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1.
In this study, we investigated an alternative method for the chemical CO2 reduction reaction in which power ultrasound (488 kHz ultrasonic plate transducer) was applied to CO2-saturated (up to 3%) pure water, NaCl and synthetic seawater solutions. Under ultrasonic conditions, the converted CO2 products were found to be mainly CH4, C2H4 and C2H6 including large amount of CO which was subsequently converted into CH4. We have found that introducing molecular H2 plays a crucial role in the CO2 conversion process and that increasing hydrogen concentration increased the yields of hydrocarbons. However, it was observed that at higher hydrogen concentrations, the overall conversion decreased since hydrogen, a diatomic gas, is known to decrease cavitational activity in liquids. It was also found that 1.0 M NaCl solutions saturated with 2% CO2 + 98% H2 led to maximum hydrocarbon yields (close to 5%) and increasing the salt concentrations further decreased the yield of hydrocarbons due to the combined physical and chemical effects of ultrasound. It was shown that CO2 present in a synthetic industrial flue gas (86.74% N2, 13% CO2, 0.2% O2 and 600 ppm of CO) could be converted into hydrocarbons through this method by diluting the flue gas with hydrogen. Moreover, it was observed that in addition to pure water, synthetic seawater can also be used as an ultrasonicating media for the sonochemical process where the presence of NaCl improves the yields of hydrocarbons by ca. 40%. We have also shown that by using low frequency high-power ultrasound in the absence of catalysts, it is possible to carry out the conversion process at ambient conditions i.e., at room temperature and pressure. We are postulating that each cavitation bubble formed during ultrasonication act as a “micro-reactor” where the so-called Sabatier reaction - - takes place upon collapse of the bubble. We are naming this novel approach as the “Islam-Pollet-Hihn process”. 相似文献
2.
Mechanistic Aspects of a Highly Active Dinuclear Zinc Catalyst for the Co‐polymerization of Epoxides and CO2 下载免费PDF全文
Stefan Kissling Peter T. Altenbuchner Dr. Maximilian W. Lehenmeier Dr. Eberhardt Herdtweck Dr. Peter Deglmann Dr. Uwe B. Seemann Prof. Dr. Bernhard Rieger 《Chemistry (Weinheim an der Bergstrasse, Germany)》2015,21(22):8148-8157
The dinuclear zinc complex reported by us is to date the most active zinc catalyst for the co‐polymerization of cyclohexene oxide (CHO) and carbon dioxide. However, co‐polymerization experiments with propylene oxide (PO) and CO2 revealed surprisingly low conversions. Within this work, we focused on clarification of this behavior through experimental results and quantum chemical studies. The combination of both results indicated the formation of an energetically highly stable intermediate in the presence of propylene oxide and carbon dioxide. A similar species in the case of cyclohexene oxide/CO2 co‐polymerization was not stable enough to deactivate the catalyst due to steric repulsion. 相似文献
3.
4.
Tuning the Basicity of Cyano‐Containing Ionic Liquids to Improve SO2 Capture through Cyano–Sulfur Interactions 下载免费PDF全文
Dr. Guokai Cui Fengtao Zhang Xiuyuan Zhou Prof. Haoran Li Prof. Jianji Wang Prof. Congmin Wang 《Chemistry (Weinheim an der Bergstrasse, Germany)》2015,21(14):5632-5639
A new approach has been developed to improve SO2 sorption by cyano‐containing ionic liquids (ILs) through tuning the basicity of ILs and cyano–sulfur interaction. Several kinds of cyano‐containing ILs with different basicity were designed, prepared, and used for SO2 capture. The interaction between these cyano‐containing ILs and SO2 was investigated by FTIR and NMR methods. Spectroscopic investigations and quantum chemical calculations showed that dramatic effects on SO2 capacity originate from the basicity of the ILs and enhanced cyano–sulfur interaction. Furthermore, the captured SO2 was easy to release by heating or bubbling N2 through the ILs. This efficient and reversible process, achieved by tuning the basicity of ILs, is an excellent alternative to current technologies for SO2 capture. 相似文献
5.
