Effect of hydrolysis of tetraethyl orthosilicate (TEOS) on titanium distribution of TS-1 zeolite

GENG An-ying; DING Guo-qiang; SHE Hao-hao; WANG Hong-xing; LI Xian-qing; ZHU Yu-lei

doi:10.1016/S1872-5813(22)60022-7

Volume 50 Issue 11

Nov. 2022

Turn off MathJax

Article Contents

Article Navigation > Journal of Fuel Chemistry and Technology > 2022 > 50(11): 1471-1479

GENG An-ying, DING Guo-qiang, SHE Hao-hao, WANG Hong-xing, LI Xian-qing, ZHU Yu-lei. Effect of hydrolysis of tetraethyl orthosilicate (TEOS) on titanium distribution of TS-1 zeolite[J]. Journal of Fuel Chemistry and Technology, 2022, 50(11): 1471-1479. doi: 10.1016/S1872-5813(22)60022-7

Citation:

GENG An-ying, DING Guo-qiang, SHE Hao-hao, WANG Hong-xing, LI Xian-qing, ZHU Yu-lei. Effect of hydrolysis of tetraethyl orthosilicate (TEOS) on titanium distribution of TS-1 zeolite[J]. Journal of Fuel Chemistry and Technology, 2022, 50(11): 1471-1479. doi: 10.1016/S1872-5813(22)60022-7

Citation:

GENG An-ying, DING Guo-qiang, SHE Hao-hao, WANG Hong-xing, LI Xian-qing, ZHU Yu-lei. Effect of hydrolysis of tetraethyl orthosilicate (TEOS) on titanium distribution of TS-1 zeolite[J]. Journal of Fuel Chemistry and Technology, 2022, 50(11): 1471-1479. doi: 10.1016/S1872-5813(22)60022-7

PDF( 16063 KB)

Effect of hydrolysis of tetraethyl orthosilicate (TEOS) on titanium distribution of TS-1 zeolite

doi: 10.1016/S1872-5813(22)60022-7

GENG An-ying^{1, 2
,},
DING Guo-qiang³,
SHE Hao-hao^{1, 2},
WANG Hong-xing^{1, 2},
LI Xian-qing³,
ZHU Yu-lei^{1, 3
,
,}

1.
State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, China
2.
University of Chinese Academy of Sciences, Beijing 100049, China
3.
Synfuels China Co. Ltd, Beijing 101407, China

More Information

Corresponding author: Tel: +86-010-69667798, E-mail: zhuyulei@sxicc.ac.cn
Received Date: 2022-03-29
Accepted Date: 2022-04-16
Rev Recd Date: 2022-04-15

Available Online: 2022-04-29

Publish Date: 2022-11-30

Abstract

Abstract

The hydrolysis process of tetraethyl orthosilicate (TEOS) was tracked by FT-IR analysis, and the effect of hydrolysis time on the distribution of titanium species in TS-1 zeolites was discussed through XRF and UV-Vis. The catalytic oxidation performance of TS-1 zeolite was tested by 1-hexene epoxidation as a model reaction. The results show that moderate hydrolysis of tetraethyl orthosilicate can effectively inhibit the formation of extra-framework Ti and increase the content of framework Ti. However, shorter or longer hydrolysis time is not conducive to the entry of titanium into the skeleton, and reduce the catalytic performance of TS-1 zeolites. TS-1 prepared with 2 h TEOS hydrolysis time has the best catalytic performance for epoxidation of 1-hexene. Under the reaction conditions of atmospheric pressure and 60 ℃, the conversion of 1-hexene can reach 37.5% and the selectivity of 1,2-epoxy hexane can maintain at about 85%, and the result has a guiding role for the development of olefin epoxidation catalyst.
- TS-1 zeolites,
- tetraethyl orthosilicate,
- hydrolysis,
- 1-hexene epoxidation

FullText(HTML)

References(28)

