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11.
Electrocatalytic Carbon Dioxide Reduction by Using Cationic Pentamethylcyclopentadienyl–Iridium Complexes with Unsymmetrically Substituted Bipyridine Ligands 下载免费PDF全文
Fanni D. Sypaseuth Corinna Matlachowski Manuela Weber Dr. Matthias Schwalbe Prof. Dr. C. Christoph Tzschucke 《Chemistry (Weinheim an der Bergstrasse, Germany)》2015,21(17):6564-6571
Eight [Ir(bpy)Cp*Cl]+‐type complexes (bpy= bipyridine, Cp*=1,2,3,4,5‐pentamethylcyclopentadienyl) containing differently substituted bipyridine ligands were synthesized and characterized. Cyclic voltammetry (CV) of the complexes in Ar‐saturated acetonitrile solutions showed that the redox behavior of the complexes could be fine tuned by the electronic properties of the substituted bipyridine ligands. Further CV in CO2‐saturated MeCN/H2O (9:1, v/v) solutions showed catalytic currents for CO2 reduction. In controlled potential electrolysis experiments (MeCN/MeOH (1:1, v/v), Eapp=?1.80 V vs Ag/AgCl), all of the complexes showed moderate activity in the electrocatalytic reduction of CO2 with good stability over at least 15 hours. This electrocatalytic process was selective toward formic acid, with only traces of dihydrogen or carbon monoxide and occasionally formaldehyde as byproducts. However, the turnover frequencies and current efficiencies were quite low. No direct correlation between the redox potentials of the complexes and their catalytic activity was observed. 相似文献
12.
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
13.
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
14.
15.
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
16.
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
17.
Anna Pawlik Magdalena Jarosz Robert P. Socha Grzegorz D. Sulka 《Molecules (Basel, Switzerland)》2021,26(6)
In implantable materials, surface topography and chemistry are the most important in the effective osseointegration and interaction with drug molecules. Therefore, structural and surface modifications of nanostructured titanium dioxide (TiO2) layers are reported in the present work. In particular, the modification of annealed TiO2 samples with —OH groups and silane derivatives, confirmed by X-ray photoelectron spectroscopy, is shown. Moreover, the ibuprofen release process was studied regarding the desorption-desorption-diffusion (DDD) kinetic model. The results proved that the most significant impact on the release profile is annealing, and further surface modifications did not change its kinetics. Additionally, the cell adhesion and proliferation were examined based on the MTS test and immunofluorescent staining. The obtained data showed that the proposed changes in the surface chemistry enhance the samples’ hydrophilicity. Moreover, improvements in the adhesion and proliferation of the MG-63 cells were observed. 相似文献
18.
Helical carbon nanotubes currently cost ~15,000–19,000 USD/kg commercially and are ~10–15 times the price of straight carbon nanotubes of similar dimensions. They have not previously been made from the greenhouse gas CO2 nor had new variants of the helical morphology been demonstrated. In this study, a novel, inexpensive electrosynthesis of these helical nanocarbon materials from CO2 is presented. This material may be produced by molten carbon growth conditions that (1) maximize torsional stresses, such as those that may occur during rapid, nucleated carbon reduction, (2) enhance defects that cause formation of heptagonal, rather than the conventional hexagonal building blocks of graphene cylindrical walls, and (3) uniformly control those enhanced defects to repeatedly induce a uniform spiral conformation. These conditions are achieved with at least two of the following experimental conditions: (i) high electrolysis current density, (ii) sp3 defect-inducing agents, such as added oxide, and (iii) controlled concentration of iron added to the electrolyte or cathode. Here, it is shown with SEM, TEM, EDX, XRF, and Raman spectroscopy that a molten controlled electrolyte carbonate synthesis to induce defect formation, and a high rate of electrolysis (0.6 A/cm2) leads to a high yield of helical nanotubes, helical nanofibers, or helical nanoplatelet carbon morphologies. 相似文献
19.
Ding Tian Taliehsadat Alebrahim Gregory K. Kline Liwen Chen Haiqing Lin Chulsung Bae 《Journal of polymer science. Part A, Polymer chemistry》2020,58(18):2654-2663
Polymeric membrane-based gas separation technology has significant advantages compared with traditional amine-based CO2 separation method. In this work, SEBS block copolymer is used as a polymer matrix to incorporate triethylene oxide (TEO) functionality. The short ethylene oxide segment is chosen to avoid crystallization, which is confirmed by differential scanning calorimetry and wide-angle X-ray scattering characterizations. The gas permeability results reveal that CO2/N2 selectivity increased with increasing content of TEO functional group. The highest CO2 permeability (281 Barrer) and CO2/N2 selectivity (31) were obtained for the membrane with the highest TEO incorporation (57 mol%). Increasing the TEO content in these copolymers results in an increase in CO2 solubility and a decrease in C2H6 solubility. For example, as the grafted TEO content increased from 0 to 57 mol%, the CO2 solubility and CO2/C2H6 solubility selectivity increased from 0.72 to 1.3 cm3(STP)/cm3 atm and 0.47 to 1.3 at 35°C, respectively. The polar ether linkage in TEO-grafted SEBS copolymers exhibits favorable interaction with CO2 and unfavorable interaction with nonpolar C2H6, thus enhancing CO2/C2H6 solubility selectivity. 相似文献
20.
Dr. Francesco Della Monica Dr. Veronica Paradiso Prof. Dr. Alfonso Grassi Dr. Stefano Milione Prof. Dr. Luigi Cavallo Prof. Dr. Carmine Capacchione 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(24):5347-5353
A new chromium(III) complex, bearing a bis-thioether-diphenolate [OSSO]-type ligand, was found to be an efficient catalyst in the copolymerization of CO2 and epoxides to achieve poly(propylene carbonate), poly(cyclohexene carbonate), poly(hexene carbonate) and poly(styrene carbonate), as well as poly(propylene carbonate)(cyclohexene carbonate) and poly(propylene carbonate)(hexene carbonate) terpolymers. 相似文献