Latest ArticlesConversion of methane into liquid alcohol such as ethanol at low temperature in a straight, selective and low energy consumption process remains a topic of intense scientific research but a great challenge. In this work, CuFe2O4/CNT composite is successfully synthesized via a facile co-reduction method and used as catalysts to selectively oxidize methane. At a low temperature of 150 ℃, methane is directly converted to ethanol in a single process on the as-prepared CuFe2O4/CNT composite with high selectivity. A mechanism is also proposed for the significant methane selective oxidation performance of the CuFe2O4/CNT composite catalysts.
Porous carbon materials have attracted much attention in the field of organic synthesis in recent years, due to their tunable properties, excellent catalytic activity and stability. Biomass-based carbohydrates emerge as an ideal precursor for the generation of these materials owing to their renewability, low cost, non-toxicity and high content of functional groups. Thus, carbon materials prepared from carbohydrates is of considerable importance for the sustainable development of organic chemistry. The present review not only summarizes recent examples of carbohydrate-derived porous carbon material-catalyzed organic reactions including the oxidation, hydrogenation, cross-coupling, esterification and condensation reactions, but also introduces the preparation and functionalization strategies of these materials. Furthermore, the challenges and opportunities of organic synthesis over these sustainable materials have also been addressed. This review will stimulate further research on exploring novel carbohydrate-derived porous carbon materials and new sustainable organic synthetic processes over these materials.
Surface oxygen vacancy defects of mesoporous CeO2 nanosheets assembled microspheres (D-CeO2) are engineered by polymer precipitation, hydrothermal and surface hydrogenation strategies. The resultant D-CeO2 with a main pore diameter of 9.3 nm has a large specific surface area (~102.3 m2/g) and high thermal stability. The mesoporous nanosheets assembled microsphere structure prevents the nanosheets from aggregation, which is beneficial to effective mass transfer and shortens the migration distance of charge carriers. After surface hydrogenation, the photoresponse extends to long wavelength region, combing with the band gap from 2.63 eV reduced to 2.39 eV. Under AM 1.5 G radiation, the photocatalytic degradation rate of tetracycline (TC) can be up to 99.99%, which is three times as high as that of pristine CeO2 microspheres. The excellent solar-driven photocatalytic performance can be attributed to the efficient surface oxygen vacancy engineering and the mesoporous nanosheets assembled microsphere structure, which narrows the band gap, shortens the migration distance of carriers, promotes the spatial separation of photogenerated electron-hole pairs and favors mass transfer. The strategy provides new insights for fabricating other high-efficient oxide photocatalysts.
Explore the photo-piezoelectric synergistic micro-mechanism by density functional theory (DFT) calculations at the electronic and atomic level is important. In this work, to understand the synergistic mechanism, atomic and electronic properties of typical piezoelectric and photocatalytic material BaTiO3 were initially investigated with different strains. Subsequently, the adsorption of volatile organic compounds (VOCs) on the BaTiO3 (001) surface was determined during the piezoelectric process. In addition, the relationship between deformation ratio, the electronic structure and adsorption energy was understood in the deformation ratio range of 7%-12% for the optimal catalytic effect. The results of charge density differences and Born effective charge reveal the synergistic mechanism of piezoelectric photocatalysis. The built-in electric field formed by polarization results in the enhanced separation of charges, which makes the surface charges aggregation, enhancing the adsorption of VOCs, and benefiting the subsequent photocatalytic degradation. This work can provide significant theoretical guidance for the piezoelectric photocatalytic degradation of pollutants with the optimal strain range.
