Latest ArticlesA novel N, O modified Mn3O4@porous carbon catalyst (NOC-Mn3O4) was prepared by direct carbonization using the manganese-metal organic framework (Mn-MOF) and covalent organic framework (COF) as precursors to activate peroxymonosulfate (PMS) for the degradation of bisphenol A (BPA) and rhodamine B (RhB). Benefiting from the N and O co-doping of COF, larger specific surface area, faster electron transfer and Mn cycling, the optimum 1NOC-Mn3O4 could significantly improve the degradation performance of BPA and RhB (92.1% and 96.9% within 30 min) as compared to C-Mn3O4 without COF doping. In addition, 1NOC-Mn3O4 showed good reusability and strong anti-interference ability. Radical quenching experiments, X-ray photoelectron spectroscopy (XPS), Electron paramagnetic resonance spectrometer (EPR) and electrochemical tests showed that the 1NOC-Mn3O4/PMS system degraded BPA and RhB by both radical and non-radical pathways. Moreover, the possible degradation pathways of BPA and RhB were proposed by liquid chromatography-mass spectrometry (LC-MS). Except for that, the toxicity of BPA, RhB and their intermediates were evaluated. This study opens up a new prospect for the design of COF-doped PMS catalysts.
Photocatalytic conversion of CO2 into small-molecule chemical feedstocks can meet the growing demand for energy and alleviate the global warming. Herein, a p-n ZnO@CDs@Co3O4 heterojunction with sandwich structure was constructed by calcination method of self-assembled ZIF-8@CDs@ZIF-67. The ZnO@CDs@Co3O4 with well-defined interfacial structure exhibited the significantly enhanced photocatalytic CO2 reduction activity, and the optimal catalyst indicated the (CO + CH4) evolution rate of 214.53 µmol g−1 h−1 under simulated solar light, which was superior to ZnO, Co3O4 and binary ZnO@Co3O4. The internal cavity, exposed active sites, multiple interfaces and constructed p-n heterojunction can facilitate the light harvesting and photoexcited electron transfer. Besides, after introduction of CDs placed in the middle layer between ZnO and Co3O4, CDs with excellent photoelectric property further promoted charge separation and migration. This work represents an appealing strategy to construct well-defined photocatalysts for boosting CO2 photoreduction.
There is a close relationship between the biological functions of lipids and their structures, and various isomers greatly increases the complexity of lipid structures. The C=C bond location and sn-position are two of the essential attributes that determine the structures of unsaturated lipids. However, simultaneous identification of both attributes remains challenging. Here, we develop a visible-light-activated aziridination reaction system, which enables the dual-resolving of the C=C bond location and sn-position isomerism of in lipids when combines with liquid chromatography-mass spectrometry (LC-MS). Based on the derivatization of C=C bonds with PhI=NTs, their location in lipids could be easily identified by tandem MS. Especially, the sn-position isomers of unsaturated phosphatidylcholine (PC) can be separated and quantified by LC-MS after the derivatization. By using the proposed method, the significant changes of the sn-position isomers ratios of PC in mouse brain ischemia were revealed. This study offers a powerful tool for deep lipid structural biology.
A facile TfOH-catalyzed oxidative cyclization of allyl compounds and isocyanide has been developed with the assistance of DDQ, where isocyanide is used as the crucial "N" and "CN" sources. Highly functionalized 2-cyanopyrroles are constructed efficiently through a new formal [3 + 2] mode, demonstrating diverse reactivity and synthetic utility in organic chemistry. 2-Cyanopyrrole is converted into a nucleobase analogue of Remdesivir and 5H-pyrrolo[2, 1-a]isoindole through a three-step or a two-step sequence, respectively. This protocol features broad substrate scope, operational simplicity and good functional group tolerance.
Electrochemical conversion of nitrate (NO3−) to ammonia (NH3) can target two birds with one stone well, in NO3−-containing sewage remediation and sustainable NH3 production. However, single metal-based catalysts are difficult to drive high-efficient NO3− removal due to the multi-electron transfer steps. Herein, we present a tandem catalyst with simple structure, Cu-Co binary metal oxides (Cu-Co-O), by engineering intermediate phases as catalytic active species for NO3− conversion. Electrochemical evaluation, X-ray photoelectron spectroscopy, and in situ Raman spectra together suggest that the newly-generated Cu-based phases was prone to NO3− to NO2− conversion, then NO2− was reduced to NH3 on Co-based species. At an applied potential of −1.1 V vs. saturated calomel electrode, the Cu-Co-O catalyst achieved NO3−-N removal of 90% and NH3 faradaic efficiency of 81% for 120 min in 100 mL of 50 mg/L NO3−-N, consuming only 0.69 kWh/mol in a two-electrode system. This study provides a facile and efficient engineering strategy for developing high-performance catalysts for electrocatalytic nitrate conversion.
