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  A mononuclear tantalum catalyst with a peroxocarbonate ligand for olefin epoxidation in compressed CO2

Ma, W., Qiao, Y., Theyssen, N., Zhou, Q., Li, D., Ding, B., et al. (2019). A mononuclear tantalum catalyst with a peroxocarbonate ligand for olefin epoxidation in compressed CO2. Catalysis Science & Technology, 9(7), 1621-1630. doi:10.1039/C9CY00056A.

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 Creators:
Ma, Wenbao1, Author
Qiao, Yunxiang2, Author              
Theyssen, Nils2, Author              
Zhou, Qingqing1, Author
Li, Difan1, Author
Ding, Bingjie1, Author
Wang, Dongqi3, Author
Hou, Zhenshan1, Author
Affiliations:
1Key Laboratory for Advanced Materials, Research Institute of Industrial Catalysis, East China University of Science and Technology, Shanghai 200237, People's Republic of China , ou_persistent22              
2Service Department Theyssen (Technical Labs), Max-Planck-Institut für Kohlenforschung, Max Planck Society, ou_1445632              
3Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, China, ou_persistent22              

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 Abstract: A new class of tantalum-based peroxocarbonate ionic liquid ([P4,4,4,4]3[Ta(η2-O2)3(CO4)]) has been generated through the reaction of pressurized CO2 with [P4,4,4,4]3[Ta(O)32-O2)] in the presence of H2O2 during the reaction process. The newly formed species has been verified by NMR, FT-IR, HRMS and density functional theory (DFT) calculations. The CO2-induced monomeric peroxocarbonate anion-based ionic liquid is more advantageous than the monomeric peroxotantalate analogue for the epoxidation of olefins under very mild conditions. Interestingly, the transformation between peroxotantalate and peroxocarbonate species is completely reversible, and CO2 can actually act as a trigger agent for epoxidation reaction. The further mechanism studies by DFT calculation reveal that peroxo η2-O2 (site a) affords higher reactivity towards the C=C bond than that of peroxocarbonate–CO4 (site b). These quantitative illustrations of the relationship between structural properties and kinetic consequences enable rational design for an efficient and environmental IL catalyst for the epoxidation of olefins.

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Language(s): eng - English
 Dates: 2019-01-102019-02-222019-02-262019-04-07
 Publication Status: Published in print
 Pages: 10
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1039/C9CY00056A
 Degree: -

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Title: Catalysis Science & Technology
  Other : Catal. Sci. Technol.
Source Genre: Journal
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Publ. Info: Cambridge : Royal Society of Chemistry
Pages: - Volume / Issue: 9 (7) Sequence Number: - Start / End Page: 1621 - 1630 Identifier: ISSN: 2044-4753
CoNE: https://pure.mpg.de/cone/journals/resource/2044-4753