Your browser doesn't support javascript.
loading
Mostrar: 20 | 50 | 100
Resultados 1 - 20 de 340
Filtrar
2.
Adv Mater ; : e2401539, 2024 Mar 29.
Artigo em Inglês | MEDLINE | ID: mdl-38549454

RESUMO

Viscous biofluids on wounds challenge conventional "water-absorbing" wound dressings in efficient drainage due to their poor fluidity, generally causing prolonged inflammation, anti-angiogenesis, and delayed wound closure. Herein, it is reported that a self-pumping organohydrogel dressing (SPD) with aligned hydrated hydrogel channels, prepared by a three-dimensional-templated wetting-enabled-transfer (3D-WET) polymerization process, can efficiently drain viscous fluids and accelerate diabetic wound healing. The asymmetric wettability of the hydrophobic-hydrophilic layers and aligned hydrated hydrogel channels enable unidirectional and efficient drainage of viscous fluids away from the wounds, preventing their overhydration and inflammatory stimulation. The organogel layer can adhere onto the skin around the wounds but can be easily detached from the wet wound area, avoiding secondary trauma to the newly formed tissues. Taking a diabetic rat model as an example, the SPD can significantly downregulate the inflammation response by ≈70.8%, enhance the dermal remodeling by ≈14.3%, and shorten wound closure time by about 1/3 compared with the commercial dressing (3M, Tegaderm hydrocolloid thin dressing). This study sheds light on the development of the next generation of functional dressings for chronic wounds involving viscous biofluids.

3.
Chemistry ; 30(24): e202304349, 2024 Apr 25.
Artigo em Inglês | MEDLINE | ID: mdl-38308610

RESUMO

Supramolecular reversible adhesives have garnered significant attention due to their potential applications in various fields. These adhesives exhibit remarkable properties such as reversible adhesion, self-healing, and high flexibility. This concept aims to present a comprehensive overview of the current research progress in developing supramolecular reversible adhesives. Firstly, the fundamentals of supramolecular chemistry and the principles underlying the design and synthesis of reversible adhesive systems are discussed. Next, the concept focuses on characterizing the reversible adhesion strength of supramolecular adhesive systems that have been developed. The adhesion performance of supramolecular reversible adhesives is summarized, highlighting their unique characteristics and promising applications. Finally, the challenges and future perspectives in the field of supramolecular reversible adhesives are discussed. The comprehensive overview provided in this concept aims to inspire further research and innovation in this exciting field.

4.
Angew Chem Int Ed Engl ; 63(8): e202318368, 2024 Feb 19.
Artigo em Inglês | MEDLINE | ID: mdl-38165266

RESUMO

Inspired by the drawstring structure in daily life, here we report the development of a drawstring-mimetic supramolecular complex at the molecular scale. This complex consists of a rigid figure-of-eight macrocyclic host molecule and a flexible linear guest molecule which could interact through three-point non-covalent binding to form a highly selective and efficient host-guest assembly. The complex not only resembles the drawstring structure, but also mimics the properties of a drawstring with regard to deformations under external forces. The supramolecular drawstring can be utilized as an interlocked crosslinker for poly(methyl acrylate), and the corresponding polymer samples exhibit comprehensive enhancement of macroscopic mechanical performance including stiffness, strength, and toughness.

5.
Dalton Trans ; 53(3): 1031-1039, 2024 Jan 16.
Artigo em Inglês | MEDLINE | ID: mdl-38088793

RESUMO

Efficient and durable electrocatalysts for the oxygen evolution reaction (OER) play an important role in the use of hydrogen energy. Rutile RuO2, despite being considered as an advanced electrocatalyst for the OER, performs poorly in stability due to its easy oxidative dissolution at very positive (oxidizing) potentials. Herein, we report a type of Co-doped RuO2 nanoparticle for boosting OER catalytic activity and stability in alkaline solutions. The replacement of Ru by Co atoms with a lower ionic valence and smaller electronegativity can promote the generation of O vacancies and increase the electron density around Ru, thus enhancing the adsorption of oxygen species and inhibiting the peroxidative dissolution of RuO2 during the OER process. It was found that Ru0.95Co0.05Oy exhibited excellent OER performance with overpotentials as low as 217 mV at 10 mA cm-2 and 290 mV at 100 mA cm-2 in 1 M KOH, as well as outstanding stability in continuous testing for 50 h at a current density of 100 mA cm-2, and nearly no significant degradation after the accelerated durability test of 2000 cycles.

