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Light-driven dry reforming of methane is a promising and mild route to convert two greenhouse gas into valuable syngas. However, developing facile strategy to atomically-precise regulate the active sites and realize balanced and stable syngas production is still challenging. Herein, we developed a spatial confinement approach to precisely control over platinum species on TiO2 surfaces, from single atoms to nanoclusters. The configuration comprising single atoms and sub-nanoclusters engenders pronounced electronic metal-support interactions, with resultant interfacial states prompting surface charge rearrangement. The unique geometric and electronic properties of these atom-cluster assemblies facilitate effective activation of CH4 and CO2, accelerating intermediate coupling and minimizing side reactions. Our catalyst exhibits an outstanding syngas generation rate of 34.41 mol gPt-1 h-1 with superior durability, displaying high apparent quantum yield of 9.1% at 365 nm and turnover frequency of 1289 h-1. This work provides insightful understanding for exploring more multi-molecule systems at an atomic scale.
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Untethered and self-transformable miniature robots are capable of performing reconfigurable deformation and on-demand locomotion, which aid the traversal toward various lumens, and bring revolutionary changes for targeted delivery in gastrointestinal (GI) tract. However, the viscous non-Newtonian liquid environment and plicae gastricae obstacles severely hamper high-precision actuation and payload delivery. Here, we developed a low-friction soft robot by assembly of densely arranged cone structures and grafting of hydrophobic monolayers. The magnetic orientation encoded robot can move in multiple modes, with a substantially reduced drag, terrain adaptability, and improved motion velocity across the non-Newtonian liquids. Notably, the robot stiffness can be reversibly controlled with magnetically induced hardening, enabling on-site scratching and destruction of antibiotic-ineradicable polymeric matrix in biofilms with a low-frequency magnetic field. Furthermore, the magnetocaloric effect can be utilized to eradicate the bacteria by magnetocaloric effect under high-frequency alternating field. To verify the potential applications inside the body, the clinical imaging-guided actuation platforms were developed for vision-based control and delivery of the robots. The developed low-friction robots and clinical imaging-guided actuation platforms show their high potential to perform bacterial infection therapy in various lumens inside the body.
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Transdermal behavior is a critical aspect of studying delivery systems and evaluating the efficacy of cosmetics. However, existing methods face challenges such as lengthy experiments, high cost, and limited model accuracy. Therefore, developing accurate transdermal models is essential for formulation development and effectiveness assessment. In this study, we developed a multiscale model to describe the transdermal behavior of active ingredients in the stratum corneum. Molecular dynamics simulations were used to construct lipid bilayers and determine the diffusion coefficients of active ingredients in different regions of these bilayers. These diffusion coefficients were integrated into a multilayer lipid pathway model using finite element simulations. The simulation results were in close agreement with our experimental results for three active ingredients (mandelic acid (MAN), nicotinamide (NIC), and pyruvic acid (PYR)), demonstrating the effectiveness of our multiscale model. This research provides valuable insights for advancing transdermal delivery methods.
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Administração Cutânea , Bicamadas Lipídicas , Simulação de Dinâmica Molecular , Niacinamida , Ácido Pirúvico , Niacinamida/química , Niacinamida/administração & dosagem , Bicamadas Lipídicas/química , Ácido Pirúvico/química , Ácidos Mandélicos/química , Ácidos Mandélicos/administração & dosagem , Difusão , Pele/metabolismo , Pele/químicaRESUMO
The integration of oxidation and reduction half-reactions to amplify their synergy presents a considerable challenge in CO2 photoconversion. Addressing this challenge requires the construction of spatially adjacent redox sites while suppressing charge recombination at these sites. This study introduces an innovative approach that utilizes spatial synergy to enable synergistic redox reactions within atomic proximity and employs spin polarization to inhibit charge recombination. We incorporate Mn into Co3O4 as a catalyst, in which Mn sites tend to enrich holes as water activation sites, while adjacent Co sites preferentially capture electrons to activate CO2, forming a spatial synergy. The direct H transfer from H2O at Mn sites facilitates the formation of *COOH on adjacent Co sites with remarkably favorable thermodynamic energy. Notably, the incorporation of Mn induces spin polarization in the system, significantly suppressing the recombination of photogenerated charges at redox sites. This effect is further enhanced by applying an external magnetic field. By synergizing spatial synergy and spin polarization, Mn/Co3O4 exhibits a CH4 production rate of 23.4 µmol g-1 h-1 from CO2 photoreduction, showcasing a 28.8 times enhancement over Co3O4. This study first introduces spin polarization to address charge recombination issues at spatially adjacent redox sites, offering novel insights for synergistic redox photocatalytic systems.
