CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Tingting Wang,Xilong Cui,Shuang Cai,Xinshu Zou,Sidi Zheng,Yanhua Li,Zhiyun Zhang
The acquired drug resistance coupled with complex physiology and pathogenesis of biofilm challenges multidrug-resistant bacterial biofilm infection treatment. Herein, antimicrobial phytochemical isoliquiritigenin (ISL) loaded rhamnolipid (RL) modified chitosan nanoparticles (ISL@RL-CS) were constructed. The obtained ISL@RL-CS NPs were able to simultaneously eradicate methicillin-resistant Staphylococcus aureus (MRSA) biofilms at all stages and relieve accompanied inflammation. In the acid environment of biofilms, RL could be detached from the ISL@RL-CS and destroyed the biofilm structure. Then, the combination of phytochemical ISL and cationic chitosan could rapidly kill the dispersed bacteria, and inhibit the re-adhesion of residual bacteria, thus preventing the re-formation of new biofilms. Additionally, the inflammatory responses at the infection site were simultaneously alleviated by the anti-inflammatory features of ISL. In the MRSA-biofilm implant infected mice model, ISL@RL-CS demonstrated prominent biofilm eradication and anti-inflammation efficacy. Taken together, ISL@RL-CS with simple formulation but multi-functions provides a comprehensive and sustainable strategy for managing the intractable MRSA biofilm infections.
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JOURNAL OF HAZARDOUS MATERIALS
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2023
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IF 13.6
Jun Wang,Hao Lv,Xiandong Tong,Wei Ren,Yi Shen,Lun Lu,Yang Zhang
In order to minimize the knowledge gap between single and binary pollutants degradation by persulfate-based advanced oxidation processes (PS-AOPs), iron-loaded N-doped carbon nanotubes (Fe-NCNT) and its acid-washing sample (Fe-NCNT-W) were synthesized as peroxymonosulfate (PMS) activator for simultaneous oxidation of acid orange 7 (AO7) and electron-rich (phenol/ibuprofen) or electron-deficient pollutants (nitrobenzene/benzoic acid). Mechanistic studies revealed that both radical (HO•, SO 4 •− ) and nonradical (electron-transfer, high-valent iron) pathways involved for organic oxidation in Fe-NCNT/PMS system, while electron-transfer pathway (ETP) and high-valent iron-oxo species accounted for pollutant degradation at the surface and inner space of Fe-NCNT-W, respectively. The oxidation performances in single or binary systems were systematically investigated. In comparison to benchmark radical-based (Fe 2+ /PMS), nonradical ETP (NCNT/PMS) and mixed (Fe-NCNT/PMS) systems, Fe-NCNT-W/PMS outperformed superior performance toward oxidation of binary pollutants with little inference from solution pH or background substances, which could also be fabricated into membrane reactor for actual dyeing sewage treatment . Such superiorities should be mainly ascribed to the particular selectivity and intensive treatment of nonradical pathways in Fe-NCNT-W/PMS system with nanoconfinement effect. This work affords novel insights into the treatment of combined pollution via PMS activation by engineered nanomaterials .
