RESEARCH ON CHEMICAL INTERMEDIATES
·
2022
·Vol. 49
·期 8
·3381-3393
·
IF 3.134
Yang Haoguo,Guo Yijun,Han Shitong,Xi Hailing,Lin Huaxiang,Yuan Rusheng,Ding Zhengxin,Long Jinlin,Lin Qun
Mustard gas is a kind of erosive poison with great harm and used as a chemical weapon since World War. It has suggested that the photocatalytic technology is an effective method to eliminate it. Because the small difference in molecular structure between 2-CEES and Mustard gas, and the less toxic of 2-CEES, 2-CEES is often used as a simulator to evaluate the photocatalytic activity of catalysts. In this work, symbiotic mixture of Bi 2 WO 6 and Bi 6 O 6 (OH) 3 (NO 3 ) 3 ·1.5H 2 O nanosheets doped with Mo (Mo-B-B) have been synthesized by a facile hydrothermal treatment. The samples were characterized by XRD, DRS, XPS, SEM, TEM, Raman, and PL. The photocatalytic activity of the samples was evaluated by measuring the degradation of 2-CEES under visible light irradiation. The results showed that the doped Mo reduce the Eg of bare symbiotic mixture and improve the separation efficiency of photo-generated carriers that is beneficial to photocatalytic activity. The optimum amount of doped Mo is 5% that exhibits the best activity for degradation for 2-CEES.
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FOOD CHEMISTRY
·
2022
·
IF 9.231
Cong Chen,Fei Yu,Xinli Wen,Shuna Chen,Kaixi Wang,Feiquan Wang,Jianming Zhang,Yuanyuan Wu,Puming He,Youying Tu,Bo Li
Two major green leaf volatiles (GLVs) in tea that contribute greatly to tea aroma, particularly the green odor, are (E)-2-hexenal and (Z)-3-hexenal. Until now, their formation and related mechanisms during tea manufacture have remained unclear. Our data showed that the contents of (E)-2-hexenal and (Z)-3-hexenal increased more than 1000-fold after live tea leaves were torn. Subsequently, a new (Z)-3:(E)-2-hexenal isomerase (CsHI) was identified in Camellia sinensis . CsHI irreversibly catalyzed the conversion of (Z)-3-hexenal to (E)-2-hexenal . Abiotic stresses including low temperature, dehydration, and mechanical wounding, did not influence the (E)-2-hexenal content in intact tea leaves during withering, but regulated the proportions of (Z)-3-hexenal and (E)-2-hexenal in torn leaves by modulating CsHI at the transcript level. For the first time, this work reveals the formation of (E)-2-hexenal during tea processing and suggests that CsHI may play a pivotal role in tea flavor development as well as in plant defense against abiotic stresses.
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APPLIED AND ENVIRONMENTAL MICROBIOLOGY
·
2020
·Vol. 86
·期 19
·
IF 4.016
Haixia Wang,Xiaoyu Wang,Hao Ren,Xuejun Wang,Zhenmei Lu
3-Hydroxypyridine (3HP) is an important natural pyridine derivative. Ensifer adhaerens HP1 can utilize 3HP as its sole sources of carbon, nitrogen, and energy to grow, but the genes responsible for the degradation of 3HP remain unknown. In this study, we predicted that a gene cluster, designated 3hpd, might be responsible for the degradation of 3HP. The analysis showed that the initial hydroxylation of 3HP in E. adhaerens HP1 was catalyzed by a four-component dehydrogenase (HpdA1A2A3A4) and led to the formation of 2,5-dihydroxypyridine (2,5-DHP). In addition, the SRPBCC component in HpdA existed as a separate subunit, which is different from other SRPBCC-containing molybdohydroxylases acting on N-heterocyclic aromatic compounds. Moreover, the results demonstrated that the phosphoenolpyruvate (PEP)-utilizing protein and pyruvate-phosphate dikinase were involved in the HpdA activity, and the presence of the gene cluster 3hpd was discovered in the genomes of diverse microbial strains. Our findings provide a better understanding of the microbial degradation of pyridine derivatives in nature and indicated that further research on the origin of the discovered four-component dehydrogenase with a separate SRPBCC domain and the function of PEP-utilizing protein and pyruvate-phosphate dikinase might be of great significance.IMPORTANCE 3-Hydroxypyridine is an important building block for the synthesis of drugs, herbicides, and antibiotics. Although the microbial degradation of 3-hydroxypyridine has been studied for many years, the molecular mechanisms remain unclear. Here, we show that 3hpd is responsible for the catabolism of 3-hydroxypyridine. The 3hpd gene cluster was found to be widespread in Actinobacteria, Rubrobacteria, Thermoleophilia, and Alpha-, Beta-, and Gammaproteobacteria, and the genetic organization of the 3hpd gene clusters in these bacteria shows high diversity. Our findings provide new insight into the catabolism of 3-hydroxypyridine in bacteria.