References

[1]	YIN J, ZHANG T Q, SCHULMAN E, LIU D X, MENG J Q. Hierarchical porous metallized poly-melamine formaldehyde (PMF) as low-cost and high-efficiency catalyst for cyclic carbonate synthesis from CO₂ and epoxides[J]. J Mater Chem A,2018,6(18):8441−8448. doi: 10.1039/C8TA00625C
[2]	OGAWA H, MIYAMOTO Y, FUJIGAKI T, CHIHARA T. Ring-opening of 1, 2-epoxyalkane with alcohols over H-ZSM-5 in liquid phase[J]. Catal Lett,1996,40(3/4):253−255.
[3]	DING J, XU L, YU Y, WU H H, HUANG S J, YANG Y L, WU J, WU P. Clean synthesis of acetaldehyde oxime through ammoximation on titanosilicate catalysts[J]. Catal Sci Technol,2013,3(10):2587−2595. doi: 10.1039/c3cy00471f
[4]	WU G Q, XIAO J H, ZHANG L, WANG W J, HONG Y P, HUANG H J, JIANG Y, LI L, WANG C R. Copper-modified TS-1 catalyzed hydroxylation of phenol with hydrogen peroxide as the oxidant[J]. RSC Adv,2016,6(103):101071−101078. doi: 10.1039/C6RA20980G
[5]	DU Q, GUO Y P, DUAN H N, LI H, CHEN Y J, LIU H Z. Synthesis of hierarchical TS-1 zeolite via a novel three-step crystallization method and its excellent catalytic performance in oxidative desulfurization[J]. Fuel,2017,188:232−238. doi: 10.1016/j.fuel.2016.10.045
[6]	刘斌, 李钢, 王祥生. TS-1/H₂O₂催化模拟汽油中噻吩的选择氧化研究[J]. 燃料化学学报,2006,34(5):629−632. doi: 10.3969/j.issn.0253-2409.2006.05.023 LIU Bin, LI Gang, WANG Xiang-sheng. Selective oxidation of thiophene from model gasoline over TS-1/H₂O₂[J]. J Fuel Chem Technol,2006,34(5):629−632. doi: 10.3969/j.issn.0253-2409.2006.05.023
[7]	CLERICI M G, INGALLINA P. Epoxidation of lower olefins with hydrogen-peroxide and titanium silicalite[J]. J Catal,1993,140(1):71−83. doi: 10.1006/jcat.1993.1069
[8]	马书启, 李钢, 王祥生, 金长子, 刘民, 郭新闻. 钛硅分子筛催化1-丁烯环氧化研究[J]. 燃料化学学报,2005,33(4):509−512. doi: 10.3969/j.issn.0253-2409.2005.04.027 MA Shu-qi, LI Gang, WANG Xiang-sheng, JIN Chang-zi, LIU Min, GUO Xin-wen. 1-Butylene epoxidation over various titanosilicate molecular sieves[J]. J Fuel Chem Technol,2005,33(4):509−512. doi: 10.3969/j.issn.0253-2409.2005.04.027
[9]	BORDIGA S, COLUCCIA S, LAMBERTI C, MARCHESE L, ZECCHINA A. XAFS study of Ti-Silicalite: structure of framework Ti(IV) in the presence and absence of reactive molecules (H₂O, NH₃) and comparison with ultraviolet-visible and IR results[J]. J Phys Chem,1994,98(15):4125−4132. doi: 10.1021/j100066a036
[10]	ALBA-RUBIO A C, FIERRO J L G, LEÓN-REINA L, MARISCAL J A, DUMESIC M, GRANADOS L. Oxidation of furfural in aqueous H₂O₂ catalysed by titanium silicalite: deactivation processes and role of extraframework Ti oxides[J]. Appl Catal B: Environ,2017,202:269−280. doi: 10.1016/j.apcatb.2016.09.025
[11]	MILLINI R, MASSARA E P, PEREGO G, BELLUSSI G. Framework composition of titanium silicalite-1[J]. J Catal,1992,137(2):497−503. doi: 10.1016/0021-9517(92)90176-I
[12]	THANGARAJ A, KUMAR R, MIRAJKAR S, RATNASAMY P. Catalytic properties of crystalline titanium silicalites I: synthesis and characterization of titanium-rich zeolites with MFI structure[J]. J Catal,1991,130(1):1−8. doi: 10.1016/0021-9517(91)90086-J
[13]	SASIDHARAN M, WU P, TAKASHI T. Direct formation of pinacols from olefins over various titano-silicates[J]. J Catal,2002,209:260−265. doi: 10.1006/jcat.2002.3595
[14]	SERRANO D P, SANZ R, PIZARRO P, PERAL A, MORENO I. Improvement of the hierarchical TS-1 properties by silanization of protozeolitic units in presence of alcohols[J]. Microporous Mesoporous Mater,2013,166:59−66. doi: 10.1016/j.micromeso.2012.04.050
