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The ion permeability and selectivity of membranes are crucial in nanofluidic behavior, impacting industries ranging from traditional to advanced manufacturing. Herein, we demonstrate the engineering of ion-conductive membranes featuring angstrom-scale ion-transport channels by introducing ionic polyamidoamine (PAMAM) dendrimers for ion separation. The exterior quaternary ammonium-rich structure contributes to significant electrostatic charge exclusion due to enhanced local charge density; the interior protoplasmic channels of PAMAM dendrimer are assembled to provide additional degrees of free volume. This facilitates the monovalent ion transfer while maintaining continuity and efficient ion screening. The dendrimer-assembled hybrid membrane achieves high monovalent ion permeance of 2.81 mol m-2 h-1 (K+), reaching excellent mono/multivalent selectivity up to 20.1 (K+/Mg2+) and surpassing the permselectivities of state-of-the-art membranes. Both experimental results and simulating calculations suggest that the impressive ion selectivity arises from the significant disparity in transport energy barrier between mono/multivalent ions, induced by the "exterior-interior" synergistic effects of bifunctional membrane channels.
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Abdominal aortic aneurysm (AAA) is a prevalent condition characterized by the weakening and bulging of the abdominal aorta. This study aimed to investigate the impact of a stiff matrix on vascular smooth muscle cells (VSMCs) in AAA development. Bioinformatics analysis revealed that differentially expressed genes (DEGs) in VSMCs of an AAA mouse model were enriched in cellular senescence and related pathways. To simulate aging-related changes, VSMCs were cultured on stiff matrices, and compared to those on soft matrices, the VSMCs cultured on stiff matrices exhibited cellular senescence. Furthermore, the mutual distance between mitochondria and endoplasmic reticulum (ER) in VSMCs was increased, indicating altered mitochondria-endoplasmic reticulum contacts (MERCs). The observed upregulation of reactive oxygen species (ROS) levels, antioxidant gene expression, and decreased mitochondrial membrane potential suggested the presence of mitochondrial dysfunction in VSMCs cultured on a stiff matrix. Additionally, the induction of ER stress-related genes indicated ER dysfunction. These findings collectively indicated impaired functionality of both mitochondria and ER in VSMCs cultured on a stiff matrix. Moreover, our data revealed that high lipid levels exacerbated the effects of high matrix stiffness on VSMCs senescence, MERC sites, and mitochondria/ER dysfunction. Importantly, treatment with the antilipemic agent CI-981 effectively reversed these detrimental effects. These findings provide insights into the role of matrix stiffness, mitochondrial dysfunction, ER stress, and lipid metabolism in AAA development, suggesting potential therapeutic targets for intervention.
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Aneurisma da Aorta Abdominal , Músculo Liso Vascular , Camundongos , Animais , Músculo Liso Vascular/metabolismo , Mitocôndrias/metabolismo , Espécies Reativas de Oxigênio/metabolismo , Aneurisma da Aorta Abdominal/metabolismo , Aorta Abdominal/metabolismo , Miócitos de Músculo Liso/metabolismoRESUMO
The extensive utilization of Zinc Oxide nanoparticles (ZnO NPs) has garnered significant attention due to their detrimental impacts on ecosystem. Unfortunately, ecotoxicity of ZnO NPs in coastal waters with fluctuating salinity has been disregarded. This study mainly discussed the toxic effects of ZnO NPs on species inhabiting the transition zones between freshwater and brackish water, who are of great ecological and economic importance among fish. To serve as the model organism, Takifugu obscurus, a juvenile euryhaline fish, was exposed to different ZnO NPs concentrations (0-200 mg/L) and salinity levels (0 and 15 ppt). The results showed that a moderate increase in salinity (15 ppt) could alleviate the toxic effect of ZnO NPs, as evidenced by improved survival rates. The integrated biomarker response index on oxidative stress also revealed that the toxicity of ZnO NPs was higher in freshwater compared to brackish water. These outcomes can be attributed to higher salinity (15 ppt) reducing the bioavailability of ZnO NPs by facilitating their aggregation and inhibiting the release of metal ions. It is noteworthy that elevated salinity was found to alleviate ZnO NPs toxicity by means of osmotic adjustment via the activation of Na+/K+-ATPase activity. This study demonstrates the salinity-dependent effect of ZnO NPs on T. obscurus, suggesting the possibility for euryhaline fish like T. obscurus to adapt their habitat towards more saline environments, under constant exposure to ZnO NPs.
