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To mitigate the environmental impact of the improper disposal of spent LiFePO4 batteries and reduce resource waste, the development of LiFePO4 recycling technologies is of paramount importance. Meanwhile, olivine-structured NaFePO4 in sodium-ion batteries has received great attention, due to its high theoretical specific capacity of 154 mAh g-1 and excellent stability. However, olivine NaFePO4 only can be synthesized from olivine LiFePO4. Accordingly, in this proposal, developing the continuous flow electrochemical solid-liquid reactor-based metal ion insertion technology is to utilize the olivine FePO4, recycled from LiFePO4, and to synthesize NaFePO4. Additionally, by employing I- as the reducing agent, NaFePO4 is successfully synthesized with a discharge-specific capacity of 134 mAh g-1 at 0.1C and a remarkable capacity retention rate of 86.5% after 100 cycles at 0.2C. And the reasons for sodium deficiency in the synthesized NFP are elucidated through first-principles calculations. Furthermore, the kinetics of the solid-solution reaction 2 (Na2/3+ßPO4â Na1-αFePO4) mechanism improve with cycling and are sensitive to temperature. Utilizing a minimal amount of reducing agent in the electrochemical reactor, NaFePO4 synthesis is successfully achieved. This innovative approach offers a new, cost-effective, and environmentally friendly strategy for preparing NaFePO4 from recycling LiFePO4.
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Na-based layered transition metal oxides with an O3-type structure are considered promising cathodes for sodium-ion batteries. However, rapid capacity fading, and poor rate performance caused by serious structural changes and interfacial degradation hamper their use. In this study, a NaPO3 surface modified O3-type layered NaNi1/3 Fe1/3 Mn1/3 O2 cathode is synthesized, with improved high-voltage stability through protecting layer against acid attack, which is achieved by a solid-gas reaction between the cathode particles and gaseous P2 O5 . The NaPO3 nanolayer on the surface effectively stabilizes the crystal structure by inhibiting surface parasitic reactions and increasing the observed average voltage. Superior cyclic stability is exhibited by the surface-modified cathode (80.1% vs 63.6%) after 150 cycles at 1 C in the wide voltage range of 2.0 V-4.2 V (vs Na+ /Na). Moreover, benefiting from the inherent ionic conduction of NaPO3 , the surface-modified cathode presents excellent rate capability (103 mAh g-1 vs 60 mAh g-1 ) at 10 C. The outcome of this study demonstrates a practically relevant approach to develop high rate and durable sodium-ion battery technology.
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Despite incorporation of organic groups into silica-based aerogels to enhance their mechanical flexibility, the wide temperature reliability of the modified silicone aerogel is inevitably degraded. Therefore, facile synthesis of soft silicone aerogels with wide-temperature stability remains challenging. Herein, novel silicone aerogels containing a high content of Si are reported by using polydimethylvinylsiloxane (PDMVS), a hydrosilylation adduct with water-repellent groups, as a "flexible chain segment" embedded within the aerogel network. The poly(2-dimethoxymethylsilyl)ethylmethylvinylsiloxane (PDEMSEMVS) aerogel is fabricated through a cost-effective ambient temperature/pressure drying process. The optimized aerogel exhibits exceptional performance, such as ultra-low density (50 mg cm-3), wide-temperature mechanical flexibility, and super-hydrophobicity, in comparison to the previous polysiloxane aerogels. A significant reduction in the density of these aerogels is achieved while maintaining a high crosslinking density by synthesizing gel networks with well-defined macromolecules through hydrolytic polycondensation crosslinking of PDEMSEMVS. Notably, the pore/nanoparticle size of aerogels can be fine-tuned by optimizing the gel solvent type. The as-prepared silicone aerogels demonstrate selective absorption, efficient oil-water separation, and excellent thermal insulation properties, showing promising applications in oil/water separation and thermal protection.
