Frontiers in Chemistry
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2022
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IF 5.545
Kuang Yi,Xia Yunlong,Wang Xing,Rao Qingqing,Yang Shengxiang
4-hydroxyl coumarin (HC), an important intermediate during the synthesis procedure of rodenticide and anti-cardiovascular drug, shows highly medicinal value and economic value. To achieve the efficient adsorption of HC from natural biological samples, a novel magnetic surface molecularly imprinted polymer (HC/SMIPs) was constructed by employing methacrylic acid (MAA) as functional monomer, organic silane modified magnetic particles as matrix carrier and HC as template molecule. Due to the numerous specific imprinted cavities on the HC/SMIPs, the maximum adsorption capacity of HC/SMIPs for 4-hydroxycoumarin could reach to 22.78 mg g−1 within 20 min. In addition, HC/SMIPs exhibited highly selective adsorption for 4-hydroxycoumarin compared with other active drug molecules (osthole and rutin) and showed excellent regeneration performance. After 8 cycles of adsorption-desorption tests, the adsorption capacity of HC/SMIPs just slightly decreased by 6.64%. The efficient selective removal and easy recycle of 4-hydroxycoumarin from biological samples by HC/SMIPs made a highly promising to advance the application of imprinting polymers in complex practical environments.
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MATERIALS CHEMISTRY AND PHYSICS
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2022
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IF 4.778
Zhijia Zhang,Huifeng Mei,Qiang Wang,Rui Li,Guojun Wang,Hao Wei,Xiao Ouyang
Unlike the organisms in nature, the synthetic materials are difficult to repair the damage via self-regulation. Even the self-healing materials generally require the external stimuli (e.g., temperature, pressure, light, etc ) to repair themselves. In this paper, self-healing polyurethane elastomer was designed and prepared based on 2-ureido-4[1 H ]-pyrimidinone compound by the simple physical blending method. The tensile strength and the elongation at break of the self-healing polyurethane elastomer were 0.65 MPa and 623.1%, respectively. The healing performance was measured by cut-off experiment, showing that the fracture of the self-healing polyurethane elastomer was healed at room temperature without external stimuli and kept excellent mechanic properties. The healing efficiencies of the tensile strength and the elongation at break were achieved to 87.7% (0.57 MPa) and 71.7% (446.7%) after healing at room temperature with 30 h, respectively. When the temperature was up to 80 °C, the healing time curtailed at 1 h. And the tensile strength and the elongation at break were recovered to 0.59 MPa and 532.1%, respectively. These promising results provide a strategy that allows increasing the life cycle of materials, adapting them to a circular economy model, thus reducing the generation of waste.
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MOLECULES
·
2022
·Vol. 27
·期 9
·2738
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IF 4.927
Lu Xu,Jinmeng Yu,Lu Jin,Le Pan
A series of 30 succinate dehydrogenase inhibitors (SDHIs) of 4-amino coumarin-based derivatives were designed and synthesized. According to the analysis of fungicidal activity in vitro, most of the compounds expressed broad-spectrum antifungal activity against four plant pathogenic fungi (Alternaria alternata, Alternaria solani, Fusarium oxysporum,andBotrytis cinerea) using the mycelium growth inhibition method. The results showed that compounds3nwith the group of 2-ene-3-methyl-butyl and4ewith the group of 2-bromo-1-oxo-hexyl displayed excellent activity againstAlternaria alternataandAlternaria solani, with EC50values of 92~145 μg/mL. Molecular docking showed that the inhibitor3nwas completely locked into the cavity of SDH, forming a conventional hydrogen bond interacting with the amino acid residue TYR58. The present work indicates that these derivatives would serve as novel potential fungicides targeting SDH.Keywords:succinate dehydrogenase;inhibitor;4-amino coumarin;fungicide;antifungal activity;molecular docking