6.
Analyst ; 149(2): 376-385, 2024 Jan 15.
Artigo em Inglês | MEDLINE | ID: mdl-38047398

RESUMO

Ag lattice doped In2O3 with a mesoporous structure was synthesized through a combination of hydrothermal and calcination methods. The structural and morphological characteristics were assessed using XRD, SEM, TEM, TGA, BET, and XPS analyses. Gas sensing measurements revealed that the 7.0 mol% Ag-doped In2O3 sensor displayed a response of 420 towards 100 ppm ethanol at 140 °C, which was 19 times higher than that of the pure In2O3 gas sensor. Density functional theory calculations indicated that Ag-doped In2O3 exhibited enhanced adsorption performance, higher adsorption energy, and electron transfer, resulting in higher sensitivity to ethanol. These findings were also supported by the electronic band structure, work function, and DOS analyses. These results indicated that the Ag doped mesoporous In2O3 has high potential for the preparation of high-performance ethanol sensors in practical applications.

7.
J Colloid Interface Sci ; 657: 208-218, 2024 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-38039881

RESUMO

Molybdenum carbide materials with unique electronic structures have received special attention as water-splitting catalysts, but their structural stability in the alkaline water electrolysis process is not satisfactory. This study reports an in situ pyrolysis method for preparing NiMo-based metal-organic framework (MOF)-derived chain-mail oxygen evolution reaction (OER) electrocatalysts and bamboo-like N-doped carbon nanotube (NCNT)-encapsulated Ni-doped MoC nanoparticles (NiMoC-NCNTs). The NCNTs can provide chain mail shells to protect the inner highly reactive Ni-doped MoC cores from electrochemical corrosion by the alkaline electrolyte and regulate their catalytic properties through charge redistribution. Benefiting from high N-doping with abundant pyridinic moieties and abundant active sites of the periodic bamboo-like nodes, the as-prepared NiMoC-NCNTs display an outstanding activity for the OER with an overpotential of 310 mV at 10 mA cm-2 and a superior long-term stability of 50 h. Density functional theory calculations reveal that the excellent electrocatalytic activity of NiMoC-NCNTs comes from the electron transfer from NiMoC nanoparticles to NCNTs, resulting in a decrease in the local work function at the carbon surface and optimized free efficiencies of OER intermediates on C sites. This work provides an effective approach to improve the structural stability of fragile catalysts by equipping them with carbon-based chain.

8.
J Colloid Interface Sci ; 656: 297-308, 2024 Feb 15.
Artigo em Inglês | MEDLINE | ID: mdl-37995400

RESUMO

Inducing the surface reconstruction of spinels is critical for improving the electrocatalytic oxygen evolution reaction (OER) activity. Herein, S-doped NiCo2O4 hollow cubic nanocage was synthesized by anion etching Metal-Organic Frameworks (MOFs) template and air annealing strategies. The hollow structure possesses a large specific surface area and pore size, facilitating active site exposure and mass transport. S2- doping regulates the electronic structure, reducing the oxidation potential of Ni sites during the OER process, thus promoting the surface reconstruction into γ-NiOOH active species. Meanwhile, S2- doping enhances conductivity, accelerating interfacial charge transfer. As a result, S-NiCo2O4-6 exhibits superior OER activity (262 mV overpotential @ 10 mA cm-2) and stability in 1.0 M KOH solution. Furthermore, 20 % Pt/C‖S-NiCo2O4-6 only needs 1.832 V to achieve 50 mA (the electrochemical active area is 4 cm2) in a homemade anion exchange membrane (AEM) electrolyzer. This work proposes a novel approach for preparing efficient anion-doped spinel-based OER electrocatalysts.

9.
J Colloid Interface Sci ; 658: 258-266, 2024 Mar 15.
Artigo em Inglês | MEDLINE | ID: mdl-38104408

RESUMO

Photoelectrocatalyzed hydrogen production plays an important role in the path to carbon neutrality. The construction of heterojunctions provides an ideal example of an oxygen precipitation reaction. In this work, the performance of the n-n type heterojunction CeBTC@FeBTC/NIF in the photoelectronically coupled catalytic oxygen evolution reaction (OER) reaction is presented. The efficient transfer of carriers between components enhances the catalytic activity. Besides, the construction of heterojunctions optimizes the energy level structure and increases the absorption of light, and the microstructure forms holes with a blackbody effect that also enhances light absorption. Consequently, CeBTC@FeBTC/NIF has excellent photoelectric coupling catalytic properties and requires an overpotential of only 300 mV to drive a current density of 100 mA cm-2 under illumination. More importantly, the n-n heterojunction was found to be effective in enhancing charge and photogenerated electron migration by examining the carrier density of each component and carrier diffusion at the interface.