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The poor machinability of halide perovskite crystals severely hampered their practical applications. Here a high-throughput growth method is reported for armored perovskite single-crystal fibers (SCFs). The mold-embedded melt growth (MEG) method provides each SCF with a capillary quartz shell, thus guaranteeing their integrality when cutting and polishing. Hundreds of perovskite SCFs, exemplified by CsPbBr3, CsPbCl3, and CsPbBr2.5I0.5, with customized dimensions (inner diameters of 150-1000 µm and length of several centimeters), are grown in one batch, with all the SCFs bearing homogeneity in shape, orientation, and optical/electronic properties. Versatile assembly protocols are proposed to directly integrate the SCFs into arrays. The assembled array detectors demonstrated low-level dark currents (< 1 nA) with negligible drift, low detection limit (< 44.84 nGy s-1), and high sensitivity (61147 µC Gy-1 cm-2). Moreover, the SCFs as isolated pixels are free of signal crosstalk while showing uniform X-ray photocurrents, which is in favor of high spatial resolution X-ray imaging. As both MEG and the assembly of SCFs involve none sophisticated processes limiting the scalable fabrication, the strategy is considered to meet the preconditions of high-throughput productions.
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Owing to their high sensitivity across a wide stress range, mechanical reliability, and rapid response time, flexible polymer foam piezoresistive sensors have been extensively used in various fields. The reliable application of these sensors under harsh environments, however, is severely limited by structural devastation and poor interfacial bonding between polymers and conductive nanoparticles. To address the above issues, robust MXene/CNT nanocoatings on the foam surface, where the chemical assembly of MXene nanosheets and the physical anchoring of CNTs lead to strong interfacial bonding, are designed and described, which endows foams with structural reliability and unexpected multi-functionalities without compromising their instinct properties. The optimized foam nanocomposites thus maintain outstanding wide-temperature flexibility (-60-210 °C) and elasticity (≈3% residual strain after 1000 cycles). Moreover, the nanocomposites display good sensitivity at a relatively wide stress range of 0-70% and remarkable stability under acidic and alkaline settings. Furthermore, the foams with exceptional fire resistance (UL-94 V-0 rating) can provide stable sensing behavior (over 300 cycles) even after being exposed to flames for 5 s, making them one of the most reliable sensing materials so far. Clearly, this work widens applications of flexible piezoresistive sensors based on silicone foam nanocomposites for various harsh environments.
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The development of innovative methods for synthesizing silylcyclopentene compounds is particularly important for enriching and improving the synthetical toolbox of organosilicon compounds. Herein, a facile approach has been developed for the synthesis of silylcyclopentenes promoted by mechanochemically generated organolithium species as silicon nucleophiles under ball milling conditions, avoiding the requirement of large amounts of bulk solvent. This operationally simple method demonstrates good functional group compatibility, which provides a great opportunity for further exploration of the synthetic applications of silylcyclopentenes. Density functional theory calculations indicated that the transient lithiosilole intermediates undergo a stepwise nucleophilic addition process, which governs this mechanic-force-promoted [4+1] cycloaddition reaction.
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The tumor suppressor p53 has been implicated in the pathogenesis of liver fibrosis. HERC5-mediated posttranslational ISG modification of the p53 protein is critical for controlling its activity. Here, we demonstrated that the expression of HERC5 and ISG15 is highly elevated, whereas p53 is downregulated, in fibrotic liver tissues of mice and transforming growth factor-ß1 (TGF-ß1)-induced LX2 cells. HERC5 siRNA clearly increased the protein expression of p53, but the mRNA expression of p53 was not obviously changed. The inhibition of lincRNA-ROR (ROR) downregulated HERC5 expression and elevated p53 expression in TGF-ß1-stimulated LX-2 cells. Furthermore, the expression of p53 was almost unchanged after TGF-ß1-stimulated LX-2 cells were co-transfected with a ROR-expressing plasmid and HERC5 siRNA. We further confirmed that miR-145 is a target gene of ROR. In addition, we also showed that ROR regulates the HERC5-mediated ISGylation of p53 through mir-145/ZEB2. Together, we propose that ROR/miR-145/ZEB2 might be involved in the course of liver fibrosis by regulating ISGylation of the p53 protein.
