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N ′-phenylpicolinohydrazide has been proven to be a promising lead compound for research and development of novel fungicides for agriculture in our previous study. As our continuing research, in this study, a series of N -substituted derivatives of N ′-phenylpicolinohydrazide were synthesized and explored for the inhibition activity on nine phytopathogenic fungi and action mechanism. The results found that eleven of the compounds had excellent antifungal activity with more than 80% inhibition rates at 50 µ g/mL on part or most of the fungi, especially A. solani and P. piricola . Compounds 5i , 5j and 5k showed EC 50 values of < 8.0 µg/mL against A. solani superior to positive control carbendazim (EC 50 = 36.0 µg/mL) while 5p and 5q exhibited the highest activity with EC 50 values of 2.72 and 2.80 µg/mL against P. piricola superior to positive control boscalid (EC 50 > 50.0 µg/mL). Furthermore, 5k also showed significant protective effect against A. solani infection on tomatoes in a concentration-dependent manner. Action mechanism research showed that 5k was able to increase the intracellular ROS level, change both MMP and permeability of cell membrane and damage mycelial morphology. Molecular docking studies showed that 5k could bind into ubiquinone-binding region of succinate dehydrogenase by hydrogen bonds, π-cation, π–π stacked, π-alkyl, and alkyl interactions. Additionally, the antibacterial activity was also investigated. Thus, N -substituted derivatives of N ′-phenylpicolinohydrazide were emerged as novel and highly promising antifungal molecular skeletons to develop new fungicides for crop protection. Graphic abstract
The mechanistic understanding of how alkylamines impact Ni-metallophotoredox C–N coupling to form diarylamines remains unclear. In this study, 12-alkylamines were evaluated as additives to determine their effects on the synthesis of diarylamines in a flow photochemical system. Notably, n-hexylamine demonstrated the most significant promotional effect. Spectroscopic studies and experimental data reveal n-hexylamine substitutes DABCO as a Ni catalyst ligand, enhancing yields particularly in sterically hindered arylamines.
Samarium oxide (Sm2O3) is a promising electrolyte for low-temperature fuel cells but lacks further exploration of performance optimization. Herein, we propose an effective approach to strengthen the proton transport characteristics via constructing a heterostructure interface in a Sm2O3/ZnO composite electrolyte. The constructed optimal 6Sm2O3-4ZnO cell device yields an improved peak power density of 920 mW cm–2 and an extended durability performance of 45 h at 500 °C. Experiments confirm the proton conduction, and the density functional theory calculation further discloses the low proton migration energy of 0.35 eV. The semiconductor junction test and theoretical calculation both reveal that the heterojunction exists at the Sm2O3/ZnO interface. The strong local electric field strength of 1.53 × 107 V m–1 at the interface effectively suppresses short circuit and accelerates proton transport, leading to significantly enhanced electrochemical performance. This study indicates that the 6Sm2O3-4ZnO material is a promising electrolyte candidate for fuel cell application.
Chitosan bis(phenylcarbamate)-( N -cyclohexylformamide)s and chitosan bis(phenylcarbamate)-( N -hexanamide)s were synthesized as chiral selectors for enantiomeric separation. Since two types of substituents with different structures were, respectively, introduced onto the 2-position and the 3-/6-positions of the glucose skeleton in the chitosans through a “heterogeneous” modification pathway, the enantioseparation performances of the chiral selectors could be improved. Influence of the type and position of the substituents on chiral recognition and enantioseparation abilities was studied in detail, and the structural dependence on enantioseparation performance was particularly demonstrated. It was found that methyl- and chloro-substituted chitosan bis(phenylcarbamate)-( N -hexanamide)s possessed comparable enantioseparation performances, whereas chloro-substituted chitosan bis(phenylcarbamate)-( N -cyclohexylformamide)s exhibited much more powerful chiral recognition and enantioseparation abilities than the methyl-substituted ones. Among all the prepared chiral selectors, those with the combination of the cyclohexyl group at the 2-position of the glucose skeleton in the chitosan derivatives and the chlorophenyl group at the 3-/6-positions seemed to be more preferable for enantiomeric separation. As a result, the chitosan bis(3,4-dichlorophenylcarbamate)-( N -cyclohexylformamide) possessed the best enantioseparation performance. The solvent tolerability of the prepared chiral selectors was also investigated in the present study. Compared with the classical coated-type chiral separation materials derived from cellulose/amylose derivatives, the N -cyclohexylcarbonyl and N -hexanoyl chitosans based chiral stationary phases were observed to possess more favorable solvent tolerability, thus possibly widening their applications for various practical enantioseparations.
N-ethyl perfluorooctane sulfonamide (N-EtFOSA) is an important perfluorooctanesulfonate (PFOS) precursor (PreFOS) which is used in sulfluramid. The present work studied the uptake, translocation and metabolism of N-EtFOSA in wheat ( Triticum aestivum L.), soybean ( Glycine max L. Merrill) and pumpkin ( Cucurbita maxima L.) by hydroponic exposure. Except for parent N-EtFOSA, its metabolites of perfluorooctane sulfonamide acetate (FOSAA), perfluorooctane sulfonamide (PFOSA), PFOS, perfluorohexane sulfonate (PFHxS) and perfluorobutane sulfonate (PFBS) were detected in the roots and shoots of all the three plant species examined. This suggested that plant roots could take up N-EtFOSA from solutions efficiently, and translocate to shoots. A positive correlation was found between root concentration factors (RCFs) of N-EtFOSA and root lipid content. Much higher proportion of N-EtFOSA transformation products in plant tissues than in the solutions suggested that N-EtFOSA could be in vivo metabolized in plant roots and shoots to FOSAA, PFOSA and PFOS, and other additional shorter-chain perfluoroalkane sulfonates (PFSAs), including PFHxS and PFBS. The results suggested that plants had biotransformation pathways to N-EtFOSA that were different than those from microorganisms and animals. This study provides important information about the uptake and metabolism of PreFOSs in plants.
