PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
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2023
·Vol. 120
·期 13
·e2220792120
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IF 11.1
Junwei Zhang,Xikun Zhang,Chiwei Xu,Yiwen Liu,Jiaxi Xu,Zhonghao Miao,Haoxiang Yu,Lei Yan,Liyuan Zhang,Jie Shu
Selenium sulfide (SeS2) features higher electronic conductivity than sulfur and higher theoretical capacity and lower cost than selenium, attracting considerable interest in energy storage field. Although nonaqueous Li/Na/K-SeS2 batteries are attractive for their high energy density, the notorious shuttle effect of polysulfides/polyselenides and the intrinsic limitations of organic electrolyte have hindered the deployment of this technology. To circumvent these issues, here we design an aqueous Cu-SeS2 battery by encapsulating SeS2 in a defect-enriched nitrogen-doped porous carbon monolith. Except the intrinsic synergistic effect between Se and S in SeS2, the porous structure of carbon matrix has sufficient internal voids to buffer the volume change of SeS2 and provides abundant pathways for both electrons and ions. In addition, the synergistic effect of nitrogen doping and topological defect not only enhances the chemical affinity between reactants and carbon matrix but also offers catalytic active sites for electrochemical reactions. Benefiting from these merits, the Cu-SeS2 battery delivers superior initial reversible capacity of 1,905.1 mAh g−1 at 0.2 A g−1 and outstanding long-span cycling performance over 1,000 cycles at 5 A g−1. This work applies variable valence charge carriers to aqueous metal–SeS2 batteries, providing valuable inspiration for the construction of metal–chalcogen batteries.
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ACS Applied Nano Materials
·
2023
·
IF 5.9
Mingjie Han,Yuhao Xu,Ri Wang,Yong Xie,Yuekun Wang,Chao Bian,Shanhong Xia
Mercury ions (Hg2+) are highly toxic, which can contaminate the environment and cause serious harm to human health. In this work, we report a portable, high-performance, and reusable boron-doped diamond (BDD) electrochemical sensor, which takes the advantages of 4-mercaptopyridine-functionalized gold nanoparticles (4-MPY/Au NPs) as the sensing element. Due to the specific coordination between Hg2+ and nitrogen of pyridine, Hg2+ can be captured by the 4-MPY to form a Hg(pyridine)2 complex, which leads to the reduction of electrochemical activity at the electrode surface. The current variations are monitored by differential pulse voltammetry (DPV) in solution containing the [Fe(CN)6]3–/4– redox probe. Under optimal conditions, the proposed sensor exhibits an excellent logarithmic relationship in the range of 0.001–10 μg/L with a low limit of detection (LOD) of 0.358 ng/L. In addition, the sensor is validated with satisfactory recovery of tap water samples, demonstrating its potential for on-site monitoring of the water environment.
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Molecular Catalysis
·
2023
·
IF 4.6
Chan Meng,Heming Zhang,Qian Su,Hanwen Yan,Changyuan Du,Yunong Li,Li Dong,Weiguo Cheng
In view of the harsh conditions of cyclic esterification reaction of ethylene glycol (EG) and carbon dioxide (CO 2 ) to synthesize ethylene carbonate (EC), the yield is low and the catalysts are mostly metals, a series of green acid-base bicentric ionic liquids (ABbILs) were developed. Among them, the ABbILs of 1,5,7-Triazabicyclo[4.4.0]dec‑5-ene glutarimide ([TBDH][Glu]) had the best catalytic performance. Under the optimal reaction conditions, the yield of EC reached 29.5%, which was higher than most of the conventional metal-based catalysts. Through activity screening results and DFT calculation, it was found that different cations affect the interaction between N on anion and H proton of EG, and the H on the cation can activate the O on EG, which would affect the ability of ABbILs to activate EG. The acid-base bicentered synergistic catalytic mechanism of Bronsted acid and Lewis base was proposed by characterization and DFT calculation. This study opens up new avenues for the efficient conversion of diols and CO 2 for the preparation of cyclic carbonates.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2023