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MicroRNAs , RNA Longo não Codificante , Humanos , Fator de Crescimento Transformador beta1/metabolismo , RNA Longo não Codificante/genética , Cirrose Hepática/metabolismo , Fibrose , RNA Interferente Pequeno , MicroRNAs/genética , Peptídeos e Proteínas de Sinalização Intracelular , Homeobox 2 de Ligação a E-box com Dedos de ZincoRESUMO
Human and animal studies support that consuming a high level of linoleic acid (LA, 18:2ω-6), an essential fatty acid and key component of the human diet, increases the risk of colon cancer. However, results from human studies have been inconsistent, making it challenging to establish dietary recommendations for optimal LA intake. Given the importance of LA in the human diet, it is crucial to better understand the molecular mechanisms underlying its potential colon cancer-promoting effects. Using LC-MS/MS-based targeted lipidomics, we find that the cytochrome P450 (CYP) monooxygenase pathway is a major pathway for LA metabolism in vivo. Furthermore, CYP monooxygenase is required for the colon cancer-promoting effects of LA, since the LA-rich diet fails to exacerbate colon cancer in CYP monooxygenase-deficient mice. Finally, CYP monooxygenase mediates the pro-cancer effects of LA by converting LA to epoxy octadecenoic acids (EpOMEs), which have potent effects on promoting colon tumorigenesis via gut microbiota-dependent mechanisms. Overall, these results support that CYP monooxygenase-mediated conversion of LA to EpOMEs plays a crucial role in the health effects of LA, establishing a unique mechanistic link between dietary fatty acid intake and cancer risk. These results could help in developing more effective dietary guidelines for optimal LA intake and identifying subpopulations that may be especially vulnerable to LA's negative effects.
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Neoplasias do Colo , Ácido Linoleico , Humanos , Camundongos , Animais , Ácido Linoleico/farmacologia , Ácido Linoleico/metabolismo , Cromatografia Líquida , Espectrometria de Massas em Tandem , Eicosanoides , Sistema Enzimático do Citocromo P-450/metabolismo , Dieta , Neoplasias do Colo/etiologiaRESUMO
The GPS-Nanoconveyor (MA-NV@DOX-Cas13a) is a targeted nanoplatform designed for the imaging and gene/chemotherapy synergistic treatment of melanoma. It utilizes rolling circle amplification (RCA) products as a scaffold to construct a DNA "Nanoconveyor" (NV), which incorporates a multivalent aptamer (MA) as a "GPS", encapsulates doxorubicin (DOX) in the transporter, and equips it with CRISPR/Cas13a ribonucleoproteins (Cas13a RNP). Carrying MA enhances the ability to recognize the overexpressed receptor nucleolin on B16 cells, enabling targeted imaging and precise delivery of MA-NV@DOX-Cas13a through receptor-mediated endocytosis. The activation of signal transducer and activator of transcription 3 (STAT3) in cancer cells triggers cis-cleavage of CRISPR/Cas13a, initiating its trans-cleavage function. Additionally, deoxyribonuclease I (DNase I) degrades MA-NV, releasing DOX for intracellular imaging and as a chemotherapeutic agent. Experiments demonstrate the superior capabilities of this versatile nanoplatform for cellular imaging and co-treatment while highlighting the advantages of these nanodrug delivery systems in mitigating DOX side effects.
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Sistemas CRISPR-Cas , Doxorrubicina , Doxorrubicina/farmacologia , Doxorrubicina/química , Doxorrubicina/administração & dosagem , Animais , Camundongos , Humanos , Aptâmeros de Nucleotídeos/química , Técnicas de Amplificação de Ácido Nucleico/métodos , Linhagem Celular Tumoral , