DOI: 10.1016/j.jcou.2014.12.004
Scopus记录号: 2-s2.0-84921381057
论文题名: Synthesis and characterization of manganese(III) and high-valent manganese-oxo complexes and their roles in conversion of alkenes to cyclic carbonates
作者: Ramidi P. ; Felton C.M. ; Subedi B.P. ; Zhou H. ; Tian Z.R. ; Gartia Y. ; Pierce B.S. ; Ghosh A.
刊名: Journal of CO2 Utilization
ISSN: 22129820
出版年: 2015
卷: 9 起始页码: 48
结束页码: 57
语种: 英语
英文关键词: Alkene
; Carbon dioxide
; Cyclic carbonate
; High-valent manganese-oxo
; Manganese(III) catalyst
Scopus关键词: Carbon
; Carbon dioxide
; Carbonation
; Catalysts
; Coordination reactions
; Crystallography
; Electrodeposition
; Electrospray ionization
; Hydrocarbons
; Isotopes
; Manganese
; Mass spectrometry
; Negative ions
; Olefins
; Oxidants
; Single crystals
; Spectrometry
; Synthesis (chemical)
; X ray diffraction
; Cyclic carbonates
; Electrospray ionization mass spectrometry
; Fourier transform infrared spectra
; High-valent manganese-oxo
; Manganese(III)
; Single crystal x-ray diffraction
; Synthesis and characterizations
; Tetrabutylammonium bromide
; X ray crystallography
英文摘要: A novel manganese(III) complex (2) of an amido-amine ligand (1) was successfully synthesized and characterized using various analytical techniques such as 1H NMR and single-crystal X-ray diffraction. X-ray crystallography data of 2 has demonstrated that the complex is a six-coordinated species. Electrospray ionization mass spectrometry (ESI-MS) also showed the characteristic peak (m/z 401.6, negative ion mode) of 2 indicating the formation of the complex. 2 was successfully employed to convert a variety of olefins to cyclic carbonate in the presence of carbon dioxide (CO2), an oxidant (e.g. tert-butylhydroperoxide, TBHP) and a co-catalyst (tetrabutylammonium bromide, TBAB) in a single-pot under mild reaction conditions. Upon reaction with an oxidant, 2 generated a non-heme high-valent manganese-oxo species (3), which was responsible for conversion of alkene to epoxide, and further cycloaddition of CO2 occurs in the presence of 2 and TBAB. The effect of reaction conditions (temperature and pressure), oxidants, and alkenes were systematically investigated for cyclic carbonate synthesis. High turnover numbers (50-240) and yield were obtained when various alkenes were employed. Additionally, 3 was characterized using various spectroscopic and mass spectrometry techniques. Fourier transform infrared spectrum (FT-IR) of 3 indicated a peak at 839 cm-1 corresponding to manganese-oxo stretching. Isotope labeling studies of the oxo group of 3 revealed a peak shift to 804 cm-1 upon exchange of the 16O with 18O. 3 was also characterized by ESI-MS. 18O isotope studies were performed to understand the role of 3 in the catalytic cycle and to further establish the mechanism of the reaction. © 2014 Elsevier Ltd. All rights reserved. 资助项目: National Science Foundation
; National Science Foundation
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资源类型: 期刊论文
标识符: http://119.78.100.158/handle/2HF3EXSE/52977
Appears in Collections: 影响、适应和脆弱性
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Recommended Citation:
Ramidi P.,Felton C.M.,Subedi B.P.,et al. Synthesis and characterization of manganese(III) and high-valent manganese-oxo complexes and their roles in conversion of alkenes to cyclic carbonates[J]. Journal of CO2 Utilization,2015-01-01,9