中国科学院大连化学物理研究所机构知识库
Advanced  
DICP OpenIR  > 中国科学院大连化学物理研究所  > 期刊论文
学科主题: 物理化学
题名: Heterogeneous Ceria Catalyst with Water-Tolerant Lewis Acidic Sites for One-Pot Synthesis of 1,3-Diols via Prins Condensation and Hydrolysis Reactions
作者: Wang, Yehong1;  Wang, Feng1;  Song, Qi1;  Xin, Qin1;  Xu, Shutao1;  Xu, Jie1
通讯作者: 王峰 ;  徐杰
刊名: JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
发表日期: 2013-01-30
DOI: 10.1021/ja310498c
卷: 135, 期:4, 页:1506-1515
收录类别: SCI ;  CCR
合作性质: 
文章类型: Article
部门归属: DNL06,DNL12
项目归属: DNL06T1,DNL1201
产权排名: 待补充
WOS标题词: Science & Technology ;  Physical Sciences
类目[WOS]: Chemistry, Multidisciplinary
资助者: 1,1
研究领域[WOS]: Chemistry
英文摘要: The use of a heterogeneous Lewis acid catalyst, which is insoluble and easily separable during the reaction, is a promising option for hydrolysis reactions from both environmental and practical viewpoints. In this study, ceria showed excellent catalytic activity in the hydrolysis of 4-methyl-1,3-dioxane to 1,3-butanediol in 95% yield and in the one-pot synthesis of 1,3-butanediol from propylene and formaldehyde via Prins condensation and hydrolysis reactions in an overall yield of 60%. In-depth investigations revealed that ceria is a water-tolerant Lewis acid catalyst, which has seldom been reported previously. The ceria catalysts showed rather unusual high activity in hydrolysis, with a turnover number (TON) of 260, which is rather high for bulk oxide catalysts, whose TONs are usually less than 100. Our conclusion that ceria functions as a Lewis acid catalyst in hydrolysis reactions is firmly supported by thorough characterizations with IR and Raman spectroscopy, acidity measurements with IR and P-31 magic-angle-spinning NMR spectroscopy, Na+/H+ exchange tests, analyses using the in situ active-site capping method, and isotope-labeling studies. A relationship between surface vacancy sites and catalytic activity has been established. CeO2(111) has been confirmed to be the catalytically active crystalline facet for hydrolysis. Water has been found to be associatively adsorbed on oxygen vacancy sites with medium strength, which does not lead to water dissociation to form stable hydroxides. This explains why the ceria catalyst is water-tolerant.
关键词[WOS]: SOLVENT-FREE CONDITIONS ;  RARE-EARTH-OXIDES ;  SOLID-STATE NMR ;  MOLYBDENUM OXIDES ;  HYDROGEN-PEROXIDE ;  ORGANIC-SYNTHESIS ;  OXYGEN VACANCIES ;  CEO2 CATALYST ;  SURFACE-AREA ;  BETA ZEOLITE
语种: 英语
原文出处: 查看原文
WOS记录号: WOS:000314492500054
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/119319
Appears in Collections:中国科学院大连化学物理研究所_期刊论文

Files in This Item: Download All
File Name/ File Size Content Type Version Access License
2013hFDWUnhAe1.PDF(4050KB)----开放获取View Download

作者单位: 1.Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, State Key Lab Catalysis, Dalian 116023, Peoples R China

Recommended Citation:
Wang, Yehong,Wang, Feng,Song, Qi,et al. Heterogeneous Ceria Catalyst with Water-Tolerant Lewis Acidic Sites for One-Pot Synthesis of 1,3-Diols via Prins Condensation and Hydrolysis Reactions[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,2013,135(4):1506-1515.
Service
 Recommend this item
 Sava as my favorate item
 Show this item's statistics
 Export Endnote File
Google Scholar
 Similar articles in Google Scholar
 [Wang, Yehong]'s Articles
 [Wang, Feng]'s Articles
 [Song, Qi]'s Articles
CSDL cross search
 Similar articles in CSDL Cross Search
 [Wang, Yehong]‘s Articles
 [Wang, Feng]‘s Articles
 [Song, Qi]‘s Articles
Related Copyright Policies
Null
Social Bookmarking
  Add to CiteULike  Add to Connotea  Add to Del.icio.us  Add to Digg  Add to Reddit 
文件名: 2013hFDWUnhAe1.PDF
格式: Adobe PDF
此文件暂不支持浏览
所有评论 (0)
暂无评论
 
评注功能仅针对注册用户开放,请您登录
您对该条目有什么异议,请填写以下表单,管理员会尽快联系您。
内 容:
Email:  *
单位:
验证码:   刷新
您在IR的使用过程中有什么好的想法或者建议可以反馈给我们。
标 题:
 *
内 容:
Email:  *
验证码:   刷新

Items in IR are protected by copyright, with all rights reserved, unless otherwise indicated.

 

 

Valid XHTML 1.0!
Powered by CSpace