JOURNAL OF HAZARDOUS MATERIALS
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2023
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IF 13.6
Guangrong Sun,Han Yeong Kaw,Meijiao Zhou,Pei Guo,Lizhong Zhu,Wei Wang
Identification of emerging disinfection byproducts (DBPs) of health relevance is important to uncover the health risk of drinking water observed in epidemiology studies. In this study, mutagenic chlorinated nucleotides were proposed as potential DBPs in drinking water, and the formation and transformation pathways of these DBPs in chlorination of nucleotides were carefully investigated. A total of eleven chlorinated nucleotides and analogs were provisionally identified as potential DBPs, such as monochloro uridine/cytidine/adenosine acid and dichloro cytidine acid, and the formation mechanisms involved chlorination, decarbonization, hydrolysis, oxidation and decarboxylation . The active sites of nucleotides that reacted with chlorine were on the aromatic heterocyclic rings of nucleobases, and the carbon among the two nitrogen atoms in the nucleobases tended to be transformed into carboxyl group or be eliminated, further forming ring-opening or reorganization products. Approximately 0.2–4.0 % (mol/mol) of these chlorinated nucleotides and analogs finally decomposed to small-molecule aliphatic DBPs, primarily including haloacetic acids, trichloromethane, and trichloroacetaldehyde. Eight intermediates, particularly chlorinated imino- D -ribose and imino- D -ribose, were tentatively identified in chlorination of uridine. This study provides the first set of preliminary evidence for indicating the promising occurrence of chlorinated nucleotides and analogs as potential toxicological-relevant DBPs after disinfection of drinking water.
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International Journal of Nanomedicine
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2023
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IF 8
Ying Chen,Lei Zhang,Fangxuan Li,Jindong Sheng,Changxiao Xu,Dan Li,Hu Yu,Wenxin Liu
Introduction Photodynamic therapy (PDT) has been widely researched by cancer therapists in recent years. This study aims to establish a drug delivery system combining PDT and chemotherapy to show that chemotherapeutic drugs provide oxygen to PDT, while PDT promotes the release of chemotherapeutic drug.Methods Firstly, poly(ethylene glycol)-lysine(Ce6)-block-poly(L-glutamate)-imidazole (mPEG-lys(Ce6)-PGA-AIM) was synthesized and self-assembled into micelles that exhibited pH- and ROS-responsiveness and buffering capacity. Perfluorohexanoate-modified cisplatin (FCP), as oxygen carriers, was encapsulated into mPEG-lys(Ce6)-PGA-AIM micelles. Then, the properties of micelles and their biological functions in vivo and in vitro were investigated.Results The micelles exhibited remarkabe stability, pH regulated drug release, good biocompatibility and effective tumor penetration. Cellular uptake demonstrated the efficient endosome/lysosome escape of CFMs, which facilitates the intracellular drug release. Both in vitro and in vivo experiments reflected that CFMs with laser irradiation showed significantly improved therapeutic activity compared with single PDT or chemotherapy.Conclusion Chemotherapy and PDT were combined in the form of mutual assistance to provide a promising strategy for clinical treatment.
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Catalysts
·
2023
·Vol. 13
·期 5
·799
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IF 3.9
Tao Wang,Jie Li,Hanwen Yan,Guoliang Zhang,Shifeng Li
Methacrolein (MAL) is an important intermediate extensively used in the manufacture of methyl methacrylate and other materials (polymers and resins). In this study, a series of secondary amines/acids were explored as catalysts for the condensation of formaldehyde and propionaldehyde to prepare MAL. It was found that the structure of the amines and acids directly affected the yield of MAL. The effect of the catalyst was closely related to the nucleophilicity of the amines as well as the steric hindrance effect, while acids also played a role as co-catalysts. Dibutylamine acetate was selected as the catalyst after investigation. The catalytic performance of the system was systematically studied by a series of single-factor experiments, including stirring rate, temperature, reaction time, acid/amine ratio, and the solvent, and the optimized reaction conditions were obtained. In the optimum condition, the yield of MAL was up to 97.3%. Kinetic experiments were performed for the condensation of formaldehyde and propionaldehyde to MAL, and the activation energies, reaction orders, and rate-limiting step of the reaction were determined. The results indicate that the decomposition of the Mannich base is a rate-limiting step.Keywords:methacrolein;aldol condensation;Mannich reaction;kinetics
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ACS Sustainable Chemistry & Engineering
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2022
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IF 9.224
Dazhen Xiong,Yang Wang,Huihui Ma,Lige Lu,Qian Zhang,Yunlei Shi,Yang Zhao,Jianji Wang