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Nanopartículas , Óxido de Zinco , Animais , Antioxidantes , Ecossistema , Peixes , Nanopartículas/toxicidade , Salinidade , Takifugu/fisiologia , Óxido de Zinco/toxicidadeRESUMO
Real-time quantitative PCR (qRT-PCR) is a pivotal technique for gene expression analysis. To ensure reliable and accurate results, the internal reference genes must exhibit stable expression across varied experimental conditions. Currently, no internal reference genes for Camellia impressinervis have been established. This study aimed to identify stable internal reference genes from eight candidates derived from different developmental stages of C. impressinervis flowers. We employed geNorm, NormFinder, and BestKeeper to evaluate the expression stability of these candidates, which was followed by a comprehensive stability analysis. The results indicated that CiTUB, a tubulin gene, exhibited the most stable expression among the eight reference gene candidates in the petals. Subsequently, CiTUB was utilized as an internal reference for the qRT-PCR analysis of six genes implicated in the petal pigment synthesis pathway of C. impressinervis. The qRT-PCR results were corroborated by transcriptome sequencing data, affirming the stability and suitability of CiTUB as a reference gene. This study marks the first identification of stable internal reference genes within the entire genome of C. impressinervis, establishing a foundation for future gene expression and functional studies. Identifying such stable reference genes is crucial for advancing molecular research on C. impressinervis.
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Camellia , Camellia/genética , Perfilação da Expressão Gênica/métodos , Transcriptoma , Reação em Cadeia da Polimerase em Tempo Real/métodos , Flores/genética , Padrões de ReferênciaRESUMO
Effective removal of phosphorus from water is crucial for controlling eutrophication. Meanwhile, the post-disposal of wetland plants is also an urgent problem that needs to be solved. In this study, seedpods of the common wetland plant lotus were used as a new raw material to prepare biochar, which were further modified by loading nano La(OH)3 particles (LBC-La). The adsorption performance of the modified biochar for phosphate was evaluated through batch adsorption and column adsorption experiments. Adsorption performance of lotus seedpod biochar was significantly improved by La(OH)3 modification, with adsorption equilibrium time shortened from 24 to 4 h and a theoretical maximum adsorption capacity increased from 19.43 to 52.23 mg/g. Moreover, LBC-La maintained a removal rate above 99% for phosphate solutions with concentrations below 20 mg/L. The LBC-La exhibited strong anti-interference ability in pH (3-9) and coexisting ion experiments, with the removal ratio remaining above 99%. The characterization analysis indicated that the main mechanism is the formation of monodentate or bidentate lanthanum phosphate complexes through inner sphere complexation. Electrostatic adsorption and ligand exchange are also the mechanisms of LBC-La adsorption of phosphate. In the dynamic adsorption experiment of simulated wastewater treatment plant effluent, the breakthrough point of the adsorption column was 1620 min, reaching exhaustion point at 6480 min, with a theoretical phosphorus saturation adsorption capacity of 6050 mg/kg. The process was well described by the Thomas and Yoon-Nelson models, which indicated that this is a surface adsorption process, without the internal participation of the adsorbent.