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PEST MANAGEMENT SCIENCE
·
2019
·Vol. 75
·期 12
·3273-3281
·
IF 3.255
Bao-Lei Wang,Hong-Wei Zhu,Zheng-Ming Li,Xiao Zhang,Shu-Jing Yu,Yi Ma,Hai-Bin Song
BACKGROUND N -Pyridylpyrazole derivatives have received continuous attention in agrochemical research during the last decade owing to their remarkable insecticidal or fungicidal potentials. To look for novel heterocyclic agrochemicals for increasing production of agriculture, a series of novel α -aminophosphonate derivatives containing N -pyridylpyrazole moiety were synthesized. RESULTS The structures of the title compounds were confirmed via melting point, IR, 1 H NMR, 13 C NMR, 31 P NMR, HRMS and elemental analysis. The single crystal structure of diethyl (3-bromo-1-(3-chloropyridin-2-yl)-1 H -pyrazol-5-yl)(2,6-dimethylphenylamino)methylphosphonate (compound 12b) was first reported. Moreover, the bioassays displayed that the title compounds exhibited modest or weak insecticidal activities against oriental armyworm at 200 μg mL −1 . The first investigation on the fungicidal potential of chlorantraniliprole showed no significant activities towards the six tested fungi found in this study, however, most of the title compounds displayed apparent in vitro fungicidal activity against some plant fungi, in particular excellent activities towards Physalospora piricola . Compounds 11a and 11b had EC 50 values of 18.8 and 17.4 μg mL −1 , respectively, which were comparable with that of fungicide control triadimefon (EC 50 = 24.7 μg mL −1 ) against Physalospora piricola . In addition, some compounds exhibited modest in vivo control efficacy at 0.5 mg mL −1 towards Sclerotinia sclerotiorum (11b: 30.1(±1.8)%), Rhizoctonia cerealis (11a: 20.4(±2.1)%; 11b: 30.2(±2.2)%), and Erysiphe graminis (11a: 30.3(±1.8)%; 12d: 40.2(±0.9)%). CONCLUSION Compounds 11a, 11b and 12d could be promising new lead structures for the development and discovery of novel fungicides towards Physalospora piricola and Erysiphe graminis . The structure-activity relationship (SAR) analysis provided useful guidance and new understanding for the design of novel pyridylpyrazole-containing agrochemicals. © 2019 Society of Chemical Industry
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Foods
·
2024
·Vol. 13
·期 2
·261
·
IF 4.7
Shanshan Liu,Mingyue Shen,Jianhua Xie,Bohan Liu,Chang Li
2-Monochloropropane-1, 3-diol (2-MCPD) esters and 3-monochloropropane-1,2-diol (3-MCPD) esters, a class of substances potentially harmful to human health, are usually formed during the refining of vegetable oils under high temperature. The effects of endogenous antioxidants in vegetable oils on the formation of 2- and 3-MCPD esters is still unknown. In this study, the effects of endogenous antioxidants (α-tocopherol, stigmasterol and squalene) on the formation of 2- and 3-MCPD esters in model thermal processing of camellia oil were investigated. The possible formation mechanism of 2- and 3-MCPD esters was also studied through the monitoring of acyloxonium ions, the intermediate ions of 2- and 3-MCPD esters formation, and free radicals by employing infrared spectra and electron paramagnetic resonance (EPR), respectively. The results indicated that the addition of α-tocopherol had either promoting or inhibiting effects on the formation of 2- and 3-MCPD esters, depending on the amount added. Stigmasterol inhibited the formation of 3-MCPD ester and 2-MCPD ester at low concentrations, while promoting their formation at high concentrations. Squalene exhibited a promotional effect on the formation of 3-MCPD ester and 2-MCPD ester, with an increased promotion effect as the amount of squalene added increased. The EPR results suggested that CCl3•, Lipid alkoxyl, N3• and SO3• formed during the processing of camellia oil, which may further mediate the formation of chlorpropanol esters. This study also inferred that squalene promotes the participation of the free radical in chlorpropanol ester formation.Keywords:MCPD esters;endogenous antioxidants;camellia oil;mechanism