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MOLECULES
·
2023
·Vol. 28
·期 16
·6063
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IF 4.6
Yali Guo,Bing Wang,Lifei Gu,Guo Yin,Shuhong Wang,Meifang Li,Lijun Wang,Xie-An Yu,Tiejie Wang
The fraud phenomenon is currently widespread in the traditional Chinese medicine Radix Astragali (RA) market, especially where high-quality RA is substituted with low-quality RA. In this case, focused on polysaccharides from RA, the classification models were established for discrimination of RA from different growth patterns, origins, species, and growth years. 1H Nuclear Magnetic Resonance (H1-NMR) was used to establish the spectroscopy of polysaccharides from RA, which were used to distinguish RA via chemical pattern recognition methods. Specifically, orthogonal partial least squares discriminant analysis (OPLS-DA) and linear discriminant analysis (LDA) were used to successfully establish the classification models for RA from different growth patterns, origins, species, and growth years. The satisfactory parameters and high accuracy of internal and external verification of each model exhibited the reliable and good prediction ability of the developed models. In addition, the polysaccharide content and immunological activity were also tested, which was evaluated by the phagocytic activity of RAW 264.7. And the result showed that growth patterns and origins significantly affected the quality of RA. However, there was no significant difference in the aspects of origins and growth years. Accordingly, the developed strategy combined with chemical information, biological activity, and multivariate statistical method can provide new insight for the quality evaluation of traditional Chinese medicine.Keywords:Radix Astragali;immunomodulatory activity;polysaccharide content;chemical pattern recognition;quality evaluation
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GREEN CHEMISTRY
·
2023
·Vol. 25
·期 17
·6869-6880
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IF 9.8
Zhikun Peng,Zhixi Wu,Xiaotong Sun,Hongji Li
Aryl ethers greatly influence lignin depolymerization and the oxygen content in lignin products. Cleaving aryl ethers normally requires harsh conditions such as high-pressure hydrogen gas and elevated temperature. Herein, we developed a synergistic method that combines photocatalytic hydrogen transfer with acid catalysis for H2-free hydrogenolysis of diphenyl ether and aromatic oxygenates at room temperature. The electron-enriched Pt/TiO2 surface stored abundant hydrogen species under light irradiation and efficiently catalyzed hydrogen transfer from isopropanol to aryl ethers. The acid mediated the hydrogenation sequence into: hydrogenolysis of aryl C–O bonds > saturation of aryl rings ≫ hydrogenolysis of aliphatic C–O bonds. DFT calculations suggested the aryl ether bond adsorbed on the Pt surface was weakened through protonation. This method delivered 98% yield of aliphatic monomers (73% cyclohexane and 25% cyclohexanol) from cleavage of diphenyl ether, and converted aromatic mixtures into cycloalkanes (57%) and aliphatic alcohols (9%) under mild conditions.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2023
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IF 4.4
Boxu Wang,Zheng Liu,Zhihong Li,Ningyi Xu,Xuejiao Zhang,Ruifang Su,Junyang Wang,Rui Jin,Chunyan Sun
Hg 2+ is highly toxic to human health and ecosystem. In this work, based on the unique fluorescent property of 2-Aminopurine (2-AP), the formation of T-Hg 2+ -T mismatch structure and the signal amplification of exonuclease III (Exo III) assisted target cycle, a fluorescent probe for facile and sensitive detection of Hg 2+ is constructed. The hairpin-looped DNA probe is rationally designed with 2-AP embedded in the stem and thymine-rich recognition overhangs extended at the termini. The cleavage of the double stranded DNA stem with stable T-Hg 2+ -T pairs catalyzed by Exo III is prompted to happen upon recognition of trace Hg 2+ . Under the optimal reaction conditions, there is an excellent linear relationship between Hg 2+ concentration and fluorescence intensity in the range of 7.5–200 nM with a detection limit of 0.38 nM. In addition, the detection results of Hg 2+ in Songhua River water and fish samples are satisfactory. The fluorescent probe avoids labeling additional quenchers or quenching materials and has strong anti-interference ability. Thus, the fluorescent probe has a broad prospect in practical application.
