多级孔钛硅分子筛催化环己烯合成环氧环己烷性能研究

王洋; 贾立明; 白红鑫

doi:10.12434/j.issn.2097-2547.20250036

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多级孔钛硅分子筛催化环己烯合成环氧环己烷性能研究

低碳分子转化合成 | 更新时间：2025-11-25

- 多级孔钛硅分子筛催化环己烯合成环氧环己烷性能研究
- Study on catalytic performances of hierarchical titanium silicate zeolites for synthesis of epoxycyclohexane from cyclohexene
- 低碳化学与化工 2025, 50(11): 36-43.
- 作者机构：
  
  中石化（大连）石油化工研究院有限公司，辽宁大连 116045
- 作者简介：
  
  王洋（1996—），硕士，助理研究员，研究方向为低碳分子合成，E-mail：wangyang.fshy@sinopec.com。
  白红鑫（1989—），博士，副研究员，研究方向为低碳分子合成，E-mail：baihongxin.fshy@sinopec.com。
- 基金信息：
  
  国家自然科学基金重点项目(22438004)
- DOI：10.12434/j.issn.2097-2547.20250036
  中图分类号： TQ23;TQ426
- 收稿：2025-01-23，
  
  修回：2025-02-27，
  
  纸质出版：2025-11-25
- 稿件说明：
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王洋,贾立明,白红鑫.多级孔钛硅分子筛催化环己烯合成环氧环己烷性能研究[J].低碳化学与化工,2025,50(11):36-43.

WANG Yang,JIA Liming,BAI Hongxin.Study on catalytic performances of hierarchical titanium silicate zeolites for synthesis of epoxycyclohexane from cyclohexene[J].Low-Carbon Chemistry and Chemical Engineering,2025,50(11):36-43.
王洋,贾立明,白红鑫.多级孔钛硅分子筛催化环己烯合成环氧环己烷性能研究[J].低碳化学与化工,2025,50(11):36-43. DOI： 10.12434/j.issn.2097-2547.20250036.

WANG Yang,JIA Liming,BAI Hongxin.Study on catalytic performances of hierarchical titanium silicate zeolites for synthesis of epoxycyclohexane from cyclohexene[J].Low-Carbon Chemistry and Chemical Engineering,2025,50(11):36-43. DOI： 10.12434/j.issn.2097-2547.20250036.

摘要

环氧环己烷作为重要的有机中间体，在化学化工领域具有广阔的应用前景。然而，目前其合成路径面临环氧环己烷选择性较低，反应效率不高等问题。钛硅分子筛具有独特的孔道结构和催化活性中心，可用于环氧环己烷的高效合成。制备了两种钛硅分子筛（Ti-CHO-1和Ti-CHO-2），采用XRD和UV-Raman等对Ti-CHO-1和Ti-CHO-2的结构进行了表征。研究了Ti-CHO-1和Ti-CHO-2在双氧水（H

）氧化环己烯合成环氧环己烷中的催化性能，并在优选钛硅分子筛的作用下优化了反应条件。结果表明，与Ti-CHO-1相比，具有多级孔结构的Ti-CHO-2的锐钛矿型TiO

含量较小、酸性较低，因此催化性能更好。在溶剂为乙腈、温度为80 ℃、时间为4.0 h、环己烯用量为40 mmol、30%（质量分数）H

用量为40 mmol（滴加时间为10 min）、乙二胺四乙酸二钠用量为60 mg和Ti-CHO-2用量为0.8 g的最优条件下，环己烯转化率、环氧环己烷选择性和环氧环己烷产率分别为87.2%、83.1%和72.5%。在最优条件下循环使用5次，Ti-CHO-2的催化性能可保持稳定，表现出良好的可回收性。

Abstract

As an important organic intermediate

epoxycyclohexane has shown a very broad application prospect in the field of chemistry and chemical engineering. However

current synthesis faces the problems of low selectivity and efficiency. Titanium silicate zeolites have unique porous structures and catalytic active centers

which can be used for efficient synthesis of epoxycyclohexane. Two types of titanium silicate zeolites (Ti-CHO-1 and Ti-CHO-2) were prepared

and their structures were characterized by XRD and UV-Raman spectroscopy

etc. The catalytic performance of Ti-CHO-1 and Ti-CHO-2 in synthesis of epoxycyclohexane by hydrogen peroxide (H

)oxidation of cyclohexene was studied

and the reaction conditions were optimized by optimal titanium silicate zeolites. The results indicate that compared to Ti-CHO-1

Ti-CHO-2 with hierarchical structure has a lower TiO

content and lower acidity

resul

ting in better catalytic performance. Under the optimal conditions of acetonitrile solvent

temperature of 80 ℃

time of 4.0 h

cyclohexene dosage of 40 mmol

30% (mass fraction) H

dosage of 40 mmol (dropping time of 10 min)

EDTA disodium salt dosage of 60 mg and Ti-CHO-2 dosage of 0.8 g

the conversion rate of cyclohexene

selectivity of epoxycyclohexane and yield of epoxycyclohexane are 87.2%

83.1%

and 72.5%

respectively. Under optimal conditions for 5 cycles

the catalytic performance of Ti-CHO-2 can remain stable

which demonstrates that it has good recyclability.

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references

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