In an era where the concept of green development is deeply rooted, magnesium (Mg) alloy as a light metal has a long-term development prospect in the process of energy saving, emission reduction and environmental improvement. However, anti-corrosion performance of Mg alloy is poor due to the high chemical activity and low equilibrium potential, which limits the development of Mg alloy products. Herein, three-dimensional mesopore hollow polypyrrole spheres (MHPS) were prepared, and the MHPS was inserted into the middle of the stacked hexagon boron nitride (h-BN) lamellae, which allowed the h-BN to be separated forming a further composite with abundant pore structure. Subsequently, the MHPS/h-BN-OH composite was uniformly sprayed on the Mg alloy surface via simple spraying method to form the superhydrophobic surface (SHS). Finally, the slippery liquid infused porous surface (SLIPS) was successfully fabricated by applying drops of silicone lubricant on the superhydrophobic coating surface. After a series of characterization and testing, the results showed that the stacking of h-BN lamellae was significantly reduced after h-BN was successfully embedded by MHPS. In addition, the fabricated SLIPS have excellent self-cleaning, mechanical stability, anti-icing and anti-corrosion properties. Therefore, the method of embedding polymer microspheres not only offers a new strategy for h-BN exfoliation, but also the successful prepared SLIPS largely retards the corrosion of Mg alloy while providing new ideas for the development of SLIPS.
In this work, we designed and synthesized cationic carbon dots (CDs) with a size distribution of 1.6–3.7 nm, which exhibited dark blue fluorescence in the aqueous solution. Based on its excellent luminescence properties, we used it as an energy donor to construct a sequential artificial light-harvesting system (LHS) by employing the energy-matching dyes eosin Y disodium salt (EY) and sulforhodamine 101 (SR101), which could regulate the white light emission (Commission Internationale de lʼEclairage (CIE) coordinate: (0.30, 0.31)) with the energy transfer efficiency (ΦET) of 53.9% and 20.0%. Moreover, a single-step artificial LHS with white light emission (0.32, 0.28) can be constructed directly using CDs and dye solvent 43 (SR) with ΦET and antenna effect (AE) of 48.8% and 6.5, respectively. More importantly, CDs-based artificial LHSs were firstly used in photocatalytic of α-bromoacetophenone, with a yield of 90%. This work not only provides a new strategy for constructing CDs-based LHSs, but also opens up a new application for further applying the energy harvested in CDs-based LHSs to the field of the aqueous solution photocatalysis.
Mesoporous titanium nanoparticles (MTNs) have emerged as an important porous semiconductor owning to their large surface area and unique electronic/optical properties. However, the fundamental research for rational manufacturing MTNs in a highly scalable manner remains a challenge. In this study, we report a two-step flash nanocomplexation (FNC) approach to large-scalable generate MTNs through the sequential combination of two multi-inlet vortex mixers. By optimizing the concentrated titanium precursor, polyethylene glycol (PEG)-functionalized silane amount and pH, we have been able to produce MTNs with small particle size (31.5 nm), larger surface area (416.9 m²/g) and pore volume (0.59 cm3/g). Different from the traditional MTNs bulk, FNC-produced MTNs exhibited well-controlled manner and exceptional photocatalytic and antibacterial properties. Importantly, the optimized MTNs outperformed commercial P25 not only in protecting ultraviolet A (UVA)-exposed skin, but also in treating P. aeruginosa-infected wound. We believe that the high controllability and scalability of sequential flash nanocomplexation method offers great opportunities in enhancing the performance of mesoporous titanium nanoparticles.
Selective molecular recognition in water is routine for bioreceptors, but remains challenging for synthetic hosts. This is principally because noncovalent interactions are usually less efficient in aqueous environments. By mimicking the cavity feature of bioreceptors, Prof. Wei Jiang proposed and clarified the concept of "endo-functionalized cavity". Through situating polar binding sites into a deep hydrophobic cavity, we designed and synthesized several macrocyclic hosts, among which amide naphthotubes are the most representative. The hosts can selectively recognize various polar molecules including organic micropollutants, drug molecules, and chiral molecules in water by employing the hydrophobic effect and shielded hydrogen bonding. In addition, these biomimetic hosts have been applied in spectroscopic analysis, adsorptive separation and self-assembly. In this review, we provide an overview of recent advances on amide naphthotubes with special emphasis on the efforts of Jiang's group. We are convinced that these biomimetic macrocycles will make further contributions to supramolecular chemistry and beyond.
Organic semiconductor single crystals (OSSCs) have shown their promising potential in high-performance organic field-effect transistors (OFETs). The interfacial dielectric layers are critical in these OFETs as they not only govern the key semiconductor/dielectric interface quality but also determine the growth of OSSCs by their wetting properties. However, reported interfacial dielectric layers either need rigorous preparation processes, rely on certain surface chemistry reactions, or exhibit poor solvent resistance, which limits their applications in low-cost, large-area, monolithic fabrication of OSSC-based OFETs. In this work, polyethylene (PE) thin films and lamellar single crystals are utilized as the interfacial dielectric layers, providing solvent resistive but wettable surfaces that facilitate the crystallization of 6,13-bis(tri-isopropylsilylethynyl)pentacene (TIPS-PEN) and 6,13-bis(triisopropylsilylethynyl)-5,7,12,14-tetraazapentacene (TIPS-TAP). As evidenced by the presence of ambipolar behavior in TIPS-PEN single crystals and the high electron mobility (2.3 ± 0.34 cm2 V-1 s-1) in TIPS-TAP single crystals, a general improvement on electron transport with PE interfacial dielectric layers is revealed, which likely associates with the chemically inertness of the saturated C-H bonds. With the advantages in both processing and device operation, the PE interfacial dielectric layer potentially offers a monolithic way for the enhancement of electron transport in solution-processed OSSC-based OFETs.
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