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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.
Dr. Manussada Ratanasak Takumi Murata Taishin Adachi Prof. Jun-ya Hasegawa Prof. Tadashi Ema 《Chemistry (Weinheim an der Bergstrasse, Germany)》2022,28(58):e202202210
BPh3 catalyzes the N-methylation of secondary amines and the C-methylenation (methylene-bridge formation between aromatic rings) of N,N-dimethylanilines or 1-methylindoles in the presence of CO2 and PhSiH3; these reactions proceed at 30–40 °C under solvent-free conditions. In contrast, B(C6F5)3 shows little or no activity. 11B NMR spectra suggested the generation of [HBPh3]−. The detailed mechanism of the BPh3-catalyzed N-methylation of N-methylaniline ( 1 ) with CO2 and PhSiH3 was studied by using DFT calculations. BPh3 promotes the conversion of two substrates (N-methylaniline and CO2) into a zwitterionic carbamate to give three-component species [Ph(Me)(H)N+CO2−⋅⋅⋅BPh3]. The carbamate and BPh3 act as the nucleophile and Lewis acid, respectively, for the activation of PhSiH3 to generate [HBPh3]−, which is used to produce key CO2-derived species, such as silyl formate and bis(silyl)acetal, essential for the N-methylation of 1 . DFT calculations also suggested other mechanisms involving water for the generation of [HBPh3]− species. 相似文献
3.
Haruki Inoue Dr. Shin-ichi Naya Atsunobu Akita Dr. Hisashi Sugime Prof. Dr. Hiroaki Tada 《Chemistry (Weinheim an der Bergstrasse, Germany)》2022,28(46):e202201653
Gold nanoparticles with different mean sizes were formed on antimony-doped tin oxide nanocrystals by the temperature-varied deposition-precipitation method (Au/ATO NCs). Au/ATO NCs possess strong absorption in the near-infrared region due to Drude excitation in addition to the localized surface plasmon resonance (LSPR) of AuNPs around 530 nm. Au/ATO NCs show thermally activated catalytic activity for the oxidation of cinnamyl alcohol to cinnamaldehyde by hydrogen peroxide. The catalytic activity increases with a decrease in the mean Au particle size (dAu) at 5.3 nm≤dAu≤8.2 nm. Light irradiation (λex >660 nm, ∼0.5 sun) of Au/ATO NCs increases the rate of reaction by more than twice with ∼95 % selectivity. Kinetic analyses indicated that the striking enhancement of the reaction stems from the rise in the temperature near the catalyst surface of ∼30 K due to the photothermal effect of the ATO NCs. 相似文献
4.
In this work, a vanillin complex is immobilized onto MCM-41 and characterized by FT-IR, X-ray diffraction, scanning electron microscopy, energy dispersive spectroscopy, thermogravimetric analysis, and BET techniques. This supported Schiff base complex was found to be an efficient and recoverable catalyst for the chemoselective oxidation of sulfides into sulfoxides and thiols into their corresponding disulfides (using hydrogen peroxide as a green oxidant) and also a suitable catalyst for the preparation of 2,3-dihydroquinazolin-4(1H)-one derivatives in water at 90°C. Using this protocol, we show that a variety of disulfides, sulfoxides, and 2,3-dihydroquinazolin-4(1H)-one derivatives can be synthesized in green conditions. The catalyst can be recovered and recycled for further reactions without appreciable loss of catalytic performance. 相似文献
5.
In this reports the facile and green synthesis of rutile-type titanium dioxide nanoparticles decorated graphene oxide nanocomposite via the ultrasonication process (frequency: 50 kHz, Power: 100 W/cm2 and Ultrasonic type: Ti-horn). Because, the sonochemical synthesis method is simple, non-explosive and harmless method than other conventional technique. Furthermore, the synthesized material was characterized by various analytical techniques including FESEM, EDX, XRD, EIS and electrochemical methods. Then, the synthesized TiO2 MPs@GOS composite was applied for the electrocatalytic detection of theophylline (TPL) using CV and amperometric (current-time) techniques. Captivatingly, the modified sensor has excellent electrocatalytic performance with the wider linear range from 0.02 to 209.6 µM towards the determination of theophylline and the LOD and sensitivity of the modified sensor was calculated as 13.26 nM and 1.183 μA·µM−1·cm−2, respectively. In addition, a selectivity, reproducibility and stability of the TiO2 MPs@GOS modified GCE were analyzed towards the determination of theophylline molecule. Finally, the real time application of TiO2 MPs@GOS modified theophylline sensor was established in serum and drug samples. 相似文献
6.
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
7.
8.
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
9.
基于单相流体的概念,超临界流体的异常传热行为已经被研究很多年了,但是关于其流动传热机理仍没有统一的认识.本文通过理论分析和实验研究了超临界二氧化碳在竖直管内向上流动过程中,浮升力和流动加速效应对其流动结构和传热过程的影响.结果表明,没有确凿的实验证据表明超临界流体的异常传热行为是浮升力和流动加速直接导致的,存在的估计浮升力和流动加速效应准则均是在常物性流体的基础上,做了大量假设得出的,不同的研究者采用浮升力和流动加速准则分析超临界流体的传热恶化得出的结论不一致.最后,基于拟沸腾理论分析超临界流体的传热恶化过程,提出超临界沸腾数区分了超临界流体正常传热与恶化传热的转换边界,为超临界流体流动传热研究提供新思路,超临界沸腾数对建立用于不同技术的超临界流体动力循环的最佳运行条件具有重要意义. 相似文献
10.
Following a thermal reduction method, platinum nanoparticles were synthesized and stabilized by polyvinylpyrrolidone. The colloidal platinum nanoparticles were stable for more than 3 months. The micrograph analysis unveiled that the colloidal platinum nanoparticles were well dispersed with an average size of 2.53 nm. The sol–gel‐based inverse micelle strategy was applied to synthesize mesoporous iron oxide material. The colloidal platinum nanoparticles were deposited on mesoporous iron oxide through the capillary inclusion method. The small‐angle X‐ray scattering analysis indicated that the dimension of platinum nanoparticles deposited on mesoporous iron oxide (Pt‐Fe2O3) was 2.64 nm. X‐ray photoelectron spectroscopy (XPS) data showed that the binding energy on Pt‐Fe2O3 surface decreased owing to mesoporous support–nanoparticle interaction. Both colloidal and deposited platinum nanocatalysts improved the degradation of methyl orange under reduction conditions. The activation energy on the deposited platinum nanocatalyst interface (2.66 kJ mol?1) was significantly lowered compared with the one on the colloidal platinum nanocatalyst interface (40.63 ± 0.53 kJ mol?1). 相似文献