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Passive radiative cooling (PRC) can spontaneously dissipate heat to outer space through atmospheric transparent windows, providing a promising path to meet sustainable development goals. However, achieving simultaneously high transparency, color-customizable, and thermal management of PRC anti ultraviolet (anti-UV) films remains a challenge. Herein, a simple strategy is proposed to utilize liquid crystalline polymer, with high mid-infrared emissive, forming customizable structural color film by molecular self-assembly and polymerization-induced pitch gradient, which guarantees the balance of transparency in visible spectrum and sunlight reflection, rendering anti-UV colored window for thermal management. By performing tests, temperature fall of 5.4 and 7.9 °C are demonstrated at noon with solar intensity of 717 W m-2 and night, respectively. Vivid red-, green-, blue-structured colors, and colorless films are designed and implemented to suppress the solar input and control the effective visible light transmissivity considering the efficiency function of human vision. In addition, temperature rise of 11.1 °C is achieved by applying an alternating current field on the PRC film. This study provides a new perspective on the thermal management and aesthetic functionalities of smart windows and wearables.
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Mimicking biological skin enabling direct, intelligent interaction between users and devices, multimodal sensing with optical/electrical (OE) output signals is urgently required. Owing to this, this work aims to logically design a stretchable OE biomimetic skin (OE skin), which can sensitively sense complex external stimuli of pressure, strain, temperature, and localization. The OE skin consists of elastic thin polymer-stabilized cholesteric liquid crystal films, an ion-conductive hydrogel layer, and an elastic protective membrane formed with thin polydimethylsiloxane. The as-designed OE skin exhibits customizable structural color on demand, good thermochromism, and excellent mechanochromism, with the ability to extend the full visible spectrum, a good linearity of over 0.99, fast response speed of 93 ms, and wide temperature range of 119 °C. In addition, the conduction resistance variation of ion-conductive hydrogel exhibits excellent sensing capabilities under pressure, stretch, and temperature, endowing a good linearity of 0.99998 (stretching from 0 to 150%) and high thermal sensitivity of 0.86% per °C. Such an outstanding OE skin provides design concepts for the development of multifunctional biomimetic skin used in human-machine interaction and can find wide applications in intelligent wearable devices and human-machine interactions.
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Liquid crystal emulsion is a new type of emulsion, in which the emulsifier molecules are located at the oil/water (O/W) interface and form a long-range ordered and short-range disordered lamellar liquid crystal. The lamellar liquid crystal formed by the emulsifier is similar to the skin stratum corneum lipid structure, which enables it to have a broad application prospect in the fields of cosmetics, pharmaceuticals, etc. In this work, a liquid crystal nanoemulsion was obtained by passing a liquid crystal emulsion stabilized by hydrogenated lecithin and phytosterol combination through a microfluidizer. The microstructure of the prepared liquid crystal nanoemulsion was investigated experimentally by dynamic light scattering, transmission electron microscopy, and small-angle X-ray scattering. The results have shown that the nanoemulsion inherited the liquid crystal emulsion property, namely, the long-range ordered and short-range disordered lamellar structure still existed at the oil/water interface even though they underwent extrusion, friction, and acceleration. At the same time, the underlying mechanisms of the existence of lamellar liquid crystal between the oil phase and the water phase for the nanoemulsion were explored theoretically by molecular dynamics simulations. The simulation results elucidated that the hydrogenated lecithin and phytosterol combination improved the flexibility of the bilayer structure composed of emulsifiers. The bilayers were the basic structure units of lamellar liquid crystals, and thus, the improved flexibility of bilayers provided insurance for the existence of lamellar liquid crystals with larger curvature around the oil droplets. In addition, the applicable properties of liquid crystal nanoemulsion were studied, and the results have shown that the liquid crystal nanoemulsion presented better slow-release and moisturizing properties than traditional nanoemulsions due to the existence of multilayers between oil and water phases. This work not only provides necessary information for the development and effective application of liquid crystal emulsions but also is helpful for in-depth understanding the inner properties of lamellar liquid crystal at molecular level.
