二氧化铈催化芳香伯醇氧化偶联制备亚胺和α,β-不饱和酮
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- 英文论文题名：The cascade synthesis of imines and α,β-unsaturated ketones via oxidative coupling of aromatic primary alcohols over ceria catalyst
- 论文作者：张志鑫 ; 王业红 ; 王敏 ; 吕建民 ; 张超锋 ; 张哲 ; 李利花 ; 李名润 ; 蒋景阳 ; 王峰
- 英文论文作者：Zhixin Zhang ; Yehong Wang ; Min Wang ; Jianmin Lu ; Chaofeng Zhang ; Zhe Zhang ; Lihua Li ; Mingrun Li ; Jingyang Jiang ; Feng Wang ; State Key Laboratory of Fine Chemicals ; College of Chemistry ; Faculty of Chemical Environmental and Biological Science and Technology ; Dalian University of Technology ; State key Laboratory of Catalysis ; Dalian National Laboratory for Clean Energy ; Dalian Institute of Chemical Physics ; Chinese Academy of Sciences
- 年：2016
- 作者机构：大连理工大学化学学院精细化工国家重点实验室;中国科学院大连化学物理研究所催化基础国家重点实验室洁净能源国家实验室;
- 论文关键词：二氧化铈 ; 氧化偶联 ; 亚胺 ; α ; β-不饱和酮 ; 晶面效应
- 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-第十五分会：表界面结构调控与催化
- 语种：中文
- 分类号：O621.251
- 学会代码：ZGHY
- 会议名称：中国化学会第30届学术年会-第十五分会 ; 表界面结构调控与催化
- 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：282k
- 原文格式：D
- 会议级别：全国
摘要
二氧化铈基催化剂因其独特的氧化还原性和酸碱性而广泛应用于有机化学中[1]。在此我们报道了CeO_2催化芳香伯醇分别与胺类和酮类化合物发生氧化偶联反应制备亚胺和α,β-不饱和酮。在此类氧化偶联反应中,CeO_2均表现出显著的晶面效应。在(100),(110),(111)这三个低指数晶面中,棒状CeO_2上的(110)晶面表现最好的催化活性。通过Raman光谱和CO_2-TPD表征可知在亚胺合成反应中,其优异的催化活性归因于增强的氧化还原性质[2];而在α,β-不饱和酮合成反应中,棒状CeO_2上共存的氧化还原位点和碱性位点均具有重要作用[3]。
Ceria-based catalysts have been developed for different applications in organic chemistry because of its unique redox and acid-base properties.We herein report the oxidative coupling of primary alcohols with amines and ketones to produce imines and α,β-unsaturated ketones over CeO_2 catalyst,respectively.Strong crystal plane effects of CeO_2 on these oxidative coupling reactions have been identified.The(110) plane of CeO_2 nanorods is the most active plane for these reactions among the three low-index planes(110),(111) and(100).The characterizations with Raman spectroscopy and CO_2-TPD have shown that the unusual catalysis of CeO_2-rod is attributed to the strong redox ability for the imines synthesis and the coexistence of redox and basic active sites for the α,β-unsaturated ketones synthesis,respectively.
Ceria-based catalysts have been developed for different applications in organic chemistry because of its unique redox and acid-base properties.We herein report the oxidative coupling of primary alcohols with amines and ketones to produce imines and α,β-unsaturated ketones over CeO_2 catalyst,respectively.Strong crystal plane effects of CeO_2 on these oxidative coupling reactions have been identified.The(110) plane of CeO_2 nanorods is the most active plane for these reactions among the three low-index planes(110),(111) and(100).The characterizations with Raman spectroscopy and CO_2-TPD have shown that the unusual catalysis of CeO_2-rod is attributed to the strong redox ability for the imines synthesis and the coexistence of redox and basic active sites for the α,β-unsaturated ketones synthesis,respectively.
引文
[1]Vivier,L.;Duprez,D.Chemsuschem 2010,3:654.
[2]Zhang,Z.;Wang,Y.;Wang,M.;Lü,J.;Li,L.;Zhang,Z.;Wang,F.et al.Chin.J.Catal.2015,36:1623.
[3]Zhang,Z.;Wang,Y.;Wang,M.;Lu,J.;Zhang,C.;Li,L.;Jiang,J.;Wang,F.Catal.Sci.Technol.2016,6:1693.
[2]Zhang,Z.;Wang,Y.;Wang,M.;Lü,J.;Li,L.;Zhang,Z.;Wang,F.et al.Chin.J.Catal.2015,36:1623.
[3]Zhang,Z.;Wang,Y.;Wang,M.;Lu,J.;Zhang,C.;Li,L.;Jiang,J.;Wang,F.Catal.Sci.Technol.2016,6:1693.