Latest ArticlesActivation of (bi)sulfite (S(Ⅳ)) by metal oxides is strongly limited by low electrons utilization. In this study, two carbon-supported cobalt ferrites spinels (CoFe2O4 QDs-GO and CoFe2O4 MOFs-CNTs) have been successfully synthesized by one-step solvothermal method. It was found that both catalysts could efficiently activate S(Ⅳ), with rapid reductive dechlorination and then oxidative degradation of a recalcitrant antibiotic chloramphenicol (CAP). Characterizations revealed that CoFe2O4 spinels were tightly coated on the carbon bases (GO and CNTs), with effectiveness of the internal transfer of electrons. O2˙− was identified for the reductive dechlorination of CAP, with simultaneously detection of both •OH and SO4˙− responsible for further oxidative degradation. The sulfur oxygen radical conversion reactions and molecular oxygen activation would occur together upon the carbon-based spinels. Spatial-separated interfacial reductive-oxidation of CAP would occur with dechlorination of CAP by O2˙− on the carbon bases, and oxidative degradation of intermediates by SO4˙−/•OH upon the CoFe2O4 catalysts.
Iron-chromium redox flow batteries (ICRFBs) possess advantages of high safety, long cycle time, and low-cost. Increasing Cr3+/Cr2+ reaction activity is suggested as one of the most promising strategies to improve the performance and prolong the lifetime of ICRFBs. To improve the slow reaction kinetics of the negative electrode, a type of defected carbon cloth with Bismuth (Bi) catalyst introduction is prepared by defect engineering method and electrochemical deposition, which provided defect sites and active sites to catalyze the redox couple's reaction of ICRFBs. Furthermore, this modified carbon cloth adsorbs Cr(Ⅲ) hydrate more easily, which has a more stable structure and can significantly improve the performance of ICRFBs. Both experimental analysis and theoretical calculation indicated that the modified electrode has excellent electrocatalytic ability, which can enhance the reaction rate of Cr3+/Cr2+, improve capacity retention and stabilize cycling performance. The capacity degradation rate of an ICRFB single cell with the modified electrodes is just 0.23% per cycle at a current density of 140 mA/cm2. Additionally, the energy efficiency (EE) remains around 83%, which is 8.45% higher than that of the pristine electrode assembled battery under 60 cycles. This work supplies a simple method to obtain a high-performance electrode material for ICRFBs and makes it a practical solution to promote ICFRBs large-scale commercialization process.
Catalyzed by cerium ammonium nitrate (CAN), the oxidative cracking reaction of alkenes occurred to produce carbonyls in good yields under mild conditions. The reaction employed molecular oxygen (O2) as the safe and clean oxidant. The catalyst dosage was reduced to as low as 0.5 mol%, while no additive was required. Thus, it may afford a generally green synthetic approach for introducing oxygen into organic molecules as well as the biomass degradation and the resource recycling from the C=C bond-containing waste polymers. X-ray photoelectron spectroscopy (XPS) analysis and control experiments demonstrated that the process proceeded via a single electron transfer (SET) reaction-initiated free radical reaction mechanism. In the process, both Ce and NO3− acted as the oxygen carrier to promote the oxidation reaction. The application of the abundantly existed nitrate in CAN was found to be the key for reducing the catalyst loading.
Nonfullerene acceptors (NFAs), which usually possess symmetric skeletons, have drawn great attention in recent years due to their pronounced advantages over the fullerene counterparts. Moreover, breaking the symmetry of NFAs could fine tune the molecular dipole, solubility, energy level, intermolecular interaction, molecular packing, crystallinity, etc., and give rise to improved photovoltaic performance. Currently, there are three main strategies for the design of asymmetric NFAs. This review highlights the recent advances of high-performance asymmetric NFAs and briefly outlooks the materials exploration for the future.
Visible-light heterogeneous photocatalyst with high activity and selectivity is crucial for the development of organic transformations, but remains a formidable challenge. Herein, a simple and effective strategy was developed to integrate tetrazine moiety, a visible light active unit, into robust metal-organic frameworks (2D MOF-1(M), M = Co, Mn, Zn, and 3D MOF-2(Co)). MOF-1 series are isomorphous 2D porous frameworks, and MOF-2(Co) displays 3D porous framework. Interestingly, benefiting from the oxidative active species of O2•−, these MOFs all exhibit obviously highly enhanced photocatalytic activities toward the straightforward condensation of o-aminothiophenol and aromatic aldehydes at room temperature in EtOH under visible-white-light irradiation. Notably, compared to 3D MOF, the 2D layered MOF-1(Co) exhibited more excellent catalytic activity with a wide range of substrates possessing preeminent tolerance of steric hindrance. Most impressively, MOF-1(Co) can be recycled at least five times without significant loss of catalytic activity or crystallinity, exhibiting excellent stability and reusability. This study sheds light on the wide-ranging prospects of visible light active 2D MOFs as green photocatalysts for the preparation of fine chemicals.