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Liquid crystalline blue phase (BP) with 3D cubic nanostructure has attracted much interest in the fields of photonic crystals due to their unique optical properties and the ability to control the flow of light. However, there remains a challenge for simultaneously achieving self-assembly and mechanochromic response of soft 3D cubic nanostructures. Herein, a scalable strategy for the preparation of soft 3D cubic nanostructured films using oligomerization of the Michael addition reaction, which can induce the assembly of double-twisted cylinders for collective replication, remodeling, recombination, and growth, with a phase transition from BPII to BPI, and to chiral nematic phase, is presented. The prepared BP patterns can be obtained by Michael addition oligomerization reaction and composite mask photopolymerization, which present distinct mechanochromic sensitive due to patterns derived from different BP state, and the pattern can be reversibly erased and recurred by mechanical force and temperature. The average domain size of BPII prepared using this strategy can achieve 96 µm, which is 2.5 times larger than that obtained using the conventional cooling approach. This work provides new insights into the self-assembly and selective chemochromism of functional materials and devices.
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The oxidized 1-palmitoyl-2-arachidonoyl-sn-glycero-3-phosphocholine (ox-PAPC) products in human high-density lipoproteins (HDLs) were investigated by low-flow capillary electrophoresis-mass spectrometry (low-flow CE-MS). To accelerate the optimization, native PAPC (n-PAPC) standard was first analyzed by a commercial CE instrument with a photodiode array detector. The optimal separation buffer contained 60% (v/v) acetonitrile, 40% (v/v) methanol, 20 mM ammonium acetate, 0.5% (v/v) formic acid, and 0.1% (v/v) water. The selected separation voltage and capillary temperature were 20 kV and 23°C. The optimal CE separation buffer was then used for the low-flow CE-MS analysis. The selected MS conditions contained heated capillary temperature (250°C), capillary voltage (10 V), and injection time (1 s). No sheath gas was used for MS. The linear range for n-PAPC was 2.5-100.0 µg/mL. The coefficient of determination (R2 ) was 0.9918. The concentration limit of detection was 1.52 µg/mL, and the concentration limit of quantitation was 4.60 µg/mL. The optimal low-flow CE-MS method showed good repeatability and sensitivity. The ox-PAPC products in human HDLs were determined based on the in vitro ox-PAPC products of n-PAPC standard. Twenty-one ox-PAPC products have been analyzed in human HDLs. Uremic patients showed significantly higher levels of 15 ox-PAPC products than healthy subjects.
