Ti-YNU-1分子筛中新型钛物种的确定及催化活性的理论计算
详细信息 查看官网全文
- 英文论文题名：Theoretical Calculations on the Determination of Novel Ti Species in Ti-YNU-1 and Catalytic Properties
- 论文作者：王译晨 ; 李蒙召 ; 周丹红
- 英文论文作者：Yichen Wang ; Mengzhao Li ; Danhong Zhou ; College of Chemistry and Chemical Engineering ; Liaoning Normal University
- 年：2016
- 作者机构：辽宁师范大学化学化工学院;
- 论文关键词：Ti-YNU-1 ; 振动光谱 ; 钛氧活性中间体 ; 活化能垒 ; 密度泛函理论
- 会议召开时间：2016-07-01
- 会议录名称：中国化学会第30届学术年会摘要集-第三十三分会：绿色化学
- 语种：中文
- 分类号：O643.36
- 学会代码：ZGHY
- 会议名称：中国化学会第30届学术年会-第三十三分会 ; 绿色化学
- 会议地点：中国辽宁大连
- 主办单位：中国化学会
- 学会名称：中国化学会
- 页数：1
- 文件大小：174k
- 原文格式：D
- 会议级别：全国
摘要
富Ti的Ti-YNU-1分子筛的红外光谱中930 cm~(-1)特征峰属于一种新的骨架钛物种,而且表现出更高的催化活性。这个新型钛物种的结构以及催化作用机理尚不明确。本文应用密度泛函理论计算,研究了Ti-YNU-1分子筛上骨架钛物种的结构和振动光谱,考察了活性中心结构以及1-己烯环氧化反应的催化机理,并与Ti-MWW分子筛进行对比。所有计算在B3LYP/6-31G(d,p)理论水平进行。结果表明,在富Ti的Ti-YNU-1分子筛的红外光谱中930 cm~(-1)的Ti特征峰归属于Ti1OH(T6nest)或Ti6OH物种。在层间开放位点的钛氧活性中心上,1-己烯环氧化反应的活化能更低,表明Ti-YNU-1分子筛的活性高于Ti-MWW分子筛,与实验结果很好地吻合。
Density functional theory was used to study the microstructure,vibrational spectra of framework Ti species in Ti-YNU-1 zeolite.We also explored the structure of active centers and the mechanism of 1-hexene epoxidation in Ti-YNU-1 and compared with Ti-MWW zeolite.The results indicated that the Ti-specific peak at 930 cm~(-1) in the IR spectrum of Ti-rich Ti-YNU-1 is attributed to Ti1OH(T6nest) or Ti60 H species.The activation energy of1-hexene epoxidation at interlayer open site is lower,showing that Ti-YNU-1 is more active than Ti-MWW,which is in very good agreement with the experiment measurements.
Density functional theory was used to study the microstructure,vibrational spectra of framework Ti species in Ti-YNU-1 zeolite.We also explored the structure of active centers and the mechanism of 1-hexene epoxidation in Ti-YNU-1 and compared with Ti-MWW zeolite.The results indicated that the Ti-specific peak at 930 cm~(-1) in the IR spectrum of Ti-rich Ti-YNU-1 is attributed to Ti1OH(T6nest) or Ti60 H species.The activation energy of1-hexene epoxidation at interlayer open site is lower,showing that Ti-YNU-1 is more active than Ti-MWW,which is in very good agreement with the experiment measurements.
引文
[1]Song,S.;Wang,P.;He,Y;Li,J.et al.Microporous Mesoporous Mater.2012,159:74.
[2]Ruan,J.;Wu,P.;Slater,B.;Terasaki,O.Angew.Chem.Int.Ed.2005,44(41):6719.
[2]Ruan,J.;Wu,P.;Slater,B.;Terasaki,O.Angew.Chem.Int.Ed.2005,44(41):6719.