·
IF 4.2
Dandan Jin,Jinyue Dai,Liyue Zhang,Qing Chen,Xiaoqing Liu
To overcome the high flammability and brittleness of epoxy resin (EP) without sacrificing its glass transition temperature (Tg) and mechanical properties, a series of hyperbranched benzoxazines (HB1.0–HB2.5) were synthesized using 6-(bis(4-hydroxyphenyl)methyl)dibenzo[1,2]oxaphosphinine 6-oxide (DOPO-2OH) as the “hard” segment and Jeffamine T403 as the “soft” segment. The property investigation revealed that HB2.0 with the optimized ratio of “hard/soft” segments was the appropriate additive for commercial EP. Furthermore, the comprehensive performance of the EP/HB2.0 system was significantly enhanced compared to the pristine EP, demonstrating a 115% increase in impact strength and 5.7 °C in Tg. Impressively, when the loading of HB2.0 was only 10 phr (phosphorus content is 0.34 wt %), the modified EP passed the UL-94 V-0 rating and achieved a limited oxygen index (LOI) value of 30.8%, mainly resulting from the flame inhibition effect of the gaseous phase. This research provided an appealing technique for simultaneously improving the toughness and flame retardancy of EP.
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JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Liwei Yang,Fashan Yang,Heng Zhang,Hongyu Zhou,Mengfan Luo,Yunmei Liu,Chuanliang Zhao,Lu Zheng,Bo Lai
At present, the potential mechanism of manganese oxide (MnO 2 ) activation of PI and the key active sites of PI activation are still unclear and controversial. To this end, three different crystal forms of MnO 2 were prepared in this study and used to activate PI to degrade pollutants. The results showed that different crystal types of MnO 2 showed different catalytic abilities, and the order was γ-MnO 2 > α-MnO 2 > β-MnO 2 . Through quenching experiments, EPR tests, Raman experiments and in situ electrochemical experiments, it has been confirmed that electron transfer-mediated non-free radical process is the main mechanism of pollutant degradation , in which the active substance is the highly active metastable intermediate complex (MnO 2 /PI*). Hydroxyl radical (HO • ), superoxide radical (O 2 •− ), singlet oxygen ( 1 O 2 ) and iodine radical (IO 3 • ) did not participate in pollutant degradation. The quantitative structure-activity relationship analysis confirmed that the catalytic performance of MnO 2 was highly positively correlated with the surface Mn(IV) content, which indicated that the surface Mn(IV) site was the main active site. Overall, this study will be of great help to the design and application of manganese dioxide activation for periodate degradation of pollutants.
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FITOTERAPIA
·
2023
·
IF 3.4
Dan Huang,Fanghua Li,Anquan Yang,Jing Wang,Min Xie,Meiling Mao,Jing Li,Xiaoli Zhang,Qingli Qu,Ranhua Xiong,Chaobo Huang
