Wacker oxidation is an industry-adopted process to transform olefins into value-added epoxides and carbonyls. However, traditional Wacker oxidation involves the use of homogeneous palladium and copper catalysts for the olefin addition and reductive elimination. Here, we demonstrated an ultrahigh loading Cu single atom catalyst(14% Cu, mass fraction) for the palladium-free Wacker oxidation of 4-vinylanisole into the corresponding ketone with N-methylhydroxylamine hydrochloride as an additive under mild conditions. Mechanistic studies by 18O and deuterium isotope labelling revealed a hydrogen shift mechanism in this palladium-free process using N-methylhydroxylamine hydrochloride as the oxygen source. The reaction scope can be further extended to Kucherov oxidation. Our study paves the way to replace noble metal catalysts in the traditional homogeneous processes with single atom catalysts. 相似文献
The oxygen reduction reaction in direct glycol fuel cells heavily relies on noble metal-based electrocatalysts. In this work, novel Pt group metal-free catalysts based on porous Fe-N-C materials are successfully synthesized as catalysts with high activity and durability for the cathode oxygen reduction reaction (ORR). Through the encapsulation of NH4SCN salt, the surface elements and pore structure of the catalyst are effectively changed, and the active sites of Fe effectively are increased. The half-wave potential of the best Fe-N-C catalyst was –0.02 V vs. Hg/HgO in an alkaline environment. The porous Fe-N-C catalyst possesses a large specific surface area(1158 m2/g) and shows good activity and tolerance to glycol. The direct glycol fuel cell with the Fe-N-C cathode achieved a maximum power density of 62.2 mW/cm2 with 4 mol/L KOH and 4 mol/L glycol solution at 25 °C and maintained discharge for more than 250 h at a 50 A/cm2 current density. 相似文献
Journal of Solid State Electrochemistry - Long-cycle stability and high-energy density are big challenges for developing high-performance hybrid supercapacitor (HSC) electrode materials. In this... 相似文献
In this work, we developed and validated a highly sensitive, rapid and stable LC–MS/MS method for the determination of ibuprofen in human plasma with ibuprofen-d3 as a stable isotopically labeled internal standard (SIL-IS). Human plasma samples were prepared by one-step protein precipitation. The chromatographic separation was achieved on a Poroshell 120 EC-C18 (2.1 × 50 mm, 2.7 μm). Aqueous solution (containing 0.05% acetic acid and 5 mm NH4Ac) and methanol were selected as the mobile phase with gradient elution. An electrospray ionization source was applied and operated in negative ion mode. Multiple reaction monitoring mode was used for quantification using target fragment ions m/z 205.0 → 161.1 for ibuprofen and m/z 208.0 → 164.0 for SIL-IS, respectively. This method exhibited a linear range of 0.05–36 μg/ml for ibuprofen with correlation coefficient >0.99. Mean recoveries of ibuprofen in human plasma ranged from 78.4 to 80.9%. The RSD of intra- and inter-day precision were both < 5%. The accuracy was between 88.2 and 103.67%. The matrix effect was negligible in human plasma, including lipidemia and hemolytic plasma. A simple, efficient and accurate LC–MS/MS method was successfully established and applied to a pharmacokinetic study in healthy Chinese volunteers after a single oral administration of ibuprofen granules. 相似文献
Two-dimensional carbon nitride(2 D-C3 N4)nanosheets are promising materials in photocatalytic water splitting,but still suffer from easy agglomeration and fast photogene rated electron-hole pairs recombination.To tackle this issue,herein,a hierarchical Nb2 O5/2 D-C3 N4 heterostructure is precisely constructed and the built-in electric field between Nb2O5 and 2 D-C3 N4 can provide the driving force to separate/transfer the charge carriers efficiently.Moreover,the strongly Lewis acidic Nb2O5 can adsorb TEOA molecules on its surface at locally high concentrations to facilitate the oxidation reaction kinetics under irradiation,resulting in efficient photogene rated electrons-holes separation and exceptional photocatalytic hydrogen evolution.As expected,the champion Nb2O5/2 D-C3N4 heterostructure achieves an exceptional H2 evolution rate of 31.6 mmol g-1 h-1,which is 213.6 times and 4.3 times higher than that of pristine Nb2O5 and2 D-C3N4,respectively.Moreover,the champion heterostructure possesses a high apparent quantum efficiency(AQE)of 45.08%atλ=405 nm and superior cycling stability.Furthermore,a possible photocatalytic mechanism of the energy band alignment at the hetero-interface is proposed based on the systematical characterizations accompanied by density functional theory(DFT)calculations.This work paves the way for the precise construction of a high-quality heterostructured photocatalyst with efficient charge separation to boost hydrogen production. 相似文献
Zinc molybdate (ZnMoO4), a layer perovskite material, has the advantages of high stability, excellent optical and charge properties. However, its high band gap and high electron–hole recombination efficiency limit its application in the photocatalytic reduction field like hydrogen production. In this study, we used CdS as a co-catalyst and successfully prepared CdS/ZnMoO4 composite photocatalysts with different loadings. The hydrogen evolution rate of CdS/ZnMoO4 reached 530.2 µmol h?1 g?1, which was approximately 11 and 100 times more than rates of pure CdS and ZnMoO4 under the same conditions, respectively. It is the presence of CdS that contributed to this improved performance, which acted as an electron acceptor to separate electrons and holes. Besides, a reasonable mechanism was provided based on photoelectrochemical characterizations. CdS loading greatly improved the hydrogen evolution performance of ZnMoO4 under visible light, providing a direction to improving the performance of perovskite based photocatalysts.
Cellulose - There has been significant interest over recent years in the production and application of sustainable and green materials. Among these, nanocellulose has incurred great interest... 相似文献
Cellulose - Heating is essential in various biomass pre-treatments and thermal conversion processes. It is of practical significance to study the characteristics of cellulose-lignin and... 相似文献
As a special subset of calix[4]arene, calix[4]resorcinarene is an excellent molecular platform which could be modified by introducing functional groups to multiple sites at the upper and lower rims. There are mainly three ways to build functionalized calix[4]resorcinarene derivatives: (1) modification on the C-2 sites of calix[4]resorcinarenes; (2) modification on the phenolic hydroxyl groups of calix[4]resorcinarenes; (3) modification on the bridging methylenes at lower rim of calix[4]resorcinarenes. Functionalized calix[4]resorcinarene derivatives play an important role in the development of self-assembly chemistry, among which hydrogen bonding and metal coordination are the two most common interactions to obtain multicomponent structures. Moreover, due to the excellent topological structures and various active substituents of functionalized calix[4]resorcinarene derivatives, their applications in various fields, such as nanoparticles, catalysts, fluorescent materials, and sensors, have been briefly presented in this paper.
The electrochemical CO2 reduction (CO2RR) is a sustainable approach to mitigate the increased CO2 emissions and simultaneously produce value-added chemicals and fuels. Metal-nitrogen-carbon (M-N-C) based single-atom catalysts (SACs) have emerged as promising electrocatalysts for CO2RR with high activity, selectivity, and stability. To design efficient SACs for CO2RR, the key influence factors need to be understood. Here, we summarize recent achievements on M-N-C SACs for CO2RR and highlight the significance of the key constituting factors, metal sites, the coordination environment, and the substrates, for achieving high CO2RR performance. The perspective views and guidelines are provided for the future direction of developing M-N-C SACs as CO2RR catalysts. 相似文献