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JOURNAL OF APPLIED POLYMER SCIENCE
·
2024
·
IF 2.7
Yaling Deng,Lei Nie,Yu Xu,Chenhong Gao,Zhe Wu
The development of highly effective bio-lubricant coatings for arthritis treatment is extremely demanded. Herein, inspired by the efficient lubrication of articular cartilage, acrylic acid (AA) with (3-(methacryloylamino) propyl) dimethyl (3-sulfopropyl) ammonium hydroxide (MPDSAH) hydrogel coatings containing nanoparticles on Ti6Al4V substrate were designed and fabricated via UV grafting technology. SiO 2 and SiO 2 grafted with PAA polymer brushes (SiO 2 -g-PAA) were separately doped into the PAA-PMPDSAH hydrogel. The PAA-PMPDSAH/SiO 2 -g-PAA exhibits good tensile and compressive properties compared with PAA-PMPDSAH/SiO 2 hydrogel, with an enhancement of 183.4% in tensile modulus and 60.8% in compressive modulus. The PAA-PMPDSAH/SiO 2 -g-PAA hydrogel coatings exhibit a low wear volume, 2.9 ± 0.16 × 10 6 μm 3 , representing a decline of 32.1% and 61.3% compared with the PAA-PMPDSAH and PAA-PMPDSAH/SiO 2 hydrogel coatings, respectively. The antiwear performance has obviously improved. The hydrophilic PAA polymer brushes prevent the agglomeration of nanoparticles and promote homogeneously dispersion within the hydrogel. The three-dimensional crosslinked network structure of hydrogel effectively protects the structural integrity of the polymer brushes, thereby facilitating enduring lubrication properties. This work provides a strategy for promising artificial joint lubrication in biomedical fields.
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POSTHARVEST BIOLOGY AND TECHNOLOGY
·
2025
·
IF 6.8
Lijun Ling,Rongxiu Mo,Wenyue Zhang,Yijuan Jiang,Fanjin Kong,Lijun Feng,Yao Li,Rui Yue,Yongpeng Zhou
The antifungal activity of six microbial-derived volatile organic compounds (VOCs) [ 3-hepten-2-one (Hep), cis-3-octen-1-ol, 3-methylvalerate, isovalerate, 1-octen-3-ol (Oct), and 2-methylbutyrate] against Aspergillus flavus was investigated by determining the minimum inhibitory concentration (MIC) and the fractional inhibitory concentration index (FICI). The results demonstrated that all 15 binary combinations of the VOCs presented additive effects against A. flavus . Among them, the combination of Hep and Oct, refers to C OH , with concentrations of 2 μL L −1 and 2.5 μL L −1 , respectively, displayed the most potent antifungal effect with the lowest concentration, in contrast to the individual MIC of Hep or Oct, which were reduced to 1/8 and 1/2. C OH can induce membrane lipid peroxidation, enhance cell membrane permeability, and cause leakage of nucleic acids and proteins within the cell, and 1-octen-3-ol might play a leading role. Finally, applying C OH at a concentration of 1/2 MIC Oct + 1/4 MIC Hep could effectively restrain the spread of A. flavus on wolfberries and exhibit excellent preservation effects. This study validates the antifungal effect of C OH and may serve as a natural alternative to antimicrobial agents for post-harvest agricultural products.