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Lotus , Poluentes Químicos da Água , Fósforo , Águas Residuárias , Fosfatos/química , Carvão Vegetal , Adsorção , Lantânio/química , Poluentes Químicos da Água/química , Sementes , CinéticaRESUMO
Oxidative stress and related oxidative damage have a causal relation with the pathogenesis of hypertension. Therefore, it is crucial to determine the mechanism of oxidative stress in hypertension by applying mechanical forces on cells to simulate hypertension while monitoring the release of reactive oxygen species (ROS) from cells under an oxidative stress environment. However, cellular level research has rarely been explored because monitoring the ROS released by cells is still challenging owing to the interference of O2. In this study, an Fe single-atom-site catalyst anchored on N-doped carbon-based materials (Fe SASC/N-C) was synthesized, which exhibits excellent electrocatalytic activity for the reduction of hydrogen peroxide (H2O2) at a peak potential of +0.1 V and can effectively avoid the interference of O2. Furthermore, we constructed a flexible and stretchable electrochemical sensor based on the Fe SASC/N-C catalyst to study the release of cellular H2O2 under simulated hypoxic and hypertension conditions. Density functional theory calculations show that the highest transition state energy barrier from the oxygen reduction reaction (ORR), i.e., O2 to H2O, is 0.38 eV. In comparison, the H2O2 reduction reaction (HPRR) can be completed only by overcoming a lower energy barrier of 0.24 eV, endowing the HPRR to be more favorable on Fe SASC/N-C compared with the ORR. This study provided a reliable electrochemical platform for real-time investigation of H2O2-related underlying mechanisms of the hypertension process.
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Peróxido de Hidrogênio , Hipertensão , Humanos , Espécies Reativas de Oxigênio , Estresse Oxidativo , Deutério , Hipóxia , OxigênioRESUMO
Though many elegant laccase mimics have emerged, these mimics generally have no substrate selectivity as well as low activity, making it difficult to fulfill the demand for monitoring in physiological conditions. Herein, inspired by the Cu-N ligand structure in the active site of natural laccase, we revealed that a carbon nanomaterial with atomically dispersed Cu and Zn atoms (CuZn-N/C) and a well-defined ligand structure could function as an effective laccase mimic for selectively catalyzing epinephrine (EP) oxidation. Catalytic activity of the CuZn-N/C nanozyme was superior to those of Cu-N/C and Zn-N/C and featured a Km value nearly 3-fold lower than that of natural laccase, which indicated that CuZn-N/C has a better affinity for EP. Density functional theory (DFT) revealed the mechanism of the superior catalytic ability of dual-metal CuZn-N/C as follows: (1) the exact distance of the two metal atoms in the CuZn-N/C catalyst makes it suitable for adsorption of the EP molecule, and the CuZn-N/C catalyst can offer the second hydrogen bond that stabilizes the adsorption; (2) molecular orbitals and density of states indicate that the strong interaction between the EP molecule and CuZn-N/C is important for EP catalytic oxidization. Furthermore, a sensitive and selective online optical detection platform (OODP) is constructed for determining EP with a low limit of detection (LOD) of 0.235 µM and a linear range of 0.2-20 µM. The system allows real-time measurement of EP release in the rat brain in vivo following ischemia with dexmedetomidine administration. This work not only provides an idea of designing efficient laccase mimics but also builds a promising chemical platform for better understanding EP-related drug action for ischemic cerebrovascular illnesses and opens up possibilities to explore brain function.
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Encéfalo , Lacase , Animais , Ratos , Ligantes , Especificidade por Substrato , EpinefrinaRESUMO
Direct electrocatalytic reduction of N2 to NH3 under mild conditions is attracting considerable interests but still remains enormous challenges in terms of respect of intrinsic catalytic activity and limited electrocatalytic efficiency. Herein, a photo-enhanced strategy is developed to improve the NRR activity on Cu single atoms catalysts. The atomically dispersed Cu single atoms supported TiO2 nanosheets (Cu SAs/TiO2 ) achieve a Faradaic Efficiency (12.88%) and NH3 yield rate (6.26 µg h-1 mgcat -1 ) at -0.05 V versus RHE under the light irradiation field, in which NH3 yield rate is fivefold higher than that under pure electrocatalytic nitrogen reduction reaction (NRR) process and is remarkably superior in comparison to most of the similar type electrocatalysts. The existence of external light field improves electron transfer ability between CuO and TiO, and thus optimizes the accumulation of surface charges on Cu sites, endowing more electrons involved in nitrogen fixation. This work reveals an atomic-scale mechanistic understanding of field effect-enhanced electrochemical performance of catalysts and it provides predictive guidelines for the rational design of photo-enhanced electrochemical N2 reduction catalysts.
