TY - JOUR
T1 - Low-cost synthesis of titanium silicalite-1 (TS-1) with highly catalytic oxidation performance through a controlled hydrolysis process
AU - Deng, Xiujuan
AU - Wang, Yuning
AU - Shen, Lu
AU - Wu, Haihong
AU - Liu, Yueming
AU - He, Mingyuan
PY - 2013/1/23
Y1 - 2013/1/23
N2 - 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-desorption, scanning electron microcopy (SEM), Fourier transform infrared spectroscopy (FT-IR), UV-vis spectroscopy, and thermal gravimetric (TG) analysis shows that currently synthesized TS-1 samples have the typical "blackberry" morphology, and the particle size is around 300-400 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.
AB - 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-desorption, scanning electron microcopy (SEM), Fourier transform infrared spectroscopy (FT-IR), UV-vis spectroscopy, and thermal gravimetric (TG) analysis shows that currently synthesized TS-1 samples have the typical "blackberry" morphology, and the particle size is around 300-400 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.
UR - https://www.scopus.com/pages/publications/84872956924
U2 - 10.1021/ie302467t
DO - 10.1021/ie302467t
M3 - 文章
AN - SCOPUS:84872956924
SN - 0888-5885
VL - 52
SP - 1190
EP - 1196
JO - Industrial and Engineering Chemistry Research
JF - Industrial and Engineering Chemistry Research
IS - 3
ER -