The study on the extraction conditions, purification, and biological activity of slash pine ( Pinus elliottii. ) is important for the development of slash pine resources. The optimal process conditions for the extraction of slash pine polysaccharide (SPP) were determined, resulting in a liquid-solid ratio of 66.94 mL/g, extraction temperature of 83.74 °C and extraction time of 2.56 h by using the response surface methodology, and the yield of SPP was 5.99% under the optimized conditions. Following the purification of SPP, the SPP-2 component was obtained and its physicochemical properties, functional group composition, antioxidant capacity, and moisturizing capacity were determined. Structural analysis suggested that SPP-2 has a molecular weight of 118.407 kDa, and was composed of rhamnose, arabinose, fucose, xylose, mannose, glucose, and galactose in a ratio of 5.98: 14.34: 1: 1.75: 13.50: 3.43: 15.79. The antioxidant activity analysis showed that SPP-2 has good free radical scavenging activity, and it was also found to have in vitro moisturizing activity and low irritation. These results suggest that SPP-2 has the potential for applications in the pharmaceutical, food, and cosmetic industries.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Zhipeng Qie,Zhaoqi Ji,Huan Xiang,Xinhan Zhang,Abdullah Alhelali,Lan Lan,Hassan Alhassawi,Guangbo Zhao,Xiaoxia Ou,Xiaolei Fan
Adsorption capacity of zeolitic adsorbents for organic pollutants can be affected severely under humid conditions and/or in aqueous systems. This study presents the development of hydrophobic Beta zeolites using a microwave-assisted post-synthetic treatment method (i.e., microwave-assisted chelation, MWAC) for adsorption removal of organics (benzene and phenol as the models) in aqueous systems. MWAC treatment enabled the dealumination of Beta zeolites in only one minute whilst increasing its hydrophobicity. Based on the characterization data, the mechanism for the hydrophobization of Beta zeolite was proposed. The influence of hydrophobicity, porosity and the property of organic molecules on adsorption behaviours were systematically studied, showing that the most hydrophobic Beta zeolite presented the highest benzene adsorption capacity per surface area of 2.87 × 10 −3 mmol/m 2 (at 1.0 g/L initial concentration). TGA and multi-cycle regeneration/adsorption experiments were employed to assess the regeneration and reusability of the adsorbents, and the results suggested that the modified Beta zeolites could be regenerated easily with the preserved physiochemical properties and adsorption capacity. The developed method and the associated zeolitic materials could be developed further for making high-performance hydrophobic zeolitic adsorbents for applications in organics removal from aqueous media.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Jinxin Li,Dan Zhong,Feiyu Li,Kefei Li,Wencheng Ma,Jun Ma,Jingna Zhang,Aoshuang Sun
A bifunctional electro-Fenton (EF) cathode with Fe 3 O 4 -LaFeO 3 /C embedded graphite felt (GF) was synthesized through a hydrothermal process, which was used for in situ electrochemical formation of active oxygen species (ROS) for coal pyrolysis wastewater (CPW) removal. Experimental results illustrated that the mineralization efficiency of dimethylphenol (DMP) was achieved at 90.7 % within 150 min reaction. On the basis of quenching test and free radical detection, the ∙OH and ∙O 2 − were the detectable ROS in the hetero-EF system for DMP removal. Meanwhile, the formed oxygen vacancies (OVs) and the redox of Fe 2+ /Fe 3+ promoted the oxygen adsorption and H 2 O 2 activation. Density functional theory (DFT) calculations further discussed that the Fe 3 O 4 -LaFeO 3 interface possessed more downward spin density of states in the conduction band, resulting in a higher total density of states (DOS) value near the Fermi level. Moreover, the Fe 3 O 4 -LaFeO 3 /C/GF cathode displayed good recyclability with low metal ion dissolution for 5 times (99.5 % DMP removal and 78.6 % TOC removal) and underlying actual CPW application potential (80.2 % of COD removal and 100 % of total phenol (Tph) removal). Overall, this work invented a novel and stable bifunctional cathode for the efficient removal of refractory CPW in the hetero-EF system.