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ACS Omega
·
2018
·
IF 0
Xin-Xin Wang,Fei-Yang Tian,Kai Chen,Yun-Qian Zhang,Zhu Tao,Qian-Jiang Zhu
In the present work, we selected hexamethylcucurbit[3,3]uril (Me6Q[3,3]) as a building block and obtained two Me6Q[3,3]-based porous supramolecular assemblies from neutral water (A) and aqueous HCl solutions (B), respectively. Both Me6Q[3,3]-based assemblies are constructed of Me6Q[3,3] molecules through the typical outer surface interaction of cucurbit[n]urils, as well as hydrogen bonding between latticed water molecules and portal carbonyl oxygens of Me6Q[3,3]. The assemblies present different porous structure features and exhibit different adsorption properties for eight common volatile organic compounds. However, the two porous assemblies exhibit similar adsorption properties for certain fluorophore dyes, including rhodamine B (G1), fluorescein (G2), and pyrene (G3), and form solid colored fluorescent compounds, some of which exhibit responses to the selected volatile organic compounds.
研究领域:
化学
·
材料科学
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JOURNAL OF CHEMICAL AND ENGINEERING DATA
·
2020
·
IF 2.369
Yanmin Shen,Wenju Liu,Paifeng Shi,Zehua Bao
In this work, solubility of exo-3,6-epoxy-1,2,3,6-tetrahydrophthalic anhydride (ETA) was measured and discussed in acetone + ethanol, methyl acetate + ethanol, 1,4-dioxane + ethanol, and ethyl acetate + ethanol mixture solvents in a temperature range from 278.15 to 323.15 K by a gravimetric method under 0.1 MPa. Experimental results indicated that solubility increased with temperature increasing and declined with the mass fraction increasing of ethanol in four kinds of mixture solvents. The solvent effect and Hansen solubility parameter were adopted to discuss the solubility behavior of ETA in selected solvents. Modeling correlation solubility data about ETA indicated that the Jouyban–Acree–Apelblat model (J–A–A) was more suitable than the Jouyban–Acree–Van’t Hoff model (J–A–V) and Ma and Sun model in mixture solvents. Processing of the dilution crystallization in acetone + ethanol system was chosen to separate and purify ETA on the basis of the solubility and solvent characteristics.
研究领域:
化学工程
·
物理化学
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GREEN CHEMISTRY
·
2015
·Vol. 17
·期 7
·3992-3999
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IF 8.02
Shujing Zhu,Xiaoqiang Ma,Erzheng Su,Dongzhi Wei
From an environmental perspective, utilizing nonconventional solvents (i.e. green solvents) with low ecological footprints is a highly beneficial alternative to using conventional organic solvents to form a reaction system. The nitrile hydratase (NHase, EC 4.2.1.84) catalyzed hydration of 2-amino-2,3-dimethylbutyronitrile (ADBN) to 2-amino-2,3-dimethylbutyramide (ADBA) in various green solvent–aqueous reaction systems was investigated in this study. After systematically optimizing the reaction conditions, the HFE-7100/H2O (v/v, 10%) biphasic system was ultimately identified as a promising reaction system for reducing product inhibition, avoiding substrate hydrolysis, and facilitating product separation and solvent recovery. The average ADBA yield of an entire batch reaction was 97.3%, which is obviously higher than those obtained with previously reported chemical or enzymatic methods. This is the first attempt to apply a fluorous solvent–aqueous biphasic system to a biocatalytic process, and the results suggest that the fluorous solvent employed in the biphasic system satisfies the requirements for green chemistry.