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Lipoproteínas HDL , Fosfolipídeos , Humanos , Células Cultivadas , Espectrometria de Massas , Eletroforese CapilarRESUMO
The application of alcohols as permeation enhancers in pharmaceutical and cosmetic formulations has attracted considerable attention, owing to their skin permeation-enhancing effect. Nonetheless, the elucidation of the fundamental mechanisms underlying the skin permeation-enhancing effect remains elusive. In this study, molecular dynamics (MD) simulations were employed to investigate the effect of 1,2-propanediol (1,2-PDO), 1,2-butanediol (1,2-BDO), and ethanol (EtOH) on the stratum corneum (SC) model membrane. The results showed that the effect of alcohols on the SC model membrane displayed a concentration-dependent nature. The alcohols can interact with SC lipids and exhibit a remarkable ability to selectively extract free fatty acid (FFA) molecules from the SC model membrane and make the SC looser. Meanwhile, 1,2-BDO and EtOH can penetrate into SC lipid bilayers at higher concentrations, leading to the formation of continuous hydrophilic defects in SC. The FFA extraction and the formation of continuous hydrophilic defects induced ceramide (CER) tail chains to become more disordered and fluid and also weakened the hydrogen bonding (H-bonding) network among SC lipids. Both the FFA extraction and the continuous hydrophilic defect formation endowed alcohols with the permeation-enhancing effect. The constrained simulations revealed that the free energy barriers decreased for the permeation of the hydrophilic model molecule (COL) across the SC model membranes containing alcohols, particularly for 1,2-BDO and EtOH. The possible permeation-enhancing mechanisms of alcohols were proposed correspondingly. This work not only provided a deep understanding of the transdermal permeation-enhancing behavior of alcohols at the molecular level but also provided necessary reference information for designing effective transdermal drug delivery systems in applications.
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Simulação de Dinâmica Molecular , Pele , Permeabilidade , Administração Cutânea , Etanol , Bicamadas LipídicasRESUMO
Background and Objectives: This study aimed to investigate the diagnostic value of immunological biomarkers in children with asthmatic bronchitis and asthma and to develop a machine learning (ML) model for rapid differential diagnosis of these two diseases. Materials and Methods: Immunological biomarkers in peripheral blood were detected using flow cytometry and immunoturbidimetry. The importance of characteristic variables was ranked and screened using random forest and extra trees algorithms. Models were constructed and tested using the Scikit-learn ML library. K-fold cross-validation and Brier scores were used to evaluate and screen models. Results: Children with asthmatic bronchitis and asthma exhibit distinct degrees of immune dysregulation characterized by divergent patterns of humoral and cellular immune responses. CD8+ T cells and B cells were more dominant in differentiating the two diseases among many immunological biomarkers. Random forest showed a comprehensive high performance compared with other models in learning and training the dataset of immunological biomarkers. Conclusions: This study developed a prediction model for early differential diagnosis of asthmatic bronchitis and asthma using immunological biomarkers. Evaluation of the immune status of patients may provide additional clinical information for those children transforming from asthmatic bronchitis to asthma under recurrent attacks.
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Asma , Bronquite , Humanos , Criança , Linfócitos T CD8-Positivos , Asma/diagnóstico , Bronquite/complicações , Bronquite/diagnóstico , Diagnóstico Diferencial , BiomarcadoresRESUMO
OBJECTIVE: The aim of this study is to assess soluble ST2 (sST2) as a potential biomarker in pediatric systemic lupus erythematous patients (pSLEs), especially to reveal the association of the sST2 levels with the disease activity and other laboratory tests. METHODS: A total of 65 pSLEs and 33 age- and sex- matched healthy controls (HCs) were enrolled in this study between July and December 2022 from Children's Hospital of Fudan University. Serum levels of sST2 were determined and clinical information and laboratory test results were collected. RESULTS: Serum sST2 levels were significantly increased in pSLEs (36.7 ng/mL, IQR 16.6-76.9) compared with HCs (10.4 ng/mL, IQR 6.4-14.8). Patients with moderate to severe disease activities had significantly elevated levels of sST2 compared with those with inactive and mild disease activities. A positive correlation was found between sST2 levels and SLE Disease Activity Index-2000 (SLEDAI-2K) scores. The serum levels of sST2 also showed positive correlations with anti-dsDNA antibody, ALT, AST, GGT, blood urea, and negative correlations with C3, C4, CH50 and ALP. ROC analysis showed that sST2 could discriminate active disease (AUC: 0.959, 95 %CI 0.878-0.992) with an optimal cut-off of 30.2 ng/mL (sensitivity: 89.7 %, specificity: 100 %) and moderate/severe disease activities (AUC: 0.962, 95 %CI 0.883-0.994) with an optimal cut-off of 45.2 ng/mL (sensitivity: 91.7 %, specificity: 90.2 %). Decreased sST2 levels were observed after clinical treatment. CONCLUSIONS: Elevated serum sST2 level in pSLEs were observed and were highly associated with disease activity, suggesting sST2 might be a potential biomarker for pSLEs.