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The study of cellular responses linked to oxidative stress mechanisms is crucial in comprehending diverse physiological and pathological life processes, including mitochondrial dysfunction. Nonetheless, despite the interference of O2, the monitoring of ROS released from cells poses a challenging task. In this study, carbon-based copper single-atom catalysts (Cu SACs) were synthesized that exhibits excellent electrocatalytic performance for H2O2 reduction with an initial potential at 0.23 V and effectively avoids interference from O2. Based on this catalyst, a flexible and stretchable oxygen-tolerant sensor was constructed and applied to monitor the calcium ion-induced ROS burst in human umbilical vein endothelial cells (HUVECs) in a simulated physiological condition. This study effectively eradicates interference that may arise from the reduction of O2 and presents a dependable platform for real-time in situ monitoring of physiologically active molecules by utilizing H2O2 detection.
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Peróxido de Hidrogênio , Oxigênio , Humanos , Peróxido de Hidrogênio/farmacologia , Espécies Reativas de Oxigênio , Cobre/química , Células Endoteliais da Veia Umbilical HumanaRESUMO
Exploring the response between benthic community changes and environmental variables has significance for restoring the health of river ecosystems. However, little is known of the impact on communities of interactions between multiple environmental factors, and frequent changes in the flow of mountain rivers are different from those in the flow of plain river networks, which also impact differently the benthic community. Thus, there is a need for research on the response of benthic communities to environmental changes in mountain rivers under flow regulation. In this study, we collected samples from the Jiangshan River in the dry season (November 2021) and the wet season (July 2022) to investigate the aquatic ecology and benthic macroinvertebrate communities in the watershed. Multi-dimension analyses were used to analyze the spatial variation in the community structure and response of benthic macroinvertebrates to multiple environmental factors. In addition, the explanatory power of the interaction between multiple factors on the spatial variation of communities, and the distribution characteristics of benthic community and their causes were investigated. The results showed that herbivores are the most abundant forms in the benthic community of mountain rivers. The structure of benthic community in Jiangshan River was significantly affected by water quality and substrate, whereas the overall community structure was affected by river flow conditions. Furthermore, nitrite nitrogen and ammonium nitrogen were the key environmental factors impacting the spatial heterogeneity of communities during the dry and wet season, respectively. Meanwhile, the interaction between these environmental factors showed a synergistic effect, enhancing the influence of these environmental factors on community structure. Thus, controlling urban and agricultural pollution and releasing ecological flow would be effective strategies to improve benthic biodiversity. Our study showed that using the interaction of environmental factors was a suitable way to evaluate the association between environmental variables and variation in benthic macroinvertebrate community structure in river ecosystems.
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Invertebrados , Rios , Animais , Invertebrados/fisiologia , Rios/química , Ecossistema , Monitoramento Ambiental , Qualidade da Água , BiodiversidadeRESUMO
The COVID-19 pandemic has resulted in a surge of fake news, creating public health risks. However, developing an effective way to detect such news is challenging, especially when published news involves mixing true and false information. Detecting COVID-19 fake news has become a critical task in the field of natural language processing (NLP). This paper explores the effectiveness of several machine learning algorithms and fine-tuning pre-trained transformer-based models, including Bidirectional Encoder Representations from Transformers (BERT) and COVID-Twitter-BERT (CT-BERT), for COVID-19 fake news detection. We evaluate the performance of different downstream neural network structures, such as CNN and BiGRU layers, added on top of BERT and CT-BERT with frozen or unfrozen parameters. Our experiments on a real-world COVID-19 fake news dataset demonstrate that incorporating BiGRU on top of the CT-BERT model achieves outstanding performance, with a state-of-the-art F1 score of 98%. These results have significant implications for mitigating the spread of COVID-19 misinformation and highlight the potential of advanced machine learning models for fake news detection.