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ACS Applied Polymer Materials
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2023
·
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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ACS Applied Polymer Materials
·
2023
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IF 5
Jingkai Liu,Liyue Zhang,Xinbei Zhu,Qing Chen,Kan Zhang,Xiaoqing Liu
Phenolic derivatives capable of reducing the ring-opening temperature of benzoxazine resin have gradually emerged as valuable modules for benzoxazine chemistry, not to mention their good compatibility, coreactivity, and network modifiability. However, the previously reported unsatisfactory promotion effects, unclear reaction mechanisms, and unstable structure have severely limited the development of benzoxazine/phenol systems. Herein, a supramolecular hydrogen-bonded system consisting of resorcinol and 2-aminopyridine benzoxazine (PH-2a) was developed. The PH-2a/resorcinol mixture system with an equivalence ratio of 1:1 exhibited a dramatic reduction in ring-opening peak temperature (Tp) from 283 to 110 °C. Experimental combined with computational investigations supported its supramolecular H-bond behavior. Based on the cross-comparison of PH-2a analogues and other diphenols, the critical roles of H-bonding interactions both in activating reactants and inducing a directional reaction were revealed. These H-bonds with appropriate strengths can self-assembly form and close the distance between potential reaction sites, facilitating the direct production of an adduct. In addition, the application potential of the PH-2a/resorcinol system was also prospected, which can promise network tailoring and low-temperature cross-linking by the design flexibility of PH-2a and resorcinol derivatives, opening up possibilities for the preparation of advanced polybenzoxazine resins at low temperature.
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MACROMOLECULES
·
2023
·
IF 5.5
Nan Li,Shengfu Yang,Kan Zhang
The future development of benzoxazine thermosetting resins as advanced polymeric materials depends on designing more attractive chemical structures and reaching a deeper understanding of the structure–property relationship at the molecular level. Herein, we synthesized a new series of benzoxazines containing the thiophenecarboxamide or thiopheneacetamide functionality at the ortho- and para-positions with respect to oxygen in the oxazine ring. Successful syntheses of thiophene-rich benzoxazine monomers and their corresponding molecular characterizations were confirmed by Fourier transform infrared (FT-IR) spectroscopy, nuclear magnetic resonance (NMR), and high-resolution mass spectroscopy. Ring-opening polymerization processes of benzoxazines and thermal properties of their resulting polybenzoxazines were studied by differential scanning calorimetry, in situ FT-IR spectroscopy, and thermogravimetric analysis. In addition, a combined experimental and computational study using both 1D and 2D NMR as well as density functional theory calculations provided kinetic insights into the effects of structural and hydrogen bonding on the polymerization mechanism. With the designed varieties of hydrogen bonds in these novel benzoxazines, it has been found that oxygen in the oxazine ring involved in stronger hydrogen bonding can generate a relatively weaker O–CH2 bond, leading to the reduced ring-opening polymerization temperature. The fundamental investigations presented in the current work provide us a deeper understanding of the hydrogen bonding interaction in benzoxazine as well as its role in polymerization behavior. Moreover, these newly obtained thiophene-rich benzoxazines also give us ample opportunities to develop high-performance polybenzoxazine thermosets with promising applications.
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JOURNAL OF MOLECULAR LIQUIDS
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2023
·
IF 6
Ziyue Zhou,Yu Cao,Kai Zong,Dongshun Deng
In chemical industry, efficient absorption of ammonia (NH 3 ) from industrial exhaust remains a challenge and significant issue for resource utilization and pollution control. Present study proposed a new strategy to design non-ionic deep eutectic solvents (DESs) using phenolic analogues. Several phenol-based DESs with multiple acidic sites were constructed by paring catechol (Cat) or resorcinol (Res) with phenol (PhOH) and investigated as feasible NH 3 absorbents from physical property, NH 3 absorption performance, and mechanism analysis. Among the as-obtained DESs, Res/PhOH (1:3) demonstrated attractive NH 3 absorption capacity at 303.15 K (11.862 mol/kg at 101.3 kPa, and 6.391 mol/kg at 5.0 kPa), surpassing most DESs and ionic liquids (ILs) reported in the literatures. Meanwhile, it displayed good reversibility, satisfactory thermal stability, and high NH 3 /CO 2 selectivity. The mechanism of NH 3 absorption was further elucidated using FTIR and NMR spectra, and Quantum chemistry calculation, and inferred as the strong and multiple interaction between NH 3 and weakly acidic sites of DESs.