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Proteína 1 Semelhante a Receptor de Interleucina-1 , Lúpus Eritematoso Sistêmico , Humanos , Criança , Lúpus Eritematoso Sistêmico/diagnóstico , Biomarcadores , Curva ROC , Índice de Gravidade de DoençaRESUMO
Highly persistent and toxic organic pollutants increasingly accumulate in freshwater resources, exacerbating the human water scarcity crisis. Developing novel microrobots with high catalytic performance, high mobility, and recycling capability integrated to harness energy from the surrounding environment to degrade pollutants effectively remains a challenge. Here, we report a kind of Spirulina (SP)-based magnetic photocatalytic microrobots with a substantially decreased band gap than that of pure photocatalysts, facilitating the generation of stable holes and electrons. Under sunlight irradiation, the degradation rate of rhodamine B (RhB) by the microrobots could be increased by 7.85 times compared with that of pure BiOCl, indicating its excellent photocatalytic performance. In addition, the microrobots can swarm in a highly controllable manner to the targeted regions and perform selective catalytic degradation of organic pollutants in specific areas by coupling effect of light and magnetic field. Importantly, the catalytic capability of the swarming microrobots can be activated by light stimulus whereas inhibited by magneto-optical stimuli, with a rate constant 2.15 times lower than that of pure light stimulation. The biohybrid and magneto-optical responsive microrobots offer a potential platform for selective pollutants catalysis at assigned regions in wastewater treatment plants.
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Background: sST2 has emerged as a potential disease biomarker of cardiac and inflammatory diseases in pediatrics. This study aimed to evaluate the performance of the new Pylon sST2 assay and establish the reference intervals of sST2 in children and adolescence in China. Methods: The experiments on precision, linearity, effects of interferents and sample stability were carried out to evaluate the analytical performances. A total of 240 healthy participants, aged from 2 to 17 years were enrolled. The nonparametric method was used to calculate the age- and sex-specified reference intervals. sST2 levels were measured in children with different diseases to evaluate the assay's diagnostic performance. Results: The repeatability and within-laboratory imprecision CVs of the assay were 6.0% and 7.6% at 19.5 ng/ml, and 3.1% and 5.9% at 289.8 ng/ml, respectively. The method showed linearity between 2.5 and 918.5 ng/ml. It was also noteworthy that the sST2 level was not affected in the presence of hemoglobin (2 mg/ml), triglyceride (30 mg/ml), bilirubin (0.3 mg/ml) and cholesterol (5 mg/ml). sST2 was found stable for 5 days at 4 °C in serum sample. The reference interval was determined as 2.1-21.0 ng/ml in general. No significant variation was observed by sex. However, sST2 increased constantly with age, especially in male. Increased sST2 was found in patients of systemic lupus erythematosus, sepsis, Crohn's diseases, respiratory failure and post cardiac surgery. Conclusions: The Pylon sST2 assay showed good analytical performances. The reference intervals were established in children and adolescence and sST2 showed potential clinical values in several diseases in pediatrics.
