DICP OpenIR
Subject Area物理化学
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; Wang F(王峰); Xu J(徐杰)
Source PublicationJOURNAL OF THE AMERICAN CHEMICAL SOCIETY
2013-01-30
DOI10.1021/ja310498c
Volume135Issue:4Pages:1506-1515
Indexed BySCI ; CCR
Cooperation Status
SubtypeArticle
DepartmentDNL06,DNL12
Funding ProjectDNL06T1,DNL1201
Contribution Rank待补充
WOS HeadingsScience & Technology ; Physical Sciences
Funding Organization1,1 ; 1,1 ; 1,1 ; 1,1
WOS SubjectChemistry, Multidisciplinary
WOS Research AreaChemistry
WOS KeywordSOLVENT-FREE CONDITIONS ; RARE-EARTH-OXIDES ; SOLID-STATE NMR ; MOLYBDENUM OXIDES ; HYDROGEN-PEROXIDE ; ORGANIC-SYNTHESIS ; OXYGEN VACANCIES ; CEO2 CATALYST ; SURFACE-AREA ; BETA ZEOLITE
AbstractThe 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.
Language英语
Funding Organization1,1 ; 1,1 ; 1,1 ; 1,1
URL查看原文
WOS IDWOS:000314492500054
Citation statistics
Cited Times:97[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://cas-ir.dicp.ac.cn/handle/321008/119319
Collection中国科学院大连化学物理研究所
Corresponding AuthorWang F(王峰); Xu J(徐杰)
AffiliationChinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, State Key Lab Catalysis, Dalian 116023, Peoples R China
Recommended Citation
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.,...&徐杰.(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.
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