[15]	WRÓBLEWSKA A, TOŁPA J, KŁOSIN D, MIĄDLICKI P, KOREN Z C, MICHALKIEWICZ B. The application of TS-1 materials with different titanium contents as catalysts for the autoxidation of α-pinene[J]. Microporous Mesoporous Mater,2020,305:110384. doi: 10.1016/j.micromeso.2020.110384
[16]	ZHANG M, REN S Y, GUO Q X, SHEN B J. Synthesis of hierarchically porous zeolite TS-1 with small crystal size and its performance of 1-hexene epoxidation reaction[J]. Microporous Mesoporous Mater,2021,326:111395. doi: 10.1016/j.micromeso.2021.111395
[17]	XUE Y, XIE Y L, WEI H J, WEN Y Q, WANG X Y, LI B J. Improving the performance of TS-1 catalysts for continuous cyclohexanone ammoximation through controlment of active species distribution[J]. New J Chem,2014,38(9):4229−4234. doi: 10.1039/C4NJ00455H
[18]	林民, 舒兴田, 汪燮卿, 赵琦, 韩秀文, 林励吾, 包信和. TS-1分子筛的合成 Ⅰ. ²⁹Si和 ¹H NMR研究正硅酸乙酯的水解[J]. 催化学报,1999,20(1):29−34. doi: 10.3321/j.issn:0253-9837.1999.01.009 LIN Min, SHU Xing-tian, WANG Xie-qin, ZHAO Qi, HAN Xiu-wen, LIN Li-wu, BAO Xin-he. Synthesis of TS-1 zeolite I. Hydrolysis of ethyl orthosilicate by ²⁹Si and¹H NMR[J]. Chin J Catal,1999,20(1):29−34. doi: 10.3321/j.issn:0253-9837.1999.01.009
[19]	范峰滔, 冯兆池, 李灿. 正硅酸乙酯水解过程的原位紫外拉曼光谱研究[C]//第十四届全国光散射学术会议论文摘要集. 北京, 2007: 179–179. FAN Feng-tao, FENG Zhao-chi, LI Can. Study on hydrolysis of ethyl orthosilicate by in situ UV Raman spectroscopy[C]//Abstracts of the 14th National Conference on Light Scattering. Beijing, 2007: 179–179.
[20]	RUBIO F, RUBIO J, OTEO J L. A FT-IR study of the hydrolysis of Tetraethylorthosilicate (TEOS)[J]. Spectrosc Lett,1998,31(1):199−219. doi: 10.1080/00387019808006772
[21]	隋学叶, 刘世权, 程新. 正硅酸乙酯的水解缩聚反应及多孔SiO₂粉体的制备[J]. 中国粉体技术,2006,3:35−39. doi: 10.3969/j.issn.1008-5548.2006.05.010 SUI Xue-ye, LIU Shi-quan, CHENG Xin. Hydrolytic polycondensation of ethyl orthosilicate and preparation of porous SiO₂ powder[J]. China Powder Sci Technol,2006,3:35−39. doi: 10.3969/j.issn.1008-5548.2006.05.010
[22]	XUE T, LIU H, WANG Y, WU H H, WU P, HE M Y. Seed-induced synthesis of small-crystal TS-1 using ammonia as alkali source[J]. Chin J Catal,2015,36(11):1928−1935. doi: 10.1016/S1872-2067(15)60955-X
[23]	WANG J G, WANG Y B, TATSUMI T, ZHAO Y L. Anionic polymer as a quasi-neutral medium for low-cost synthesis of titanosilicate molecular sieves in the presence of high-concentration alkali metal ions[J]. J Catal,2016,338:321−328. doi: 10.1016/j.jcat.2016.03.027
[24]	WANG W H, LI G, LI W G, LIU L P. Synthesis of hierarchical TS-1 by caramel templating[J]. Chem Commun,2011,47(12):3529−3531.
[25]	SHAKERI M, DEHGHANPOUR S B. Preparation of efficient TS-1 with small particle size and enhanced framework Ti[J]. ChemistrySelect,2019,4(16):4771−4774. doi: 10.1002/slct.201900457
[26]	KLAAC J, KULAWIK K, SCHULZ-EKLOFF G, JAEGER N. Comparative spectroscopic study of TS-1 and zeolite-hosted extraframework Titanium oxide dispersions[J]. Stud Surf Sci Catal,1994,84:2261−2268.
[27]	LV Q, LI G, SUN H. Synthesis of hierarchical TS-1 with convenient separation and the application for the oxidative desulfurization of bulky and small reactants[J]. Fuel,2014,130:70−75. doi: 10.1016/j.fuel.2014.04.042
[28]	刘瑶, 苏雪筠. TiO₂溶胶的制备及其性能研究[J]. 佛山陶瓷,2016,9(117):1−5. LIU Yao, SU Xue-jun. Preparation and properties of TiO₂ sol[J]. Foshan Ceramics,2016,9(117):1−5.