井冈山大学学报(自然科学版)2024,Vol.45Issue(4) :27-34.DOI:10.3969/j.issn.1674-8085.2024.04.005

层间孔道扩张结构Ti-MWW分子筛的合成及其在环己烯环氧化反应中的应用

SYNTHESIS OF INTERLAYER EXPANSION TI-MWW MOLECULAR SIEVE AND IT'S CATALYTIC PERFORMANCE IN CYCLOHEXENE EPOXIDATION

郭舒隽 李欣澳 胡元 郑笑笑 李德晶
井冈山大学学报(自然科学版)2024,Vol.45Issue(4) :27-34.DOI:10.3969/j.issn.1674-8085.2024.04.005

层间孔道扩张结构Ti-MWW分子筛的合成及其在环己烯环氧化反应中的应用

SYNTHESIS OF INTERLAYER EXPANSION TI-MWW MOLECULAR SIEVE AND IT'S CATALYTIC PERFORMANCE IN CYCLOHEXENE EPOXIDATION

郭舒隽 1李欣澳 2胡元 1郑笑笑 1李德晶1
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作者信息

  • 1. 闽江学院材料与化学工程学院,福建,福州 350108
  • 2. 福州大学化工学院,福建,福州 350108
  • 折叠

摘要

制备具有更大反应通道的Ti-MWW分子筛,可以极大地解决大分子化合物在孔道中的扩散问题,进而提高催化反应的活性.目前通过研究开发了一种新的合成方法,用于合成具有层间孔道扩张结构的Ti-MWW分子筛,将气相二氧化硅、硼酸、六氟钛酸/过氧化氢和四乙基氢氧化铵溶液混合后蒸干制备干凝胶.用干凝胶转换法合成出Ti-MWW前驱体,通过酸洗焙烧得到Ti-MWW分子筛.使用XRD、TEM及BET的表征手段确定Ti-MWW层间扩张结构和额外的介孔结构的存在,原位生成的MWW片状前驱体上层间的硅羟基与过氧钛酸物种的缩合是形成扩张结构的原因.主要是具有更大的反应通道,相比于传统的Ti-MWW,其在使用过氧化氢为氧化剂的环己烯环氧化中转化率从5.46%增加至12.7%,环氧环己烷的选择性也增加至49.5%.尤其是使用TBHP为氧化剂时,环氧环己烷的选择性进一步提高至80.5%.

Abstract

Preparation of Ti-MWW zeolite with larger reaction channel is great important in improving diffusion and catalytic activity in oxidation of bulky molecules.Herein,an innovative strategy of synthesizing interlayer expansion Ti-MWW was proposed in the present study via evaporating the fumed SiO2,boric acid,H2TiF6/H2O2 and TEAOH solution to get mixture dry-gel.The mixture was converted to Ti-MWW precursor by dry-gel conversion,the precursor was then washed by HNO3 and further calcined to fabricate Ti-MWW.Ti-MWW was characterized by XRD,TEM and BET to examine the interlayer expansion structure and extra mesopore volume,the interlayer expansion structure was created via the interaction of silanol group on in-situ ERB lamellar precursor and peroxotitanium.The conversion of cyclohexene increased from 5.46%to 12.7%,and selectivity of 1,2-Epoxycyclohexane(CHO)increased to 49.5%.Furthermore the selectivity of CHO improved to 80.5%when using anhydrous TBHP as an oxidant.

关键词

层间修饰/液相环氧化/Ti-MWW分子筛

Key words

interlayer modification/liquid phase epoxidation/Ti-MWW zeolites

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出版年

2024
井冈山大学学报(自然科学版)
井岗山大学

井冈山大学学报(自然科学版)

影响因子:0.298
ISSN:1674-8085
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