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Conventional polymeric membranes are broadly employed in water treatment processes; however, most of them suffer from relatively low water permeance and severe membrane fouling phenomena owing to their relatively hydrophobic nature. In this work, a novel class of inorganic-organic composite membranes was developed through a newly developed vapor-ventilated in situ chemical deposition method, where the Ti and Si precursors were first hydrolyzed and then conferred into metal oxides to form a continuous TiO2-SiO2 modification layer. Owing to the distinct physicochemical properties, the Ti and Si precursors were leveraged as quasi-molecular regulators to tune the membrane surface chemistry and pore aperture (within the nanoscale) to benefit highly efficient water purification by underpinning the rapid transport of water molecules and featuring an excellent fouling-resistant and fouling-releasing property against typical pollutants. The as-developed TiO2-SiO2/PES composite membrane showed a high water permeance of 187.4 L·m-2·h-1·bar-1, together with a relatively small mean pore aperture of 4.2 nm, showing an outstanding permeating efficiency among state-of-the-art membranes with a similar separation accuracy. This study provides a paradigm shift in membrane materials that could open avenues for developing high-performance inorganic-organic composite membranes for complex wastewater treatment.
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Cell mechanotransduction plays an important role in vascular regulation and disease development. Excessive accumulation of ROS, especially superoxide anion radicals (O2Ë-), is closely related to cardiovascular diseases. Lately, NADPH oxidases, which are the major source of O2Ë- production in vascular tissues, have been demonstrated to be involved in cardiovascular diseases. Therefore, in situ and real-time monitoring of superoxide anions (O2Ë-) is essential for exploring the mechanisms of mechanotransduction associated with NADPH oxidase function in living cells. Here we report a rationally designed ultrasonication-assisted approach for growing Au nanoflower films on a flexible surface, which serves as the desired interface for cysteine and superoxide dismutase (SOD) anchoring to form a flexible and stretchable electrode (SOD/Cys/Au SE). The SOD/Cys/Au SE shows good stretchability, fast electron-transfer rates, and high selectivity to measure O2Ë- released from cells during the stretching states. Our strategy provides a basis for developing more sophisticated stretchable biosensing tools to induce and monitor transient biochemical signals during cell mechanotransduction.
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Técnicas Biossensoriais , Doenças Cardiovasculares , Humanos , Mecanotransdução Celular , Superóxido Dismutase/metabolismo , Superóxidos/metabolismoRESUMO
Remote control of cells and the regulation of cell events at the molecular level are of great interest to the biomedical field. In addition to mechanical forces and genes, chemical compounds and light play pivotal roles in regulating cell fate, which have boosted the fast growth of biology. Herein, we synthesized light-regulated, atomically dispersed Fe-N4immobilized on a carbon substrate nanozyme (Fe-N/C single atom catalysts), whose peroxidase- and catalase-like properties can be enhanced by 120% and 135%, respectively, under 808-nm laser irradiation through the photothermal effect of Fe-N/C. Interestingly, a switch to love/switch to kill interaction between Fe-N/C dose and near-infrared (NIR) light co-regulating the Fe-N/C nanozyme to modulate cell fate was discovered. Based on this, we found that under NIR light irradiation, when the dose of Fe-N/C is low, it can scavenge more reactive oxygen species (ROS) and achieve cell protection; when the dose of Fe-N/C is too high, it tended to lead to cell apoptosis. This work not only provides an effective strategy for the regulation of nanozyme activity but also realizes the dual-functional application of nanozyme materials for the treatment of some specific diseases.
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Ferro , Carbono/química , Catalase , Ferro/química , Ferro/farmacologia , Espécies Reativas de OxigênioRESUMO
Water and ion transport in nanochannels is an intriguing topic that has been extensively investigated in several energy- and environment-related research fields. Recently developed two-dimensional (2D) materials are ideal building blocks for constructing confined nanochannels by self-stacking. Among these, graphene oxide (GO) is the most frequently employed as the starting material because of its excellent solution processability. Since solvation of the GO nanostructure usually impairs the function of nanochannels, in this study, chemically converted graphene was prepared using a one-step method, to simultaneously acquire the desired stability and functionality of the nanochannels. The confined channels with high charge densities are capable of excluding â¼90% NaCl solutes from water in a pressure-driven filtration process. This surpasses the performance of most GO desalination membranes reported in the literature. Thus, this study provides useful information for the feasible development of ion-exclusion nanochannel membranes based on the proposed nanochannel-confined charge repulsion mechanism.