10.
Sci Total Environ ; 912: 169419, 2024 Feb 20.
Artigo em Inglês | MEDLINE | ID: mdl-38128661

RESUMO

As an emerging contaminant, microplastics are absorbed by crops, causing diverse impacts on plants. Plants may have different physiological responses to different uptake modes of microplastics various stage of growth. In this study, the distribution of polystyrene (PS) microspheres in the roots of oilseed rape and the physiological responses at different growth stages were investigated by confocal laser scanning microscope, scanning electron microscopy, and biochemical analysis. This study, conducted via scanning electron microscopy, discovered that agglomerates of microspheres, rather than individual plastic pellets, were taken up by plant roots in solution for the first time. The agglomerates subsequently migrate into the vascular bundles of the root system. Moreover, this study provided the proof for the first time that PS is transported in plants via the symplast system. On the physiological and biochemical function, the exposure of PS at the flowering and bolting stages caused oxidative stress on oilseed rape. That is, the addition of PS with different particle sizes significantly increased peroxidase (POD), malondialdehyde (MDA), photosynthetic rate, chlorophyll content and inhibited superoxide dismutase (SOD) content in oilseed rape at different developmental stages. These changes regulated the chloroplast structure and chlorophyll synthesis, maintained a high photosynthetic rate, and mitigated the toxicity of PS. In addition, correlation analysis showed that MDA and citric acid contents were significantly positively correlated with chlorophyll contents (p < 0.05), which suggested that the 80 nm PS treatment stimulated organic acid secretion in oilseed rape at the bolting stage to maintain a higher chlorophyll content. This study expands the current understanding of the effects of microplastics on crop growth, and the results holding significant implications for exploring the impact of microplastics on vegetables during various developmental stages and for future risk assessment.


Assuntos
Brassica napus , Microplásticos , Microplásticos/metabolismo , Plásticos/toxicidade , Plásticos/metabolismo , Brassica napus/metabolismo , Peroxidases/metabolismo , Clorofila/metabolismo , Poliestirenos/toxicidade , Poliestirenos/metabolismo , Raízes de Plantas/metabolismo
11.
J Hazard Mater ; 464: 132963, 2024 02 15.
Artigo em Inglês | MEDLINE | ID: mdl-37976850

RESUMO

A comprehensive study was conducted to investigate how ultraviolet (UV) irradiation combined with electrochemistry (EC) can efficiently remove human body fluids (HBFs) related pollutants, such as urea/creatinine/hippuric acid, from swimming pool water (SPW). In comparison with the chlorination, UV, EC, and UV/chlorine treatments, the EC/UV treatment exhibited the highest removal rates for these typical pollutants (TPs) from HBFs in synthetic SPW. Specifically, increasing the operating current of the EC/UV process from 20 to 60 mA, as well as NaCl content from 0.5 to 3.0 g/L, improved urea and creatinine degradation while having no influence on hippuric acid. In contrast, EC/UV process was resilient to changes in water parameters (pH, HCO3-, and actual water matrix). Urea removal was primarily attributable to reactive chlorine species (RCS), whereas creatinine and hippuric acid removal were primarily related to hydroxyl radical, UV photolysis, and RCS. In addition, the EC/UV procedure can lessen the propensity for creatinine and hippuric acid to generate disinfection by-products. We can therefore draw the conclusion that the EC/UV process is a green and efficient in-situ technology for removing HBFs related TPs from SPW with the benefits of needless chlorine-based chemical additive, easy operation, continuous disinfection efficiency, and fewer byproducts production.


Assuntos
Líquidos Corporais , Piscinas , Poluentes Químicos da Água , Purificação da Água , Humanos , Cloro/química , Creatinina , Desinfecção/métodos , Raios Ultravioleta , Oxirredução , Halogenação , Líquidos Corporais/química , Água , Ureia , Poluentes Químicos da Água/química , Purificação da Água/métodos
12.
J Fluoresc ; 2023 Dec 05.
Artigo em Inglês | MEDLINE | ID: mdl-38051402

RESUMO

Cy5.5 and 7.5 are the most commonly used NIR 2-region fluoresceins, which have good luminescence properties and important biomedical tracer applications. In this paper, their molecular non-covalent interactions, UV-Vis absorption spectra, main bond lengths, electrostatic potential distributions, frontier molecular orbitals (HOMO and LUMO) and energy gaps were calculated by density functional theory (DFT). We found that the differences in the luminescence properties and energy gaps of Cy5.5 and Cy7.5 molecules may be caused by the length of the conjugated chains between the two aromatic rings in the molecule. By calculating the relevant molecular characteristics, this paper can provide ideas and theoretical basis for the relevant modification and application, as well as the development of new fluorescent dyes.