5-Hydroxymethylfurfural (HMF) is a key biobased platform compound for the production of high-value chemicals and fuels. However, separation and purification of HMF is currently the bottleneck for HMF production. In this work, a novel class of temperature-responsive deep eutectic solvent (DES)–water systems have been explored to selectively separate HMF from reaction mixtures. The fructose dehydration reaction was conducted in homogeneous DES–H2O systems, and then, the produced HMF was migrated to the DES-rich phase while the unreacted fructose was retained in the H2O-rich phase upon cooling. Thus, selective separation of HMF was realized. It was found that water–water and DES–DES interactions predominate over DES–water interactions during cooling, thus resulting in upper critical solution temperature phase separation. Under optimal conditions, the partition coefficient and separation factor of HMF could reach up to 78 and 609, respectively, which is about 5 and 13 times those reported in ionic liquid-based aqueous biphasic systems. Furthermore, HMF could be removed from the DES-rich phase, giving a high recovery efficiency of 69%, which is much higher than the best value reported in the literature. At the same time, DES was regenerated and reused in the next process, and no obvious decrease in partition coefficient of HMF was observed after six cycles.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2023
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IF 8.2
Jiabao Qiu,Shuai Yuan,Honggang Xiao,Jinfu Liu,Tao Shen,Zhuotao Tan,Wei Zhuang,Hanjie Ying,Ming Li,Chenjie Zhu
Lignin-based hybrid fillers are of increasing importance with regards to the valorization of low-value biomass and the requirement of sustainability in rubber industry, however, a facile lignin modification approach tuning the supramolecular interactions to favor the assembly of the hybrids is in demand. This study aimed to design a lignin/SiO 2 nano-hybrid via an in-situ assembly of diethylamine grafted lignin (DL) and SiO 2 , and investigate its reinforcing effect on natural rubber (NR). DL was prepared through Mannich modification of lignin, and the grafted diethylamine can be clearly identified by FTIR, NMR and elemental analysis. The resultant hybrid (DLSi) displays as homogeneous nanospheres with well integrated DL and SiO 2 components as shown in the TEM images, and the hybrid (DLSi1) prepared with weight ratio of DL/SiO 2 = 1/2 shows a minimum particle size of 101.8 nm and significantly reduced polarity. Compared to the reference composite filled only with carbon black (CB), NR composites filled with DLSi/CB of 10/40 phr shows comparable mechanical properties and reduced rolling resistance, which is due to the low particle size, homogenous dispersion and strong rubber-filler interfacial affinity. Such remarkable performance suggests that the DLSi hybrid can be a promising versatile biobased filler for the application in gasoline-saving “green” tires.
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JOURNAL OF CHROMATOGRAPHY A
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2022
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IF 4.601
Qifang He,Qian Lei,Shaoquan Huang,Yufang Zhou,Yuqin Liu,Sujin Zhou,Dong Peng,Xiulong Deng,Jun Xue,Xun Li,Hongdeng Qiu
The efficient and green extraction of bioactive ingredients from natural plants play a vital role in their corresponding drug effects and subsequent studies. Recently, deep eutectic solvents (DESs) have been considered promising new green solvents for efficiently and selectively extracting substances from varied plants. In this work, an environment-friendly DESs-based ultrasonic-assisted extraction (DESs-UAE) procedure was developed for highly efficient and non-polluting extraction of alkaloids from the roots of Stephania tetrandra (ST). A total of fifteen different combinations of DESs, compared with traditional organic solvents (methanol and 95% ethanol) and water, were evaluated for extraction of bioactive alkaloids (FAN and TET) from ST, and the results revealed that DESs system made up of choline chloride and ethylene glycol with mole ratio of 1:2 exhibited the optimal extraction efficiency for alkaloids. Additionally, a four-factor and three-level Box-Behnken design (BBD), a particular pattern of response surface methodology (RSM), was used to optimize extraction conditions. RSM results indicated that the maximum extraction yields of FAN, TET, and TA were attained 7.23, 13.36, 20.59 mg/g, respectively, within extraction temperature of 52 °C, extraction time of 82 min, DES water content of 23% (v/v), and liquid-solid ratio of 23 mL/g. The measured results were consistent with the predicted values. Notably, the optimized DES extraction efficiency of TA, according to the experimental data analysis, is 2.2, 3.3 and 4.1 times higher than methanol, 95% ethanol and water, respectively. Meanwhile, based on 3D response surface plots, interactive effects plots and contour maps, the effects of the aforementioned four essential factors on the extraction yield and their interactions on the response were visualized. The results revealed that the mutual interactions between extraction temperature and liquid-solid ratio exhibited positive effects on all responses, while extraction time and water content in DES posed a negative effect. Therefore, these results suggest that DESs, as a class of novel green solvents, with the potential to substitute organic solvent and water, can be widely and effectively applied to extract bioactive compounds from natural plants.