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Grafite , Nanoestruturas , Membranas Artificiais , Soluções , ÁguaRESUMO
A highly permselective nanofiltration membrane was engineered via zwitterionic copolymer assembly regulated interfacial polymerization (IP). The copolymer was molecularly synthesized using single-step free-radical polymerization between 2-methacryloyloxyethyl phosphorylcholine (MPC) and 2-aminoethyl methacrylate hydrochloride (AEMA) (P[MPC-co-AEMA]). The dynamic network of P[MPC-co-AEMA] served as a regulator to precisely control the kinetics of the reaction by decelerating the transport of piperazine toward the water/hexane interface, forming a polyamide (PA) membrane with ultralow thickness of 70 nm, compared to that of the pristine PA (230 nm). Concomitantly, manipulating the phosphate moieties of P[MPC-co-AEMA] integrated into the PA matrix enabled the formation of ridge-shaped nanofilms with loose internal architecture exhibiting enhanced inner-pore interconnectivity. The resultant P[MPC-co-AEMA]-incorporated PA membrane exhibited a high water permeance of 15.7 L·m-2·h-1·bar-1 (more than 3-fold higher than that of the pristine PA [4.4 L·m-2·h-1·bar-1]), high divalent salt rejection of 98.3%, and competitive mono-/divalent ion selectivity of 52.9 among the state-of-the-art desalination membranes.
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Membranas Artificiais , Polímeros , Nylons , Polimerização , ÁguaRESUMO
Diabetes is a metabolic syndrome associated with hyperglycemia, hypertension, atherosclerosis, and endothelial dysfunction. Applying the mechanical stretch on cells to simulate blood circulation while monitoring the cell glucose metabolism in a high-glucose environment is important for better comprehension of the underlying mechanisms of atherosclerosis caused by diabetes. Herein, we developed a facile strategy integrating zeolitic imidazolate framework-8-encapsulated glucose oxidase (GOx@ZIF-8) and an gold (Au) stretchable electrode (Au SE) to construct a flexible and stretchable glucose sensor (GOx@ZIF-8/Au SE) for investigating the glucose metabolism mechanism of stretched endothelial cells in hyperglycemia. The encapsulation of GOx with ZIF-8 prevents the aggregation and detachment of GOx from the sensing interface and endows the biosensor with high stability. Additionally, the Au SE with inherent stretchability can act as an integrated platform for mechanical stimulation as well as for transient signal sensing during the mechanotransduction process. Moreover, this flexible and stretchable glucose sensor is successfully used for monitoring the glucose metabolism of mechanically stimulated cells in hyperglycemia, and it was found for the first time that the glucose utilization ability of cells under static conditions is higher than that in the stretched state. This facile and straightforward method paves a promising route for designing a stable enzyme-based stretchable biosensor for detecting the underlying mechanisms of atherosclerosis caused by diabetes.
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Aterosclerose/diagnóstico , Técnicas Biossensoriais , Diabetes Mellitus/diagnóstico , Células Endoteliais/química , Glucose/análise , Hiperglicemia/metabolismo , Aterosclerose/metabolismo , Células Cultivadas , Diabetes Mellitus/metabolismo , Eletrodos , Células Endoteliais/metabolismo , Glucose/metabolismo , Glucose Oxidase/química , Glucose Oxidase/metabolismo , Ouro/química , Humanos , Zeolitas/químicaRESUMO
Artificial nanozymes have been designed to solve the problems of high cost and poor stability involving natural enzymes in analytical applications. Nevertheless, the catalytic efficiency of the nanozyme still needs to be improved so that it can meet the stability and sensitivity requirements of continuous biological detection. We presented an effective tailoring strategy to enhance the enzyme-like activities of Prussian-blue-analog-based nanozymes. Molybdenum-polysulfide-deposited nickel-iron bimetal Prussian-blue-analog-based hollow nanocages (Nanocages) with peroxidase-, catalase-, and laccase-mimicking activities were synthesized. The doping of molybdenum successfully tailored the size, morphology, composition, and complex structure of the Nanocage, and the peroxidase- and laccase-mimicking activities of the Nanocage nanozyme were enhanced by over 37 and 27 times, respectively, compared with pristine Prussian blue analogs. Moreover, in environments of harsh pH, high temperature, and high salt concentration, Nanocages exhibited much higher stability than natural enzymes. The peroxidase- and catalase-mimicking activities were applied to eliminate reactive oxygen species in cells, whereas the laccase-like activity of Nanocages was integrated with an online sensing platform for in vivo and continuous optical hydrogen sulfide monitoring in the brains of living rats. Our findings may provide possibilities for advancing the design strategy of highly active nanozymes as well as nanozyme-based in vivo detection methods and will offer unique opportunities for their involvement in bioanalytical chemistry.