13.
Huan Jing Ke Xue ; 44(11): 6267-6278, 2023 Nov 08.
Artigo em Chinês | MEDLINE | ID: mdl-37973109

RESUMO

Microplastics(MPs), as a new type of environmental pollutants, have gradually attracted widespread attention since they were introduced by British scientists in 2004. Soil is an important accumulation site for microplastics, which can expand the scope of contamination and accumulate with agricultural practices such as irrigation and tillage. Microplastics in soil cause a variety of toxicities to terrestrial plants. The small particle size, difficult degradation, and strong adsorption capacity bring a challenge to the microplastic pollution treatment of soil. In this study, the toxicity of microplastics to terrestrial plants was reviewed in terms of their direct or indirect toxicity and combined effects with other pollutants, mainly in terms of mechanical injury, induction of oxidative stress, and cytotoxicity and genotoxicity to plants, resulting in plant growth and plant tissue metabolism obstruction. In general, the toxicity of microplastics depended on the polymer type, size, and dose; plant tolerance; and exposure conditions. In addition, the production of secondary microplastics and endogenous contaminants during their degradation in soil enhanced the biotoxicity of microplastics. Further, the physical, chemical, and microbial degradation mechanisms of microplastics were introduced in this study based on the current research. At first, the physical and chemical degradation of microplastics mainly occurred by changing the particle size and surface properties of microplastics and producing intermediates. Then, smaller-sized microplastics and their intermediates could eventually be converted to water and carbon dioxide through physical, chemical, and biological functions. Finally, further prospects regarding soil microplastics were introduced, and we provided information for future improvement and pollution control of microplastics.


Assuntos
Poluentes Ambientais , Poluentes do Solo , Microplásticos/toxicidade , Solo/química , Plásticos/toxicidade , Poluentes do Solo/toxicidade , Poluentes do Solo/análise , Agricultura , Plantas , Ecossistema
14.
J Agric Food Chem ; 2023 Nov 06.
Artigo em Inglês | MEDLINE | ID: mdl-37930889

RESUMO

The covalent interactions between proanthocyanidins (PAs) and pectin during thermal processing was investigated. An acid-butanol assay clearly showed that PAs were covalently bound to pectin. Computational studies indicated that a nucleophilic substitution reaction occurred between the carbocation generated by the PAs and carboxyl or hydroxyl groups on the pectin, leading to the formation of PAs-pectin adducts. Thermal processing and PAs significantly affected the physicochemical, functional, and biological properties of pectin. Thermal processing reduced the molecular weight and increased the gelling properties of pectin, whereas PAs increased both the molecular weight and the gelling properties. Finally, we found that the covalent attachment of PAs to pectin greatly enhanced its antioxidant, prebiotic, and α-glucosidase inhibitory activity. Overall, our results suggest that the thermal processing of fruits has the potential to induce a covalent interaction between PAs and pectin, which would impact the physicochemical characteristics and functional properties of pectin.

15.
Org Biomol Chem ; 21(41): 8364-8371, 2023 Oct 25.
Artigo em Inglês | MEDLINE | ID: mdl-37815482

RESUMO

A Ce(III)-catalyzed, visible-light induced aerobic oxidative dehydrogenative coupling reaction between glycine derivatives and electron-rich arenes is disclosed. The protocol proceeds efficiently under mild conditions, providing an efficient method for the rapid synthesis of α-arylglycine derivatives without the need for an external photosensitizer and additional oxidant. Moreover, this protocol could be performed on a 5 mmol scale, without obvious reduction of the efficiency.

16.
Chem Commun (Camb) ; 59(85): 12783-12786, 2023 Oct 24.
Artigo em Inglês | MEDLINE | ID: mdl-37815520

RESUMO

A visible-light-induced aerobic oxidative [2+3] cycloaddition reaction between glycine derivatives and thiiranes has been disclosed, which provides an efficient and atom-economical strategy for the rapid synthesis of thiazolidine-2-carboxylic acid derivatives and the post-modification of glycine-derived dipeptides under mild conditions with good yield and high diastereoselectivities. A preliminary mechanistic study favors a pathway involving a cooperative photoredox catalysis and iron catalysis.

