中文版 | English
Title

Highly efficient multi-site synergistic catalysis of a polyoxovanadate-based metal-organic framework for benzylic C-H bond oxidation

Author
Corresponding AuthorLu, Ying; Liu, Shu-Xia
Publication Years
2022-07-01
DOI
Source Title
ISSN
2050-7488
EISSN
2050-7496
Volume10Pages:16514-16523
Abstract
The selective oxidation of C-H bonds of benzylic compounds to synthesize high-value-added ketones remains a challenge under mild conditions, and the ambiguity of its oxidation mechanism limits the further development of this field. In this work, we construct a polyoxometalate-based metal-organic framework (POMOF), [(Cu2CuII)-Cu-I(bix)(2)]{V4O12} (1, bix = 1,4-bis(imidazole-1-ylmethyl)benzene), successfully achieving the efficient oxidation catalysis of various benzylic compounds with outstanding conversion, selectivity and durability under mild conditions. Our experimental studies suggest that the highly catalytic activity of 1 derives from its attractive structure with multiple active sites, which consists of VV centers in a unique U-type {V4O12}(4-) ({V-4}) cluster and Cu-I and Cu-II centers bridged to the {V-4} cluster. Importantly, further theoretical calculations indicate that there exists synergistic catalysis between Cu-I/{V-4} sites and Cu-II/{V-4} sites for 1 as catalyst in the oxidation of benzylic compounds, where the {V-4} cluster mainly provides deprotonation and oxidation sites, and the CuI site plays a role in the reduction of the oxidant, while the Cu-II site plays a role in the adsorption of the oxidant. This is the first POMOF whose catalytic mechanism towards the oxidation of benzylic C-H bonds is deeply studied through the combination of experiments and theoretical calculations, providing a new perspective for the design of related catalysts.
URL[Source Record]
Indexed By
SCI ; EI
Language
English
SUSTech Authorship
Others
Funding Project
National Natural Science Foundation of China["22172022","22071019","21872021"]
WOS Research Area
Chemistry ; Energy & Fuels ; Materials Science
WOS Subject
Chemistry, Physical ; Energy & Fuels ; Materials Science, Multidisciplinary
WOS Accession No
WOS:000827058800001
Publisher
EI Accession Number
20223112468372
EI Keywords
Catalyst activity ; Catalytic oxidation ; Ketones ; Metal-Organic Frameworks ; Organic polymers ; Oxidants
ESI Classification Code
Air Pollution Control:451.2 ; Metallurgy:531.1 ; Chemical Reactions:802.2 ; Chemical Agents and Basic Industrial Chemicals:803 ; Chemical Products Generally:804 ; Organic Compounds:804.1 ; Organic Polymers:815.1.1
Data Source
Web of Science
Citation statistics
Cited Times [WOS]:6
Document TypeJournal Article
Identifierhttp://kc.sustech.edu.cn/handle/2SGJ60CL/359461
DepartmentDepartment of Chemistry
深圳格拉布斯研究院
Affiliation
1.Northeast Normal Univ, Coll Chem, Minist Educ, Key Lab Polyoxometalate & Reticular Mat Chem, Changchun 130024, Jilin, Peoples R China
2.Southern Univ Sci & Technol, Shenzhen Grubbs Inst, Dept Chem, Shenzhen 518055, Guangdong, Peoples R China
Recommended Citation
GB/T 7714
Dang, Tian-Yi,Li, Run-Han,Tian, Hong-Rui,et al. Highly efficient multi-site synergistic catalysis of a polyoxovanadate-based metal-organic framework for benzylic C-H bond oxidation[J]. Journal of Materials Chemistry A,2022,10:16514-16523.
APA
Dang, Tian-Yi,Li, Run-Han,Tian, Hong-Rui,Guan, Wei,Lu, Ying,&Liu, Shu-Xia.(2022).Highly efficient multi-site synergistic catalysis of a polyoxovanadate-based metal-organic framework for benzylic C-H bond oxidation.Journal of Materials Chemistry A,10,16514-16523.
MLA
Dang, Tian-Yi,et al."Highly efficient multi-site synergistic catalysis of a polyoxovanadate-based metal-organic framework for benzylic C-H bond oxidation".Journal of Materials Chemistry A 10(2022):16514-16523.
Files in This Item:
There are no files associated with this item.
Related Services
Fulltext link
Recommend this item
Bookmark
Usage statistics
Export to Endnote
Export to Excel
Export to Csv
Altmetrics Score
Google Scholar
Similar articles in Google Scholar
[Dang, Tian-Yi]'s Articles
[Li, Run-Han]'s Articles
[Tian, Hong-Rui]'s Articles
Baidu Scholar
Similar articles in Baidu Scholar
[Dang, Tian-Yi]'s Articles
[Li, Run-Han]'s Articles
[Tian, Hong-Rui]'s Articles
Bing Scholar
Similar articles in Bing Scholar
[Dang, Tian-Yi]'s Articles
[Li, Run-Han]'s Articles
[Tian, Hong-Rui]'s Articles
Terms of Use
No data!
Social Bookmark/Share
No comment.

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