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Chemical Engineering and Processing-Process Intensification
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2021
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IF 4.237
Zhou Lan,Yangcheng Lu
In this work, a tubular reactor with a micromixer was introduced in attempt to enhance the amination reaction of 4-nitrochlorobenzene in terms of the process efficiency and safety. It was found that the reaction system containing a large excess of ammonia water can become homogeneous at high temperature. Thus, as both micromixing and the heat transfer performance were guaranteed, the set-up combining a micromixer and a microtube reactor enabled the reaction to exhibit homogeneous reaction characteristics, meeting the demands of efficiency and reliability. Furthermore, using a multi-channel sampling system connected behind the micromixer, the reaction kinetics were studied in a modified “stop flow” mode, which is adaptable for in-situ fast homogenization, high temperature, and high pressure. The reaction conditions were screened and a kinetic model was developed. Accordingly, we propose and verify a self-circulation strategy to reduce the burden of ammonia separation and recovery in a continuous tubular reactor system.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2021
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IF 8.128
Xiangquan Liu,Jiaqi Tang,Jinglun Yang,Helan Zhang,Yu Fang
Preparation of nanofilms which are able to reject water-soluble low molecular weight organic compounds in nanofiltration remains to be a challenge. Herein, we report a new kind of self-standing, defect-free, robust, centimeter-sized and thickness controllable calix[4]pyrrole (C[4]P)-based nanofilms with excellent molecular sieving performance in nanofiltration. The nanofilms were prepared via confined dynamic condensation of the tetra-benzoyl-hydrazine derivative of calix[4]pyrrole (CPTBH) with 1,3,5-benzenetricarboxaldehyde (BTC) at the air/dimethyl sulfoxide (DMSO) interface. Nanofiltration tests under 2 bar pressure with porous polyethylene terephthalate (PET) as the support and a CsF treated CPTBH-BTC nanofilm (∼100 nm) as the selective layer depicted a water permeance of 15 L m -2 h −1 bar −1 and a methanol permeance of 45 L m -2 h −1 bar −1 . High rejection rates (>95%) were found in aqueous solution for most of the tested dyes and pharmaceuticals. Remarkably, the composite membrane also demonstrated good separation performance in aqueous phase to some amino acids and organic dyes with molecular weights around 200 g/mol. High-performance nanofiltration in methanol was also realized. In this case, the molecular weight cutoff value is ∼ 800 g/mol. These findings showed that introduction of macrocyclic hosts is an effective way to develop nanofilms with high solvent permeance but low molecular weight cutoff value.
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INORGANIC CHEMISTRY
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2021
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IF 5.165
Jianping Zhao,Fei Qian,Wenping Guo,Jianfeng Li,Zeyuan Lin
Three different manganese(II) porphyrins have been exploited to react with 4-methylimidazolate (4-MeIm–), and the five-coordinate products are characterized by ultraviolet–visible, single-crystal X-ray, and electronic paramagnetic resonance spectroscopies. Interestingly, 4-MeIm– is found to bond to the metal center through either of the two N atoms (N1 or N3), which yielded two linkage isomers with either an unhindered or a hindered ligand conformation, respectively. Investigations revealed it is the large metal out-of-plane displacements (Δ24 and Δ4 ≥ 0.59 Å) that have rendered the equivalence of two isomers with a small energy difference (5.2–8.3 kJ/mol). The nonbonded intra- and intermolecular interactions thus become crucial factors in the balance of linkage isomerization. All of the products in both solution and solid states show the same characteristic resonances of high-spin Mn(II) (S = 5/2) with g⊥ ≈ 5.9 and g∥ ≈ 2.0 at 4 K, consistent with the weak effects of the axial ligand on core conformation and metal electronic configurations. Zero-field splitting parameters obtained through simulations are also reported.