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Materials Today Bio
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2022
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IF 10.761
Zunhan Hu,Wenzhen Wu,Meizhe Yu,Zhi Wang,Zhenyu Yang,Xiaodong Xing,Xiaofang Chen,Lina Niu,Fan Yu,Yuhong Xiao,Jihua Chen
Mussels can form tough and long-lasting adhesions to organic and inorganic surfaces in saline and impactive severe aquatic environments. Similar to mussel adhesion, dentin bonding occurs in a wet environment. However, unlike mussels, it is difficult to achieve long-lasting bonds with dentin. Moreover, water is considered a major hindrance in dentin bonding. Inspired by the synergistic effect of cationic lysine (Lys) and catechol on the elimination of the hydration layer during mussel adhesion, a catechol- and Lys-functionalized polymerizable polymer (catechol–Lys–methacrylate [CLM]) was synthesized to replicate the complex synergy between amino acids and catechol. The bond-promoting potential of 5 mg/mL CLM primer was confirmed using an in vitro wet dentin-bonding model, which was characterized by an improvement in bond strength and durability. CLM can adhere to wet demineralized dentin, with Lys acting as a molecular vanguard to expel water. Subsequently, a myriad of interfacial interactions can be obtained by introducing the catechol group into the interface. Additionally, tough and long-lasting adhesion, similar to that formed by mussels, can be achieved by grafting CLM onto type I collagen via covalent bonds, hydrogen bonds, Van der Waals interactions, and cation–π interactions, which can enhance the mechanical and chemical stability of collagen, increase the enzymatic resistance of collagen, and provide additional physical/chemical adhesion to dentin bonds. Catechol- and cationic Lys-functionalized polymers can improve the stability of the resin–dentin interface under wet conditions.
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Reaction Chemistry & Engineering
·
2022
·Vol. 8
·期 3
·645-655
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IF 5.2
Zhenhua Tian,Jianzhong Ma,Qiwu Liu,Hui Zhang
Amphoteric acrylic polymers are some of the commonly used leather retanning agents, and possess assistant-dyeing function in contrast to traditional anionic acrylic retanning agents. To further enhance the cationic modification degree of anionic acrylic retanning agents, various amines (dimethylamine, diethylamine, dipropylamine, diethanolamine, dicyclohexylamine and diphenylamine) with different structural characteristics were selected as raw materials to prepare amphoteric acrylic retanning agents via the Mannich reaction. Then, the obtained amphoteric acrylic retanning agents were used in leather-making, and the retanning and assistant-dyeing properties were investigated. Compared with the anionic acrylic retanning agents, all amphoteric acrylic retanning agents have better assistant-dyeing owing to the presence of amino groups. The retanning agents modified by different amines exhibit different properties. The amination degree of the acrylic polymer retanning agent modified by diethanolamine was the highest (40.8%) and had better assistant-dyeing, which was confirmed by its highest dye-uptake (87.5%) and K/S value (17.0). The tensile strength of leather retanned with diphenylamine-modified acrylic polymer was the highest (23.6 MPa). The thickening rate of the leather retanned with dipropylamine-modified acrylic polymer was the highest (23.8%). Considering these properties, the overall performance of the amphoteric acrylic polymer modified by diethanolamine was found to be the best.
