SiO₂ (>0.18). Additionally, currently synthesized TS-1 exhibits excellent catalytic oxidation performance in epoxidation of alkene and ammoximation of ketone, even better than that of conventional TS-1. Obviously, fast hydrolysis of a small part of TEOS at a high concentration of TPA⁺ in the first step induces more nuclei, which in turn accelerates crystallization in the subsequent step. Therefore, effective utilization of TPAOH to build the TS-1 framework is significantly increased. This strategy can greatly reduce the synthesis cost of TS-1, which is suitable for synthesis of TS-1 on an industrial scale.