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RESEARCH ON CHEMICAL INTERMEDIATES
·
2020
·Vol. 46
·期 11
·5117-5131
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IF 2.262
Sun Li,Zhou Mingliang,Yin Zheng,Zhang Lixin,Dou Binlin,Su Wenxian
Abstract A green, rapid and controllable synthesis of gold nanoparticles (Au NPs) was achieved using the mulberry fruit (MF) extract as reducing and capping agent at room temperature. Obtained Au NPs were characterized by ultraviolet–visible spectrum, transmission electron microscopy, energy-dispersive X-ray spectroscopy, high-resolution transmission electron microscopy, selected area electron diffraction, X-ray photoelectron spectroscopy and Fourier transform infrared spectroscopy analyses. It could be found that Au NPs had a small size of 4.2–20.1 nm, face-centered cubic crystalline structure and homogeneous dispersion, indicating strong reducing and capping capacities of the MF extract. Meanwhile, the morphology (quasi-sphere/sphere) of Au NPs could be controlled only by adjusting the MF extract concentration. Furthermore, based on the 4-nitrophenol (4-NP) reduction reaction, as-prepared Au NPs exhibited excellent photocatalytic activity and stability in 30 days. Under sunlight irradiation, 4-NP could be completely reduced in 4 min and its rate constant could reach up to 0.91 min −1 . And the rate constant could be linearly adjusted by the MF extract concentration or the amount of Au NPs hydrosol. In addition, it could also be found that the light source with short wavelength could obviously elevate the photocatalytic activity of Au NPs, attributed to the hot-electron effect. Clearly, as-obtained Au NPs can have great potential applications in wastewater treatment. Graphic abstract
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SOLAR ENERGY
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2019
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IF 4.674
Wenhui Zhao,Xiaoyan Gan,Lili Ke,Liling Guo,Hanxing Liu
Two-dimensional layered organic-inorganic perovskite hybrids have attracted increasing attention due to their outstanding moisture resistance and promising optoelectronic properties. However, the photovoltaic performance in solar cells is still a huge challenge for two-dimensional perovskite films. With the aim to improve the efficiency of 2D perovskite solar cells, the new (ClC 6 H 4 C 2 H 4 NH 3 ) 2 MA n−1 Pb n I 3n+1 perovskite family (abbreviated as (CPEA) 2 MA n−1 Pb n I 3n+1 ) are synthesized by a simple one-step hot-casting method in this study. It is found that the variation of n value (n = 3–6) has great influence on the microstructure, grain size, charge mobility, trap density and photovoltaic performance of the 2D (CPEA) 2 (MA) n−1 Pb n I 3n+1 . Due to the best film quality and prolonged carrier lifetime, the (CPEA) 2 MA 4 Pb 5 I 16 (n = 5) perovskite solar cell exhibits a highest efficiency of 11.86%, with a V oc of 0.989 V, a J sc of 19.92 mA/cm 2 and FF of 60%, respectively. It is anticipated that our approach to explore new organic spacer cations in 2D perovskites may pave the way for their application with high performance.
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Sustainability
·
2022
·Vol. 14
·期 21
·14300
·
IF 3.889
Qinghong Wang,Siyu Li,Xin Wang,Zhuoyu Li,Yali Zhan,Chunmao Chen
The extensive use of pharmaceuticals and personal care products (PPCPs) causes high concentrations of pharmaceutical metabolites to exist in aquatic environments. Though the removal of parent PPCPs has raised concerns, the degradation of pharmaceutical metabolites was rarely investigated. In this study, the degradation of 4-acetylaminoantipyrine (4-AAA), a typical dipyrone metabolite frequently detected worldwide in surface water and wastewater, was initially studied using persulfate (PDS)-based advanced oxidation processes (AOPs). Compared with commonly used activation methods of alkali, ultrasonic, ultraviolet, and Fe2+, 4-AAA achieved its best degradation (98.9%) within 30 min in a thermally activated PDS system due to the promotion of both radical production and the reaction rate with the rise in temperature. The optimum degradation of 4-AAA could be achieved with the temperature of 80 °C regardless of initial pH values, indicating a wide suitable pH range. Moreover, over 80% of the degradation of 4-AAA could be achieved with the presence of Cl−(0–16 mM), HCO3−(0–8 mM), and humic acid (0–30 mg/L), further indicating the application potential of the system. Both sulfate radicals (SO4•−) and hydroxyl radicals (•OH) contributed to 4-AAA degradation and the contribution of •OH increased with the pH rising from 3 to 11 due to the transformation from SO4•−when reacting with OH−. Three hydroxylated and ring-opening intermediates were detected during the 4-AAA degradation. The ECOSAR prediction indicated that the acute toxicity of most intermediates decreased than 4-AAA while the chronic toxicity increased, which suggested the transformation of intermediates should be further focused on in SO4•−and •OH based AOPs. This study would provide technical reference for the control of 4-AAA in wastewater treatment processes, raise concerns on the influence of PPCPs metabolites, and throw light on reducing the harm of PPCPs and their metabolites in aquatic environments.Keywords:4-acetylaminoantipyrine (4-AAA);heat activation;persulfate;degradation pathway;toxicity
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INORGANIC CHEMISTRY COMMUNICATIONS
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2022
·
IF 3.428
Jiashun Liang,Kaili Liang,Lifeng Li,Yuqi Cao,Xiong Cao
This paper investigates the effect of Fe 2 O 3 nanosheets as catalysts on the catalytic decomposition performance of DAP-4. Our laboratory has successfully fabricated Fe 2 O 3 nanosheets and DAP-4. The morphology and composition of DAP-4 and Fe 2 O 3 nanosheets were investigated using SEM, XRD and XPS. The catalytic decomposition performance of DAP-4 and DAP-4/Fe 2 O 3 nanosheets mixture samples were characterized by DSC. The results show that the synthesized Fe 2 O 3 nanosheets can reduce the activation energy of DAP-4, Fe 2 O 3 nanosheets have good catalytic activity. And calculate the relevant kinetic parameters for the mixed samples using the Kissinger equation.