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Face masks with multiple functionalities and exceptional durability have attracted increasing interests during the COVID-19 pandemic. How to integrate the antibacterial property, comfortability during long-time wearing, and breath monitoring capability together on a face mask is still challenging. Here we developed a kind of face mask that assembles the particles-free water-repellent fabric, antibacterial fabric, and hidden breath monitoring device together, resulting in the highly breathable, water-repellent, and antibacterial face mask with breath monitoring capability. Based on the rational design of the functional layers, the mask shows exceptional repellency to micro-fogs generated during breathing while maintaining high air permeability and inhibiting the passage of bacteria-containing aerogel. More importantly, the multi-functional mask can also monitor the breath condition in a wireless and real-time fashion, and collect the breath information for epidemiological analysis. The resultant mask paves the way to develop multi-functional breath-monitoring masks that can aid the prevention of the secondary transmission of bacteria and viruses while preventing potential discomfort and face skin allergy during long-period wearing.
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Objective: To investigate the epidemiology and infectious characteristics of Epstein-Barr virus (EBV) infection among children in Shanghai, China from 2017 to 2022. Methods: We conducted a retrospective analysis of 10,260 inpatient patients who were subjected EBV nucleic acid testing from July 2017 to December 2022. Demographic information, clinical diagnosis, laboratory findings, etc. were collected and analyzed. EBV nucleic acid testing were performed by real-time PCR. Results: A total of 2192 (21.4%) inpatient children were EBV-positive, with the average age of 7.3 ± 0.1 y. EBV detection was stable from 2017 to 2020 (26.9~30.1%), but showed essential decreases in 2021 (16.0%) and 2022 (9.0%). EBV was highest (>30%) detected from three quarters (Q) including 2018-Q4, 2019-Q4 and 2020-Q3. There were 24.5% of EBV coinfection with other pathogens, including bacteria (16.8%), other viruses (7.1%) and fungi (0.7%). EBV viral loads increased when coinfecting with bacteria ((142.2 ± 40.1) ×104/mL) or other viruses ((165.7 ± 37.4) ×104/mL). CRP significantly increased in EBV/fungi coinfection, while procalcitonin (PCT) and IL-6 showed remarkable increases in EBV/bacteria coinfection. Most (58.9%) of EBV-associated diseases belonged to immune disorders. The primary EBV-related diseases were systemic lupus erythematosus (SLE, 16.1%), immunodeficiency (12.4%), infectious mononucleosis (IM, 10.7%), pneumonia (10.4%) and Henoch-schonlein purpura (HSP, 10.2%). EBV viral loads were highest ((233.7 ± 27.4) × 104/mL) in patients with IM. Conclusion: EBV was prevalent among children in China, the viral loads increased when coinfecting with bacteria or other viruses. SLE, immunodeficiency and IM were the primary EBV-related diseases.
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Coinfecção , Infecções por Vírus Epstein-Barr , Lúpus Eritematoso Sistêmico , Humanos , Criança , Infecções por Vírus Epstein-Barr/epidemiologia , Herpesvirus Humano 4/genética , Estudos Retrospectivos , Coinfecção/epidemiologia , Coinfecção/complicações , China/epidemiologia , Lúpus Eritematoso Sistêmico/complicaçõesRESUMO
Lignified stone cell content is a key factor used to evaluate fruit quality, influencing the economic value of pear (Pyrus pyrifolia) fruits. However, our understanding of the regulatory networks of stone cell formation is limited due to the complex secondary metabolic pathway. In this study, we used a combination of co-expression network analysis, gene expression profiles, and transcriptome analysis in different pear cultivars with varied stone cell content to identify a hub MYB gene, PbrMYB24. The relative expression of PbrMYB24 in fruit flesh was significantly correlated with the contents of stone cells, lignin, and cellulose. We then verified the function of PbrMYB24 in regulating lignin and cellulose formation via genetic transformation in homologous and heterologous systems. We constructed a high-efficiency verification system for lignin and cellulose biosynthesis genes in pear callus. PbrMYB24 transcriptionally activated multiple target genes involved in stone cell formation. On the one hand, PbrMYB24 activated the transcription of lignin and cellulose biosynthesis genes by binding to different cis-elements [AC-I (ACCTACC) element, AC-II (ACCAACC) element and MYB-binding sites (MBS)]. On the other hand, PbrMYB24 bound directly to the promoters of PbrMYB169 and NAC STONE CELL PROMOTING FACTOR (PbrNSC), activating the gene expression. Moreover, both PbrMYB169 and PbrNSC activated the promoter of PbrMYB24, enhancing gene expression. This study improves our understanding of lignin and cellulose synthesis regulation in pear fruits through identifying a regulator and establishing a regulatory network. This knowledge will be useful for reducing the stone cell content in pears via molecular breeding.