Palladium-containing zeolites catalyze the cycloisomerization of diethyl diallylmalonate to dimethylcyclopentenes. When the reaction is carried out in toluene, the performance of the palladium catalyst depends on the pore size of the zeolites. At 60 °C, palladium adsorbed on large pore size Beta zeolite (pore size ∼7.4 Å) is more active than medium pore size ZSM-5 (pore size ∼5.4 Å). This lower activity of ZSM-5 compared to Beta is attributable to the restricted diffusion of reagent and products through the ZSM-5 channels as compared to Beta zeolite. However, due to the gas-like diffusion characteristic of the supercritical state, the activity of ZSM-5 increases and becomes identical to that of Beta zeolite using supercritical CO2 as medium. 相似文献
6.
The Mannich-type reaction of imines with (1-methoxy-2-methylpropenyloxy)trimethylsilane and aza-Diels-Alder reaction of imines with Danishefsky's diene can be carried out in scCO2 in the presence of lithium heptadecafluorooctanesulfonate which offer a way to synthesize β-amino carbonyl compounds and nitrogen-containing six-membered ring compounds under environmentally benign conditions. 相似文献
7.
Taek‐Joong Kim Baoan Li May‐Britt Hgg 《Journal of Polymer Science.Polymer Physics》2004,42(23):4326-4336
Fixed‐site–carrier membranes were prepared for the facilitated transport of CO2 by casting polyvinylamine (PVAm) on various supports, such as poly(ether sulfone) (PES), polyacrylonitrile (PAN), cellulose acetate (CA), and polysulfone (PSO). The cast PVAm on the support was crosslinked by various methods with glutaraldehyde, hydrochloric acid, sulfuric acid, and ammonium fluoride. Among the membranes tested, the PVAm cast on polysulfone and crosslinked by ammonium fluoride showed the highest selectivity of CO2 over CH4 (>1000). The permeance of CO2 was then measured to be 0.014 m3 (STP)/(m2 bar h) for a 20 μm thick membrane. The effect of the molecular weight of PVAm and feed pressure on the permeance was also investigated. The selectivity increased remarkably with increasing molecular weight and decreased slightly with increased pressure in the range of 1 to 4 bar. © 2004 Wiley Periodicals, Inc. J Polym Sci Part B: Polym Phys 42: 4326–4336, 2004 相似文献
8.
Absolute total electron scattering cross sections for carbon dioxide have been measured at low electron energies using a photoelectron
source. The measurements have been carried out at 27 electron energies varying from 0.91–9.14 eV with an accuracy of ±3%.
The cross sections obtained in the present experiment have been compared with other measurements and theoretical computations. 相似文献
9.
Reactions of the hydrated electron, H atoms, 2-propanol, and methanol radicals with the TiO2 nano-particles have been studied either directly or by competition kinetics. The radicals were produced by radiolysis of 2-propanol, t-butanol, or methanol aqueous solutions in acid pH's. The reactions involve electron injection to the conduction band. As expected, the t-butanol radical is inert towards TiO2 under our conditions, while the other reducing radicals react with TiO2. The reactivity decreases in the order: eaq−>H>CH3COHCH3>CH2OH. Two TiO2 nanocrystallite sizes, with average diameters of 1.0 and 4.7 nm were compared. For equal concentrations (in terms of TiO2 molecules), the rate of electron injection shows relatively little dependency on particle size. The rates of interfacial electron transfer and transfer coefficient are also reported. 相似文献
10.
Solubility of carbon dioxide in aqueous solutions of sodium chloride: Experimental results and correlation 总被引:2,自引:0,他引:2
The solubility of carbon dioxide in aqueous solutions of sodium chloride was measured in the temperature range from 40 to 160°C, up to 6 mol-kg salt solutions and total pressures up to 10 MPa. Pitzer's(1) equations as well as the Chen and Evans(2) model were used to correlate the new data. Results are reported and compared to literature data and correlations. 相似文献