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ACS ES&T Water
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2023
·
IF 5.3
Jiayue Dong,Peizeng Yang,Gregory V. Korshin,Junhe Lu
Bromide (Br–) and nitrite (NO2–) can be transformed to brominated and nitrophenolic byproducts, respectively, in sulfate radical (SO4·–)-based oxidation processes, which has raised growing concern. In the present work, we examined the byproducts in the heat-activated persulfate oxidation system with the copresence of Br– and NO2–, finding that Br– acted as a catalyst to accelerate the NO2– transformation and nitrophenolic byproduct formation. Nitryl bromide (NO2Br) was the key intermediate in this process. It was generated by the reaction between NO2– and free bromine in situ formed as the product of the oxidation of Br– by SO4·–. As a strong nitrating agent, NO2Br reacted with natural organic matter directly, resulting in nitrophenolic byproducts. Alternatively, it reacted with excess NO2– to form N2O4, which hydrolyzed to NO3– ultimately. Both pathways were accompanied by releasing Br–. There was little Br– loss in the earlier reaction phase. Only after NO2– was completely transformed, brominated byproduct formation occurred. Thus, the transformations of Br– and NO2– are interweaved in SR-AOPs, which facilitates the formation of nitrophenolic byproducts but inhibits brominated byproducts. These new insights underscore the potential hazardous effects when SO4·– oxidation is applied under realistic environmental conditions.
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NEW JOURNAL OF CHEMISTRY
·
2023
·
IF 3.3
Yujie Zhang,Yingjiang Wang,Zhaohui Li,Lingbo Qu,Lanlan Yu
Nanozymes, which possess similar catalytic activities to natural enzymes, are considered promising alternatives to natural enzymes. In the present study, a new bimetallic Fe/Mn metal–organic framework (MOF) nanomaterial was synthesized by doping Mn in MIL-101(Fe). Despite the low doping amount of Mn, the Fe/Mn MOF displayed remarkably enhanced peroxidase-like activity, catalyzing the conversion of chromogenic substrate ABTS to blue-green ABTS˙+. Subsequently, the addition of environmental pollutant aminophenol isomers induced different color changes in a solution, which provided a simple and feasible approach to differentiate them by the naked eyes. Based on the effect of aminophenol isomers on the absorption spectrum of ABTS˙+, colorimetric methods were developed to quantitatively determine m-AP and p-AP with detection limits of 0.13 μM and 0.20 μM, respectively. Furthermore, taking advantage of a smart phone software-color recognizer to analyze the RGB value, a rapid detection method for m-AP was proposed, offering a solution to detect m-AP in the absence of any analytical instruments. This work verified the essential role of doping Mn in enhancing the enzyme-like activity of nanozymes. Simultaneously, the proposed simple, rapid, and accurate sensing method provided a new option to differentiate and determine aminophenol isomers, which has great potential for environmental application.
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iScience
·
2023
·
IF 5.8
Yuanyuan Zhang,Jie Zheng,Shiraku Margaret Linyerera,Richard Odongo Magwanga,Yuqing Hou,Yuhong Wang,Yanchao Xu,Aziz Khan,Shuxun Yu,Zhongli Zhou,Fang Liu,Xiaoyan Cai
Summary The 5′-deoxyadenosine deaminase (DADD), a member of the amidohydrolase family regulates biological purine metabolism. In this study, bioinformatic analysis, overexpression and knockdown of GhdadD gene were detected to identify its potential role in drought and salt stress tolerance. The results revealed that GhdadD was induced by ABA, Auxin, MBS and light responsive elements. In transgenic Arabidopsis, seed germination rate and root length were increased under drought or salt stress. GhdadD overexpressed seedlings resulted in higher plant height, less leaf damage and lower ion permeability. The expression of osmotic stress and ABA-responsive genes were up regulated. While in GhdadD -silenced cotton seedlings, CAT, SOD activity and soluble sugar content were reduced, MDA content was increased, and the stoma opening was depressed under drought or salt stress. Some osmics stress marker genes were also up regulated. These data indicating that GhdadD enhanced plant resistance to drought and salt stress through ABA pathways.
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