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Frutas , Pyrus , Frutas/genética , Frutas/metabolismo , Pyrus/genética , Pyrus/metabolismo , Lignina/metabolismo , Fatores de Transcrição/metabolismo , Regulação da Expressão Gênica de PlantasRESUMO
Nanoplastics (NPs) are mainly generated from the decomposition of plastic waste and industrial production, which have attracted much attention due to the potential risk for humans. The ability of NPs to penetrate different biological barriers has been proved, but the understanding of molecular details is very limited, especially for organic pollutant-NP combinations. Here, we investigated the uptake process of polystyrene NPs (PSNPs) combined with benzo(a)pyrene (BAP) molecules by dipalmitoylphosphatidylcholine (DPPC) bilayers by molecular dynamics (MD) simulations. The results showed that the PSNPs can adsorb and accumulate BAP molecules in water phase and then carried BAP molecules to enter DPPC bilayers. At the same time, the adsorbed BAP promoted the penetration of PSNPs into DPPC bilayers effectively by hydrophobic effect. The process of BAP-PSNP combinations penetrating into DPPC bilayers can be summarized into four steps including adhesion on the DPPC bilayer surface, uptake by the DPPC bilayer, BAP molecules detached from the PSNPs, and the PSNPs depolymerized in the bilayer interior. Furthermore, the amount of adsorbed BAP on PSNPs affected the properties of DPPC bilayers directly, especially the fluidity of DPPC bilayers that determine the physiologic function. Obviously, the combined effect of PSNPs and BAP enhanced the cytotoxicity. This work not only presented a vivid transmembrane process of BAP-PSNP combinations and revealed the nature of the effects of adsorbed benzo(a)pyrene on the dynamic behavior of polystyrene nanoplastics through phospholipid membrane, but also provide some necessary information of the potential damage for organic pollutant-nanoplastic combinations on human health at a molecular level.
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Poluentes Ambientais , Fosfolipídeos , Humanos , Benzo(a)pireno/química , Microplásticos , Poliestirenos , Simulação de Dinâmica Molecular , 1,2-Dipalmitoilfosfatidilcolina/químicaRESUMO
Nanoplastics are mainly generated from the decomposition of plastic waste and artificial production and have attracted much attention due to their wide distribution in the environment and the potential risk for humans. As the largest organ of the human body, the skin is inevitably in contact with nanoplastics. Stratum corneum is the first barrier when the skin is exposed to nanoplastics. However, little is known about the interactions between nanoplastics and stratum corneum. Here, the effects of particle size and surface functionalization (amino-modified and carboxy-modified) of polystyrene nanoplastics on the stratum corneum models were studied by Langmuir monolayer and molecular dynamics simulations. An equimolar mixture of ceramide/cholesterol/free fatty acid was used to mimic stratum corneum intercellular lipids. The Langmuir monolayer studies demonstrated that the larger size and surface functionalization of polystyrene nanoplastics significantly reduced the stability of stratum corneum lipid monolayer in a concentration-dependent fashion. Simulation results elucidated that functionalized polystyrene oligomers had a stronger interaction with lipid components of the stratum corneum model membrane. The cell experiments also indicated that functionalized polystyrene nanoplastics, especially for amino-modified polystyrene nanoplastics, had significant cytotoxicity on normal human dermal fibroblast cells. Our results provide fundamental information and the basis for a deeper understanding of the health risks of nanoplastics to humans.