[1]王漫云,刘涛,潘志爽,等.纳米级钛硅分子筛合成及其催化乙烯制乙二醇性能[J].石化技术与应用,2024,3:181-185.
WANG Man-yun,LIU Tao,PAN Zhi-shuang,et al.Synthesis of nanoscale titanium silicalite molecular sieve and its catalytic performance for ethylene to ethylene glycol[J].Petrochemical technology & application,2024,3:181-185.
点击复制
纳米级钛硅分子筛合成及其催化乙烯制乙二醇性能(PDF)
《石化技术与应用》[ISSN:1009-0046/CN:62-1138/TQ]
- 期数:
-
2024年3期
- 页码:
-
181-185
- 栏目:
-
- 出版日期:
-
2024-05-10
文章信息/Info
- Title:
-
Synthesis of nanoscale titanium silicalite molecular sieve and its catalytic performance for ethylene to ethylene glycol
- 文章编号:
-
1009-0045(2024)03-0181-05
- 作者:
-
王漫云1; 刘涛1; 潘志爽1; 吕鹏刚1; 赵鸣芝1; 蔡进军1; 段宏昌1; 何涛2
-
1.中国石油石油化工研究院 兰州化工研究中心,甘肃 兰州 730060;2.中国石油云南石化有限公司 生产一部,云南 安宁 650399
- Author(s):
-
WANG Man-yun1; LIU Tao1; PAN Zhi-shuang1; L?譈 Peng-gang1; ZHAO Ming-zhi1; CAI Jin-jun1; DUAN Hong-chang1; HE Tao2
-
1.Lanzhou Petrochemical Research Center,Petrochemical Research Institute,PetroChina,Lanzhou 730060,China;2.Production Division Ⅰ of Yunnan Petrochemical Co Ltd,PetroChina,Anning 650399,China
-
- 关键词:
-
钛硅分子筛; 硅酸四乙酯; 催化氧化; 乙烯; 乙二醇; 选择性
- Keywords:
-
titanium silicalite molecular sieve; tetraethyl orthosilicate; catalytic oxidation; ethylene; ethylene glycol; selectivity
- 分类号:
-
TQ 426;TQ 223.16+2
- DOI:
-
DOI:10.19909/j.cnki.ISSN1009-0045.2024.03.0181
- 文献标识码:
-
B
- 摘要:
-
以四丙基氢氧化铵为模板剂,钛酸四丁酯为Ti源,硅酸四乙酯(TEOS)、钠型硅溶胶或铵型硅溶胶分别为Si源,通过水热晶化法制备出一系列钛硅分子筛(TS-1),利用X射线衍射仪、自动物理吸附仪、荧光光谱仪、傅里叶红外光谱仪、扫描电子显微镜、紫外可见分光光度计等仪器对合成的样品进行了表征,考察了Ti源引入温度、Si源种类、晶化时间以及硅钛比[n(Si)/n(Ti),下同]对合成TS-1的影响,并对比评价了系列TS-1催化乙烯制乙二醇(EG)的性能。结果表明:在常温下引入Ti源,选择TEOS作Si源,晶化时间为1 d,硅钛比为50的条件下所合成TE-50 N-1样品的催化性能最优,H2O2转化率为80.04%,EG选择性为97.19%。
- Abstract:
-
A series of titanium silicalite molecular sieves (TS-1) were prepared by hydrothermal crystallization method by using tetrapropylammonium hydroxide as template, tetrabutyl titanate as Ti source, tetraethyl orthosilicate (TEOS), sodium silica sol or ammonium silica sol as the Si sources, respectively. The synthesized samples were characterized by X-ray diffractometer, automatic physical adsorption instrument, fluorescence spectrometer, Fourier transform infrared spectrometer, scanning electron microscope and ultraviolet-visible spectrophotometer. The effects of Ti source introduction temperature, Si source type, crystallization time and Si/Ti ratio [n (Si)/n (Ti), the same below] on the synthesis of TS-1 were investigated, and the catalytic performance of a series of TS-1 for ethylene to ethylene glycol (EG) was compared and evaluated. The results showed that the TE-50 N-1 sample synthesized under the conditions of introducing Ti source at room temperature, selecting TEOS as Si source, crystallization time of 1 d, and Si/Ti ratio of 50 had the best catalytic performance, with H2O2 conversion rate of 80.04% and EG selectivity of 97.19%.
参考文献/References
[1] Snamprogetti S P A.Preparation of porous crystalline synthetic material comprised of silicon and titanium oxides:US, 39337982 A[P].1983-10-18.[2] 夏清华,王公慰,应慕良,等.Ti-ZSM-5沸石的合成及表征[J].石油化工,1993(12):781-785.[3] Corma A,Camblor M A,Esteve P,et al.Activity of Ti-beta catalyst for the selective oxidation of alkenes and alkanes[J].Journal of Catalysis,1994,145(1):151-158.[4] Blasco T,Corma A,Navarro M T,et al.Synthesis, characterization and catalytic activity of Ti-MCM-41 structures[J].Journal of Catalysis,2010,156(3):64-74.[5] And P W,Tatsumi T,And T K,et al.Postsynthesis, characterization, and catalytic properties in alkene epoxidation of hydrothermally stable mesoporous Ti-SBA-15[J].Chemistry of Materials,2002,14(4):1657-1664.[6] 魏珍妮,黄鑫,全民强,等.乙烯一步法制乙二醇工艺的研究现状[J].炼油与化工,2020,31(2):4-6.[7] Yue H R,Zhao Y J,Ma X B,et al.Ethylene glycol: Properties,synthesis,and applications[J].Chemical Society Reviews,2012,41(11):4218-4244.[8] 王永胜.影响合成气制乙二醇质量关键指标的因素及控制方法[J].化肥设计,2019(4):28-30.[9] Lin D,Zhang Q D,Qin Z X, et al.Reversing titanium oligomers formation towards high-efficiency and green synthesis of titanium-containing molecular sieves[J].Angewandte Chemie,2021,60(7):3443-3448.[10] Huo C,Tian X,Nan Y,et al.3 D printing of hierarchically porous monolithic TS-1 catalyst for one-pot synthesis of ethylene glycol[J].Chemical Engineering Journal,2022,450:138259. [11] Millini R,Massara E P,Perego G,et al.Framework composition of titanium silicalite-1[J].Journal of Catalysis,1992,137(2):497-503.[12] Emdadi L,Oh S C,Wu Y,et al.The role of external acidity of meso-/microporouszeolites in determining selectivity for acid-catalyzed reactions of benzyl alcohol[J].Journal of Catalysis,2016,335:165-174.[13] Kraushaar B,Hooff V J.A test reaction for titanium silicalite catalysts[J].Catalysis Letters,1989,2(1):43-47.[14] Zhuang J,Ding M A,Yan Z,et al.Effect of acidity in TS-1 zeolites on product distribution of the styrene oxidation reaction[J].Applied Catalysis :A General,2004,258(1):1-6.[15] Xiong G,Cao Y Y,Guo Z D,et al.The roles of different titanium species in TS-1 zeolite in propylene epoxidation studied by in situ UV Raman spectroscopy[J].Physical Chemistry Chemical Physics,2016,18(1):190-196.
备注/Memo
- 备注/Memo:
-
中国石油天然气集团有限公司资助项目(项目编号:LZSH 202206)
更新日期/Last Update:
2024-05-10