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Foods
·
2023
·Vol. 12
·期 11
·2151
·
IF 5.2
Baorong Chen,Xiaodan Wang,Yumeng Zhang,Wenyuan Zhang,Xiaoyang Pang,Shuwen Zhang,Jing Lu,Jiaping Lv
This study aimed to determine chemical composition and assess exposure in flavored milk among Chinese residents, based on risk assessment methodologies of acceptable daily intake (ADI) and toxicological concern threshold (TTC). Esters (32.17%), alcohols (11.19%), olefins (9.09%), aldehydes (8.39%), and ketones (7.34%) comprised the majority of the flavoring samples. Methyl palmitate (90.91%), ethyl butyrate (81.82%), and dipentene (81.82%) had the highest detection rates in flavor samples. This study screened fifteen flavor components of concern and discovered that 2,3,5-trimethylpyrazine, furfural, benzaldehyde, and benzenemethanol were detected in 100% of flavored milk samples. Benzenemethanol was found in the highest concentration (14,995.44 μg kg−1). The risk assessment results revealed that there was no risk for Chinese residents in consuming flavored milk, and the maximum per capita daily consumption of 2,3,5-trimethylpyrazine, furfural, and benzenemethanol were 226.208 g, 140.610 g, and 120.036 g, respectively. This study could provide guidelines for amounts of flavor additive ingredients in milk.Keywords:flavored milk;SPME-GC/MS;flavor components;acceptable daily intake;toxicological concern threshold
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2023
·
IF 8.2
Xiaoli Zhang,Qingli Qu,Anquan Yang,Jing Wang,Weixia Cheng,Aying Zhou,Ranhua Xiong,Chaobo Huang
Bacterial infections pose a serious threat to public health, causing worldwide morbidity and about 80 % of bacterial infections are related to biofilm. Removing biofilm without antibiotics remains an interdisciplinary challenge. To solve this problem, we presented a dual-power driven antibiofilm system Prussian blue composite microswimmers based on alginate-chitosan, which designed into an asymmetric structure to achieve self-driven in the fuel solution and magnetic field. Prussian blue embedded in the microswimmers given it the ability to convert light and heat, catalyze Fenton reaction, and produce bubbles and reactive oxygen species. Moreover, with the addition of Fe 3 O 4 , the microswimmers could move in group under external magnetic field. The composite microswimmers displayed excellent antibacterial activity against S. aureus biofilm with an efficiency as high as 86.94 %. It is worth mentioning that the microswimmers were fabricated with device-simple and low-cost gas-shearing method. This system integrating physical destruction, chemical damage such chemodynamic therapy and photothermal therapy, and finally kill the plankton bacteria embedded in biofilm. This approach may cause an autonomous, multifunctional antibiofilm platform to promote the present most areas with harmful biofilm difficult to locate the surface for removal.
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Foods
·
2023
·Vol. 12
·期 11
·2160
·
IF 5.2
Si Li,Fangwei Liu,Mulan Wu,Yuhao Li,Xiaoxiao Song,Junyi Yin
In this study, different drying methods, including hot air drying, sun drying, and freeze drying were employed to dry fresh broad beans. The nutritional composition, volatile organic components and bioactive substances of the dried broad beans were systematically compared. The results indicated significant differences (p< 0.05) in nutritional composition, such as protein and soluble sugar content. Among the 66 identified volatile organic compounds, freeze drying and hot air drying significantly promote the production of alcohols and aldehydes, while sun drying effectively preserves esters. In terms of bioactive substances, broad beans dried by freeze drying exhibit the highest total phenol content as well as the strongest antioxidant capacity and gallic acid, followed by sun drying. The chemometric analysis revealed that the bioactive compounds in broad beans dried by three different methods were primarily composed of flavonoids, organic acids, and amino acids with significant differentiation. Notably, freeze-dried and sun-dried broad beans exhibited a higher concentration of differential substances.Keywords:broad beans;drying method;nutrition composition;bioactive substances
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SENSORS AND ACTUATORS B-CHEMICAL
·
2023
·
IF 8.4
Jizhong Wu,Wenya Wei,Muhammad Zareef,Shuhua Li,Qin Ouyang,Quansheng Chen
Bisphenol A (BPA) is an endocrine disrupting chemical having estrogenic properties that can enter the body through leaking from food containers or the food chain. An upconversion nanoparticle-based aptasensor integrated with microfluidic chip was simply designed to achieve the determination of BPA in foodstuff. Core-shell structured upconversion nanoparticles with 6.41-fold luminescence enhancement were used as fluorescence donors and gold nanoparticles as fluorescence acceptors to construct fluorescence resonance energy transfer (FRET) system. The BPA aptamer serves as a link between the building of the FRET system and the BPA-specific recognition component. The fishbone-structured microfluidic chip only needs 0.5 μL sample solution and 4 min to determine the presence of BPA. The proposed method has good linearity for BPA in the range of 0.02–100 ng/mL with calibration curve of y = 0.0918 x + 0.6477 and limit of detection of 0.014 ng/mL. It is tremendously competitive to perform on-chip analysis that enables microsampling and rapid determination.
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危险品化学品经营许可证（带存储）