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Corantes/química , Ferrocianetos/química , Sulfeto de Hidrogênio/análise , Molibdênio/química , Nanoestruturas/química , Animais , Encéfalo/metabolismo , Catalase/química , Catalase/metabolismo , Corantes/metabolismo , Ferrocianetos/metabolismo , Células HeLa , Humanos , Lacase/química , Lacase/metabolismo , Molibdênio/metabolismo , Tamanho da Partícula , Peroxidase/química , Peroxidase/metabolismo , Ratos , Espécies Reativas de Oxigênio/metabolismo , Propriedades de SuperfícieRESUMO
The continuous detection of hydrogen sulfide (H2S) is significant for revealing its role in the neuron protection and diagnosis of various diseases. In this study, a Prussian blue analog nanocubes (PBA NCs)-based oxidase-like mimic was synthesized and designed for continuous H2S monitoring in a visible light absorption-based online optical detection platform (OODP). A specific chemical reaction between H2S and the PBA NCs induce a decreasing oxidase-like activity of the PBA NCs, generating lower amounts of oxidized products of 3,3'5,5'-tetramethylbenzidine (TMB) and increasing the light intensity. By coupling the microdialysis techniques with OODP, excellent linearity in the range of 0.1-20 µM H2S with a limit of detection of 33 nM and outstanding stability, reproducibility, and specificity in the response to H2S were exhibited. By using this OODP, near real-time response and continuous H2S measurements in the brains of living rats were successfully achieved. This new idea of integrating enzyme-like mimics with specific chemical reactions to form an online optical detection platform for continuous monitoring of neurochemical in the brain may be highly meaningful for thoroughly understanding the function of the brain.
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Encéfalo , Ferrocianetos/química , Sulfeto de Hidrogênio/análise , Luz , Animais , Tamanho da Partícula , Ratos , Ratos Sprague-Dawley , Propriedades de SuperfícieRESUMO
The continuous detection of glucose is significant for revealing its role in neuron protection and for diagnosis of various diseases. In this study, for the first time, a nonenzymatic online optical detection platform (OODP) for glucose measurement in rat brain utilizing the tandem enzyme activity of V2O5 nanobelts is developed. V2O5 nanobelts were synthesized via a facile solvothermal strategy, and for the first time it is found that the V2O5 nanobelts possess dual enzyme-like activity, i.e., glucose oxidase (GOx)-like and peroxidase-like activity, and can act as a "tandem nanozyme". To investigate the mechanisms of the GOx-like property, we built an adsorption model, and the RPBE density functional calculations indicate that the glucose molecule can be adsorbed on the V2O5 plane. Based on the ability of V2O5 nanobelts to mimick tandem enzymes, a nonenzymatic online optical detection platform (OODP) for the continuous monitoring of glucose in rat brain was designed, which exhibits excellent stability, high selectivity, and a wide linear detection range from 0.2 to 5 mM and records cerebral glucose alterations in the calm/ischemia model. This facile but reliable nonenzymatic online optical glucose measurement compares favorably with natural enzyme-based online electrochemical glucose analytical systems, and its ready adoption by physiologists and pathologists will facilitate the understanding of brain function and the pathogenesis of diabetes.