A flexible, tough, highly transparent and piezoelectric polyacrylamide hydrogel was fabricated induced by blue light photocuring, with camphorquinone/diphenyliodonium hexafluorophosphate (CQ/DPI) as the blue light initiator, acrylamide (AM) and N, N-dimethylacrylamide (DMAA) as monomers, polyethylene glycol diacrylate (PEGDA) as the crosslinker, lecithin as the dispersant, and BaTiO3 as the piezoelectric material. Various performance tests were carried out on the hydrogel, the results showed that lecithin enhances the dispersion of BaTiO3 within the system and improved the tensile properties (>100% strain) of the hydrogel, and the addition of PEGDA not only improves the photopolymerization performance of hydrogel, but also significantly improves its fracture strength (~ 0.3 MPa). In addition, BaTiO3 enables the result hydrogels show excellent conductivity (> 1.5) and stable response to strain. The assembled hydrogel sensor shows a sensitive response to human joint activities, which is expected to be applied in self-powered sensors and energy collection.
The wormlike micelles formed by surface active N -alkyl- N -methylpyrrolidinium bromide ionic liquids (ILs) have been investigated in aqueous solution. The typical rheological parameters and the viscoelastic properties of wormlike micelles were characterized by rheological measurements and cryogenic-transmission electron microscopy (cryo-TEM). The typical rheological parameters were further evaluated by Maxwell model and the viscoelastic properties were discussed based on the living polymer model. Cryo-TEM images confirmed the formation of wormlike micelles in aqueous solution. The effect of the hydrocarbon chain length of the ILs on the wormlike micelles formation was also studied.
Thermal conductivity is a very important thermal property parameter in the process of hydrocarbons transportation, storage, combustion and cooling. Therefore, accurate thermal conductivity is important in the utilization of hydrocarbons. In this work, the thermal conductivity of n-hexane and n-heptane in the temperature range of 298.15 K∼523.15 K and pressure range of 0.1 MPa∼15.0 MPa was studied by using transient hot-wire method. In order to facilitate engineering application, function polynomials of temperature and pressure are fitted and correlated with experimental data. The average absolute error of the experimental data and fitting data of n-hexane and n-heptane are 0.72 and 0.61 %, respectively, which proves that the function polynomial can describe the experimental data well. In addition, we compare the collected literature data with our results and find that the literature data is very close to our results. This work is expected to expand the range of available data on the thermal conductivity of n-hexane and n-heptane and contribute to the industrial applications of these two substances.
Due to the unique properties of heterojunction interfaces, heterojunction materials have broad application prospects in gas sensors. In this study, we synthesized In2O3 microrods through direct calcination of MIL-68(In) at ambient condition. Subsequently, WO3/In2O3 n-n heterojunction composites were built via a solvothermal method. The sensors fabricated with this heterojunction demonstrated exceptional TEA sensing capabilities, such as excellent selectivity and stability, a high response value of 678.43 to 20 ppm TEA, a fast response time (11 s) and a low operating temperature of 160°C. The increased sensing performance is attributed to the improved specific surface area, distinct barrier-controlled electron transport present in n-n type heterojunctions, and the unique selectivity of WO3 to TEA. This work not only offers a strategy for creating heterojunction-rich sensing materials, but also an efficient way for TEA detection.
Real-time monitoring of triethylamine (TEA) is essential for environmental safety and various applications in daily life. However, TEA gas sensors still encounter specific technical challenges, such as high operating temperatures and insufficient sensitivity. In this study, in order to reduce the operating temperature and improve sensitivity, WO 3 -MoO 3 (WMo) n-n heterojunctions were synthesized via calcination and subsequent solvothermal method, in which WO 3 tightly bound to the MoO 3 nanobelt surface. The resulting heterojunction demonstrated excellent TEA sensing performance. The optimized gas sensor achieved a high response of 627.28 to 20 ppm TEA at a low operating temperature (100 °C). In addition, the device exhibited strong selectivity and stability. These improvements in gas sensing performance were attributed to the formation of n-n heterojunction between MoO 3 and WO 3 , as well as the surface gas sensing reaction of oxygen species facilitated by oxygen vacancies at the heterojunction interface. This study can be applied to the design of novel n-n type metal oxide heterojunction materials for the application of low-temperature high-sensitivity TEA sensors.
Rechargeable aqueous Zn batteries are considered as promising energy-storage devices because of their high capacity, environmental friendliness and low cost. However, the hydrogen evolution reaction and growth of dendritic Zn in common aqueous electrolytes severely restrict the application of Zn batteries. Here, we develop a simple strategy to suppress side reactions and boost the reversibility of the Zn electrode. By introducing 30% (volume fractions) N,N-dimethylformamide (DMF) to the 2 M Zn(CF3SO3)2–H2O electrolyte (ZHD30), the preferential hydrogen-bonding effect between DMF and H2O effectively reduces the water activity and hinders deprotonation of the electrolyte. The ZHD30 electrolyte improves the Zn plating/stripping coulombic efficiency from ∼95.3% to ∼99.4% and enhances the cycles from 65 to 300. The Zn–polyaniline full battery employing the ZHD30 electrolyte can operate over a wide temperature range from –40°C to +25°C and deliver capacities of 161.6, 127.4 and 65.8 mAh g–1 at 25, –20 and –40°C, respectively. This work provides insights into the role of tuning solvent effects in designing low-cost and effective aqueous electrolytes.
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