DOI: 10.1016/j.jcou.2017.12.003
Scopus记录号: 2-s2.0-85036663414
论文题名: Efficient solvent-free fixation of CO2 catalyzed by new recyclable bifunctional metal complexes
作者: Peng J. ; Yang H.-J. ; Wang S. ; Ban B. ; Wei Z. ; Lei B. ; Guo C.-Y.
刊名: Journal of CO2 Utilization
ISSN: 22129820
出版年: 2018
卷: 24 起始页码: 1
结束页码: 9
语种: 英语
英文关键词: Activation energy
; Atmospheric pressure
; Bifunctional metal complexes
; Chemical fixation of carbon dioxide
; Cyclic carbonate
; Selectivity
Scopus关键词: Activation energy
; Atmospheric chemistry
; Atmospheric pressure
; Carbon
; Carbon dioxide
; Carbonation
; Catalysis
; Catalyst activity
; Catalyst selectivity
; Catalysts
; Chemical activation
; Chemical bonds
; Chemical reactions
; Cobalt compounds
; Copper
; Copper compounds
; Kinetic theory
; Lead compounds
; Metal complexes
; Metal ions
; Metals
; Nickel
; Nickel compounds
; Synthesis (chemical)
; Zinc
; Zinc compounds
; Activation energies (Ea)
; Apparent activation energy
; Bi-functional
; Bi-functional catalysts
; Catalytic performance
; Chemical fixation of carbon dioxide
; Cyclic carbonates
; Optimized reaction conditions
; Chlorine compounds
英文摘要: A series of metal complexes containing a metal ion (Zn, Cu, Pb, Ni, Co) and two quaternary phosphonium salt units anchored on the ligands were designed and synthesized as efficient single-component bifunctional catalyst for the solvent-free coupling reaction of CO2 and epoxides without any co-catalysts. The effects of various reaction variables on the catalytic activity were investigated systematically and the optimized reaction conditions were screened as (130 °C, 1 MPa and 5 h). The order of the catalytic activity for these single-component bifunctional metal complexes was found to be Zn-PPBCl (96%) > Co-PPBCl (90%) ≈ Ni-PPBCl (90%) > Pb-PPBCl (86%) > Cu-PPBCl (15%). Notably, a high turnover frequency (TOF) value (1230 h−1) for bifunctional catalyst Zn-PPBCl was achieved via adjusting reaction variables. Moreover, this series of catalysts can also catalyze the coupling reaction at atmospheric pressure, and most of them showed high conversion of epoxide (propylene carbonate (PC) yield > 90%) within 7 h. The catalysts are also applicable to a variety of epoxides and good catalytic performances were achieved for producing the corresponding cyclic carbonates in most cases. Furthermore, the catalyst can be easily recycled and reused for at least five times without dramatic activity loss after simple filtration and drying. Finally, kinetic studies were carried out preliminarily for four metal (Zn, Co, Ni, Pb) catalysts and the formation activation energies (Ea) of cyclic carbonate were obtained. The apparent activation energy Ea catalyzed by Zn-PPBCl is only 37.6 kJ/mol, while the Ea (Pb-PPBCl) is 70.0 kJ/mol, Ea (Ni-PPBCl) is 65.6 kJ/mol, and Ea (Co-PPBCl) is 43.1 kJ/mol. The sequence of Ea agrees well with the catalytic activity. Based on the kinetic studies and experimental results, an inferred mechanism was deduced. © 2017 Citation statistics:
资源类型: 期刊论文
标识符: http://119.78.100.158/handle/2HF3EXSE/111941
Appears in Collections: 气候减缓与适应
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作者单位: The State Key Laboratory of Power Transmission Equipment & System Security and New Technology, College of Chemistry and Chemical Engineering, Chongqing University, Chongqing, 400044, China; Key Laboratory of Catalysis and Materials Science of the State Ethnic Affairs Commission & Ministry of Education, Hubei Province, Key Laboratory of Analytical Chemistry of the State Ethnic Affairs Commission, National Demonstration Center for Experimental Ethnopharmacology Education, College of Chemistry and Materials Science, South-Central University for Nationalities, Wuhan, 430074, China; School of Chemical Sciences, University of Chinese Academy of Sciences, Beijing, 100049, China
Recommended Citation:
Peng J.,Yang H.-J.,Wang S.,et al. Efficient solvent-free fixation of CO2 catalyzed by new recyclable bifunctional metal complexes[J]. Journal of CO2 Utilization,2018-01-01,24