A great concern has been raised regarding the issue of fluoroquinolones (FQs) in the environment. In this work, the transformation of FQs by commonly used oxidant permanganate (Mn(Ⅶ)) in the absence and presence of humic acid (HA), ubiquitously existing in aquatic environments, was systematically investigated. Here, the catalytic role of in-situ formed MnO2 on Mn(Ⅶ) oxidation of FQs depending on solution pH and co-existing substrates was firstly reported. It was interestingly found that HA could appreciably accelerate FQs degradation by Mn(Ⅶ) at environmentally relevant pH. HA as a reductant in accelerating FQs by Mn(Ⅶ) oxidation was distinctly elucidated for the first time, where MnO2 in situ formed from the reduction of Mn(Ⅶ) by HA served as a catalyst. Similar products were observed in the presence versus absence of HA. Considering that the accelerating role of HA was related to its reducing ability, an activation method based on Mn(Ⅶ) and reductant (i.e., Fe(Ⅱ), Mn(Ⅱ) and (bi)sulfite) was proposed, which exhibited considerable potential for application in the treatment of FQs contaminated water.
(±)-Pyriindolin (1) with a rare molecular backbone formed by fusing a 2, 2′-bipyridine nucleus into a spiro[furan-3, 3′-indoline] skeleton, was isolated from the Streptomyces albolongus EA12432. The constitution and the relative configuration of (±)-1 were determined by extensive spectroscopic analyses, 13C calculation and DP4+ probability analysis. The absolute configurations of optically pure (+)-1 and (−)-1 which were obtained after a chiral high performance liquid chromatography (HPLC) separation were further identified by electronic circular dichroism (ECD) calculations. (+)- and (−)-Pyriindolins displayed moderate cytotoxicity against HCT-116 cell line with the half-maximal inhibitory concentration (IC50) values of 2.89 ± 0.17 µmol/L and 4.47 ± 0.26 µmol/L, respectively.
Sodium (Na) O2 batteries have high energy density and low cost. However, high polarization, complex discharge products, and low Coulombic efficiency (CE) lead to poor cyclability. Here, we proposed an atomically dispersed Ru catalyst on nitrogen-doped graphene for Na-O2 batteries. The catalysts enable the discharge to proceed via a surface-mediated route, which leads to uniform deposition of Na2-xO2 and low polarization during recharge. The first-principle calculation revealed that Ru-N4 complex in the catalyst has strong chemical adsorption to intermediate superoxides, facilitating uniform deposition and enhancing rapid kinetics. In contrast, Ru nanoparticles, despite the catalytic activity, induce bulk deposition via a solution-mediated route because the exposed graphene surface shows weak interaction to superoxides, thereby lowering CEs and cyclability. In brief, the atomically-dispersed Ru catalyst endows Na-O2 batteries with excellent electrochemical properties via a surface-mediated discharge.
With the in-depth research of sodium-ion batteries (SIBs), the development of novel sodium-ion anode material has become a top priority. In this work, tube cluster-shaped SbPS4 was synthesized by a high-temperature solid phase reaction. Then the typical short tubular ternary thiophosphate SbPS4 compounded with graphene oxide (SbPS4/GO) was successfully synthesized after ultrasonication and freeze-drying. SbPS4 shows a high theoretical specific capacity (1335 mAh/g) according to the conversion-alloying dual mechanisms. The unique short tube inserted in the spongy graphene structure of SbPS4/GO results in boosting the Na ions transport and alleviating the huge volume change in the charging and discharging processes, improving the sodium storage performance. Consequently, the tubular SbPS4 compounded with 10% GO provides an outstanding capacity of 359.58 mAh/g at 500 mA/g. The result indicates that SbPS4/GO anode has a promising application potential for SIBs.
Mineralization of the ZIF-8 in the presence of biomacromolecules has been demonstrated to be a general way for making bioentities@ZIFs composites. The ZIF-8 crystals permit controlled storage and utilization of the bioentities, thus can benefit drug delivery, cold-chain breaking etc. With the increasing needs on personal care and distributed manufacturing, automated synthesis controlled by a computer becomes the next challenge. In this work, we designed an automatic synthesis system to prepare PEG mineralized ZIF-8 composite particles. This system is based on flow chemistry with the microfluidic chips fabricated by femtosecond laser micromachining. The particles were synthesized and monitored automatically. Furthermore, this synthesizer could be extended for fabrication of vaccine particles under remote control through internet.
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