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Sustainable Chemistry and Pharmacy
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2023
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IF 6
Qingli Zhu,Xiao Chen,Heng Gu,Zhi Yun
With the rapid increasing of environmental pollution concerns and declining petroleum assets, bio-based lubricants industry has aroused increasingly more attention and study. The present paper proposed two methods (a two-step process and a direct hydrosiylation process) for the production of biolubricant from soybean oil with organosilicon. At first, soybean oil was subjected to transesterification with potassium hydroxide under certain conditions. Then, the transesterified soybean oil was undergone urea inclusion for obtaining unsaturated fatty acid methyl esters (UFAMEs). After urea inclusion, the content of UFAMEs was increased to 88.1%. Next, the chemical modification of UFAMEs by the two-step process (epoxidation and ring-opening reaction) and the direct hydrosiylation process (with triethylsilane in present of catalyst) were systematically studied, respectively. With the optimal conditions, the conversions of UFAMEs in the two-step process and direct hydrosiylation process were 86.1% and 82.1%, respectively. In addition, the structure characteristics of material and products were determined by Fourier-transformed infrared (FTIR) spectroscope and 29 Si-Nuclear magnetic resonance ( 29 Si-NMR) spectrascopy. The lubrication performances of the two products were proved to be much better than soybean oil according to industry standards. Therefore, both of the two processes appeared to be feasible for bio-lubricant production.
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Nano-Micro Letters
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2023
·Vol. 15
·期 1
·1-9
·
IF 26.6
Wang Yuhan,Ren Yanxiong,Cao Yu,Liang Xu,He Guangwei,Ma Hanze,Dong Hongliang,Fang Xiao,Pan Fusheng,Jiang Zhongyi
For the first time, the hydrogen-bonded organic frameworks (HOFs)-based mixed-matrix membranes were designed for CO2 separation
A size-controllable method for synthesis of HOF-21 nanoparticles was proposed via diethylamine-modulated framework assembly process
The HOF-21 mixed-matrix membranes exhibited outstanding separation performance with PCO2 of ~ 800 Barrer, and SCO2/CH4 of ~ 40, SCO2/N2 of ~ 60, surpassing the 2008 Robosen upper bound.
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ACS Sustainable Chemistry & Engineering
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2023
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IF 8.4
Jian-Dong Wang,Qi Gu,Zi-Hui Cai,Guo-Sheng Liu,Quan Zhou,Li-Na Fu,Shi-Liang Yang,Su Zhang,Yujie Fu
In this study, a green CO2-responsive switchable hydrophilic solvent (SHS) was screened in the strategy of extracting and enriching active components with different polarities from a plant matrix. The mechanism of solvent switching was confirmed by Fourier transform infrared spectroscopy (FT-IR) and nuclear magnetic resonance (NMR) spectroscopy. Furthermore, the function of SHS polarity switching was proven by Kamlet–Taft parameters, and the polarity parameter π* of the solvent increased from 0.34 to 1.01 after introducing CO2. The solvent system was used to extract the active ingredients from Rosa roxburghii; a series of single factor experiments were conducted using the Box-Behnken design in order to optimize the process. In addition, the phenomenon of the SHS/water two-phase system being heated by ultrasound to produce an O/W micellar system was observed, which provided solvent solubilization. Moreover, after 5 cycles, the solvent still ensured a high extraction capacity of the target components. In addition, density functional theory (DFT) and molecular dynamics theory revealed that van der Waals forces and hydrogen bonding made the SHS more biocompatible with the target compounds and that van der Waals forces played a significant impact. In conclusion, the current process offered an ecologically acceptable, promising, and long-term alternative approach for simultaneously extracting and enriching hydrophilic and hydrophobic phytochemicals from plant materials.
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SENSORS AND ACTUATORS B-CHEMICAL
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2023
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IF 8.4
Jialu Pan,Man Li,Feng Zhang,Xiaoran Wang,Yanqing Cong,Shi-Wen Lv
It is of great significance to exploit simple and efficient methods for detecting hazardous substances in the fields related to food safety and environmental protection. Herein, for the first time, a newly-designed hollow Co-N/C nanocage with oxidase-like activity was synthesized via a feasible method. Benefiting from the construction of hollow structure and the introduction of carbon layer , the specific surface area of enzyme mimic was improved, so exposing more active sites. Importantly, hollow Co-N/C nanocage displayed an excellent performance in interfacial charge transfer, which provided convenience for the occurrence of chromatic reaction between enzyme mimic and TMB . As predicted, hollow Co-N/C nanocage can effectively oxidize colorless TMB to blue oxTMB in the absence of H 2 O 2 , and the analyses about catalytic mechanism suggested that both the redox couples of Co 3+ /Co 2+ and O 2 •− were involved in the oxidation of TMB. Furthermore, a chromogenic sensing method for the detection of Na 2 SO 3 and Cr 6+ was exploited, and a broad linear range and a low LOD can be achieved. More interestingly, developed detection method still possessed good recovery even in real samples. In a word, current work will share novel insights into the design of enzyme mimics and the analyses on chromogenic mechanism.
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