Compartmentalization in the biological world brings excellent efficiency and specificity to the formation of complex compounds, inspiring supramolecular chemists to continuously search for defined spaces that can mimic such natural binding sites. Bowl-shaped cavitands built up from resorcinarenes (RA) present rigid and preorganized concave surfaces, which are capable of mimicking the molecular recognition properties of enzymes. The versatile scaffold of RA endows the cavitand with terrific variety and excellent binding behavior. This review provides a comprehensive overview over the structural modification to date in the high attention field of RA-based cavitands development. Different strategies for synthesizing diverse cavitands, such as small cavity cavitands, wider cavity cavitands, deep cavity cavitands, biscavitands, and asymmetric cavitands, are discussed in details. Furthermore, insights into their applications including catalysis, separations and sensing are provided.
It is established that monitoring blood glucose on a daily basis is one of the most effective solutions to prevent and treat diabetes. Consequently, developing a glucose sensing platform with outstanding sensing performance occupies an indispensable position for the early diagnosis and risk assessment of diabetes. Recently, biosensor has been deemed as a promising apparatus to acquire the signals for glucose monitoring based on 2D materials. However, it is unsatisfied to deploy some materials widely as a result of some inherent defects. Carbon nanotubes have comparatively high toxicity. MoS2 with unfavourable biocompatibility are still arduously implemented on being functionalized. Fortunately, MXene, a brand-new and rapidly developing two-dimensional material, exhibits marvellous application potential in the domain of biosensing. Therefore, it has exerted tremendous attention from diverse scientific fields owning to its remarkable properties, such as excellent hydrophilicity, metal-like conductivity, abundant surface functional groups, unique layered structure, large specific surface area and remarkable biocompatibility. This review mainly focuses on the main synthetic route of MXenes, as well as the recent advancements of biosensors involving MXenes as an electrode modifier for glucose detection. In addition, the promising prospects and challenges of glucose sensing technology based on MXenes are also discussed.
Uncontrolled microglial activation is decisively involved in the neuroinflammatory pathogenesis of brain diseases. Consequently, suppression of microglial overactivation appears to be a strategy for the prevention of nerve injury. In this paper, a novel vanadium complex, vanadyl N-(p-N,N-dimethylaminophenylcarbamoylmethyl)iminodiacetate (VO(p-dmada)), was synthesized from vanadyl sulfate and N,N-dimethyl-p-phenylenediamine, which was structurally characterized by Fourier transform infrared spectrum and ESI-MS analysis. The effect of VO(p-dmada) on neuroinflammation was investigated by using the models of lipopolysaccharide (LPS)-induced BV2 microglial cells and BALB/c mice. Our data demonstrated that VO(p-dmada) significantly suppressed microglial activation by downregulating inflammatory mediators and associated proteins, and inactivating nuclear factor-κB (NF-κB) signaling pathway. VO(p-dmada) also upregulated peroxisome proliferator activated receptor gamma (PPARγ) by reducing transglutaminase 2 and heat shock protein 60 expression. Co-treatment with PPARγ antagonist GW9662 significantly impeded the inhibitory effect of VO(p-dmada) on LPS-induced neuroinflammation. These cumulative findings demonstrated that VO(p-dmada) is a potential new drug for the treatment of neuroinflammation-related neurodegenerative diseases.
As one of the 2D transition metal sulfides, 1T phase MoS2 nanosheets (NSs) have been studied because of their distinguished conductivity and suitable electronic structure. Nevertheless, the active sites are limited to a small number of edge sites only, while the basal plane is catalytically inert. Herein, we report that boron (B) doped 1T phase MoS2 NSs can replace precious metals as a co-catalyst to assist in photocatalytic H2 production of 2D layered g-C3N4 nanosheets (g-C3N4 NSs). The H2 evolution rate of prepared B-MoS2@g-C3N4 composites with 15 wt% B-MoS2 (B-MoS2@g-C3N4–15, 1612.75 µmol h−1 g−1) is 52.33 times of pure g-C3N4 NSs (30.82 µmol h−1 g−1). Furthermore, the apparent quantum efficiency (AQE) of B-MoS2@g-C3N4–15 composites under the light at λ = 370 nm is calculated and reaches 5.54%. The excellent photocatalytic performance of B-MoS2@g-C3N4–15 composites is attributed to the B ions doping inducing the distortion of 1T phase MoS2 crystal, which can activate more base planes to offer more active sites for H2 evolution reaction (HER). This work of B-MoS2@g-C3N4 composites offers experience in the progress of effective and low-price photocatalysts for HER.
In recent years, vanadate has attracted the attention of researchers for its application in electrode materials due to its high specific capacity and layered crystal structure. Herein, a typical manganese vanadium oxides (MnV2O6) product is efficient synthesis via a simple one-step hydrothermal method at 200 ℃ for 16 h. The as-prepared MnV2O6 sample is found to be the unique one-dimensional fan-like superstructure consist of several nanorods. From a microcosmic point of view, VO6 octahedra sheets are connected by sharing edges which provides highly-open framework for rapid the intercalation and deintercalation of guest ions Therefore, stable MnV2O6 was prepared and used as a cathode material in aqueous zinc ion batteries, which displayed favorable specific discharge capacity, excellent coulombic efficiency and well cycling performance.