17.
ACS Nano ; 17(20): 19914-19924, 2023 10 24.
Artigo em Inglês | MEDLINE | ID: mdl-37791763

RESUMO

Venous thromboembolism (VTE) is the most fatal complication in cancer patients. Unfortunately, the frequent misdiagnosis of VTE owing to the lack of accurate and efficient evaluation approaches may cause belated medical intervention and even sudden death. Herein, we present a rapid, easily operable, highly specific, and highly sensitive procoagulant extracellular vesicle barcode (PEVB) assay composed of TiO2 nanoflower (TiNFs) for visually evaluating VTE risk in cancer patients. TiNFs demonstrate rapid label-free EV capture capability by the synergetic effect of TiO2-phospholipids molecular interactions and topological interactions between TiNFs and EVs. From ordinary plasma samples, the PEVB assay can evaluate potential VTE risk by integrating TiNFs-based EV capture and in situ EV procoagulant ability test with machine-learning-assisted clinical data analysis. We demonstrate the feasibility of this PEVB assay in VTE risk evaluation by screening 167 cancer patients, as well as the high specificity (97.1%) and high sensitivity (96.8%), fully exceeding the nonspecific and posterior traditional VTE test. Together, we proposed a TiNFs platform allowing for highly accurate and timely diagnosis of VTE in cancer patients.


Assuntos
Vesículas Extracelulares , Neoplasias , Trombose , Tromboembolia Venosa , Humanos , Tromboembolia Venosa/complicações , Neoplasias/complicações
18.
Org Biomol Chem ; 21(43): 8744-8748, 2023 Nov 08.
Artigo em Inglês | MEDLINE | ID: mdl-37873567

RESUMO

A p-TsOH/halotrimethylsilane facilitated cycloketonization of γ-hydroxyl ynones is detailed. This methodology enables the one-step synthesis of polysubstituted 3(2H)-furanone products. It is remarkable that the reaction exhibits excellent regio- and chemoselectivity by the addition of very small quantities of p-toluenesulfonic acid and water.

19.
Adv Mater ; 35(46): e2307705, 2023 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-37742109

RESUMO

Enabling the living capability of secreting liquids dynamically triggered by external stimuli while maintaining the bulk frame is a significant challenge for mucosa-inspired hydrogels. A mucosa-inspired electro-responsive hydrogel is developed in this study using the synergy between electro-responsive silk fibroin supramolecular non-covalent networks and covalent polyacrylamide and polyvinyl alcohol polymer networks. The formed supramolecular-covalent hydrogel exhibits a partial gel-sol transition upon the application of an electric field, and the liquid layer on the hydrogel surface near the cathode is used to mimic the mucus-secreting capability to regulate lubrication. The electro-responsive lubricating process can operate under a safe voltage and exhibits good reversibility. It is also a universal strategy to construct an electro-responsive hydrogel by introducing an electro-responsive supramolecular network into the polymer network. This mucosa-inspired electro-responsive supramolecular-covalent hydrogel offers a promising method for designing soft actuators or robots that can regulate lubrication using an electric strategy.

20.
Nat Commun ; 14(1): 5779, 2023 Sep 18.
Artigo em Inglês | MEDLINE | ID: mdl-37723155

RESUMO

Dispersion of colloidal particles in water or oil is extensively desired for industrial and environmental applications. However, it often strongly depends on indispensable assistance of chemical surfactants or introduction of nanoprotrusions onto the particle surface. Here we demonstrate the omnidispersity of hydrophilic-hydrophobic heterostructure particles (HL-HBPs), synthesized by a surface heterogeneous nanostructuring strategy. Photo-induced force microscopy (PiFM) and adhesion force images both indicate the heterogeneous distribution of hydrophilic domains and hydrophobic domains on the particle surface. These alternating domains allow HL-HBPs to be dispersed in various solvents with different polarity and boiling point. The HL-HBPs can efficiently adsorb organic dyes from water and release them into organic solvents within several seconds. The surface heterogeneous nanostructuring strategy provides an unconventional approach to achieve omnidispersion of colloidal particles beyond surface modification, and the omnidispersible HL-HBPs demonstrate superior capability for dye recycle merely by solvent exchange. These omnidispersible HL-HBPs show great potentials in industrial process and environmental protection.

SELEÇÃO DE REFERÊNCIAS
DETALHE DA PESQUISA