研究领域:
生物化学
·
环境科学
·
绿色化学
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MICROCHEMICAL JOURNAL
·
2021
·
IF 4.821
Jian-Bo Chen,Xueyan Zhao,Zhenqi Zhang,Ya Chen,Xiaolin Fu,Yu Liu
Recently, 3,3-diamino-4,4-azoxyfurazan (DAAF) as one of most promising energetic furazan compounds has been widely studied because of its excellent explosive performances. Nowadays, the Oxone oxidation method is regarded as a main pathway to synthesize DAAF. However, several unknown impurities are yielded when the Oxone method is used to prepare DAAF. The identification of DAAF’s impurities is beneficial to optimize synthetic route of DAAF and then improve its purity. In this study, chemical structures of DAAF and its main impurities were analyzed by developing an unknown analysis workflow based on ultrahigh-performance liquid chromatography-tandem diode array detector -tandem high resolution mass spectrometry (UHPLC-DAD-HRMS). They were fully separated by UHPLC after the optimization of chromatographic conditions. HRMS based on a Q-Orbitrap system was performed to elucidate chemical structure of the impurities by determining exact mass of the impurities and their MS/MS fragments. Besides DAAF, eight unknown impurities were detected under negative ion mode ([M-H] - ) of HRMS with a heated electrospray ionization. Comprehensive analysis of UHPLC-DAD-HRMS provided more information including the retention time, UV–Vis spectrum, elementary composition and MS/MS fragments, and then possible structures of the impurities were proposed in this work. Further, the ion at m / z 211.0328, impurity I and impurity V were confirmed to be DAAF, DAF and DAAzF, respectively, through 1 H NMR and 13 C NMR after synthesizing their reference materials. In addition, the source of these impurities during the synthesis of DAAF has been analyzed. The impurities were originated from the precursor, the intermediate and byproduct of preparing DAAF through the hydrazine, the isomerism and the nitrosation.
研究领域:
化学
·
材料科学
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ACS Applied Materials & Interfaces
·
2026
·
IF 7.8
Xiaopeng Zhang,Lin Chen,Longzhu Li,Xiaoming Yan,Junjiang Bao,Ning Zhang,Gaohong He
The introduction of guest metal molecules into metal–organic frameworks (MOFs) is an outstanding method to prepare dual-atom catalysts (DACs) with good oxygen reduction reaction (ORR) activity. However, most of the MOF-derived dual-atom catalysts reported to date exhibit a microporous structure and, therefore, suffer from the underutilization of active sites and poor mass transfer. This study employed NH2-MIL-101 as a precursor to form defect-bearing mesoporous Fe-NC via one-step pyrolysis for adsorbing [Co(en)3]3+, followed by secondary pyrolysis to generate Fe–Co binuclear site catalysts. The mesopores of NH2-MIL-101 are beneficial to [Co(en)3]3+ introduction and can improve the mass transfer of the ORR. Furthermore, the elevated nitrogen content within the [Co(en)3]3+ complex facilitates the co-coordination of Fe and Co with nitrogen, thereby enhancing the formation of Fe–Co diatomic sites. As a result, the obtained FeCo-NC-40 catalyst showed excellent ORR performance with a half-wave potential of 0.915 V (vs RHE). In addition, the liquid-phase Zn–air battery employing FeCo-NC-40 as the cathode catalyst demonstrated a peak power density of 178.13 mW·cm–2 and achieved a discharge specific capacity of 806.13 mAh·g–1 at 10 mA·cm–2, and there was no significant decay in stability for 10 days of continuous cycling.
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