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Fermentation-Basel
·
2023
·Vol. 9
·期 12
·998
·
IF 3.7
Yi Wei,Guangyao Mei,Jinlin Zhao,Shaoyang Zhang,Wenping Qin,Qing Sheng,Zhongyi Yang
Testosterone (TS) is an important androgen drug and a precursor of steroid drug synthesis. Ketoreductase 2 (KR-2) (GenBank accession no. ABP64403.1) is observed to stereo-selectively catalyze the bioreduction of 4-androstene-3,17-dione (4-AD) to testosterone and contribute to the regeneration of NADH using isopropanol as a co-substrate. The Km value of KR-2 was 2.22 mmol/L with 4-AD, and the optimal pH was 6.5–7.0. The enzyme is stable and demonstrates relatively high-level enzyme activity at 40 °C. Acetone significantly inhibits this activity. This inhibition was overcome using an intermittent vacuum during the reaction process. Finally, the amount of TS reached 65.42 g/L after a 52 h reaction with 65.8 g/L 4-AD, 10% isopropanol, and 2 g/L β–NAD+at 40 °C, with a conversion rate of 98.73%. A total of 6.15 g of TS was obtained from 6.58 g of 4-AD after the reaction and purification; the HPLC purity was 99.82%, and the overall yield was 92.81%. This enzyme provides a promising route for the green biosynthesis of testosterone for industrial applications.Keywords:testosterone;bifunctional ketoreductase;NADH regeneration;enzymatic synthesis
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ACS Applied Polymer Materials
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2023
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IF 5
Siyuan Zhang,Jiao He,Xinjian Cheng
Amphiphilic hyperbranched polymers (AHBPs) possess important characteristics, such as high solubility, low viscosity, and multiple functional groups, making them of significant scientific interest. In this work, a chain transfer agent (CTA) with a styrene unit was synthesized at first. Subsequently, the CTA was polymerized with a coumarin derivative containing a −C=C bond through reversible addition-fragmentation chain transfer-self-condensing vinyl polymerization (RAFT-SCVP) to obtain the hyperbranched polymer HP-1. Finally, using HP-1 as a macromolecular CTA, amphiphilic hyperbranched fluorescent probes AHP-2 and AHP-3 were synthesized via RAFT polymerization of hydrophilic monomers poly[oligo(ethylene glycol) methacrylate] (PEGMA) and 2-(dimethylamino)ethyl methacrylate (DMAEMA). The as-prepared AHP-2 and AHP-3 were characterized and confirmed. These macromolecular fluorescent probes enable highly sensitive and specific recognition of 4-nitrophenol (4-NP) with detection limit as 0.59 μM. A unique fluorescence quenching effect, termed “enriching inner filter effect (IFE)”, was revealed through the study of the recognition mechanism of the probes for 4-NP in hyperbranched polymers. This effect has the potential to expand the preparation methods of both fluorescent probes and functional hyperbranched polymers. This work investigates the synthesis methodology of amphiphilic hyperbranched polymers and the performance of fluorescent probes, providing a valuable approach for the development of highly sensitive polymer fluorescent probes in the future.
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