Heterogeneous Ceria Catalyst with Water-Tolerant Lewis Acidic Sites for One-Pot Synthesis of 1,3-Diols via Prins Condensation and Hydrolysis Reactions

	Heterogeneous Ceria Catalyst with Water-Tolerant Lewis Acidic Sites for One-Pot Synthesis of 1,3-Diols via Prins Condensation and Hydrolysis Reactions
	Wang, Yehong; Wang, Feng; Song, Qi; Xin, Qin; Xu, Shutao; Xu, Jie
刊名	journal of the american chemical society
	2013-01-30
卷号	135 期号:4 页码:1506-1515
通讯作者	王峰 ; 徐杰
产权排序	待补充
合作状况	英
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.
学科主题	物理化学
WOS标题词	science & technology ; physical sciences
类目[WOS]	chemistry, multidisciplinary
研究领域[WOS]	chemistry
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
收录类别	SCI ; CCR
资助信息	1，1
原文出处	1515
语种	英语
WOS记录号	WOS:000314492500054
公开日期	2014-09-11
内容类型	期刊论文
源URL	[http://159.226.238.44/handle/321008/119319]
专题	大连化学物理研究所_中国科学院大连化学物理研究所
作者单位	Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, State Key Lab Catalysis, Dalian 116023, Peoples R China
推荐引用方式 GB/T 7714	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.
APA	Wang, Yehong,Wang, Feng,Song, Qi,Xin, Qin,Xu, Shutao,&Xu, Jie.(2013).Heterogeneous Ceria Catalyst with Water-Tolerant Lewis Acidic Sites for One-Pot Synthesis of 1,3-Diols via Prins Condensation and Hydrolysis Reactions.journal of the american chemical society,135(4),1506-1515.
MLA	Wang, Yehong,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".journal of the american chemical society 135.4(2013):1506-1515.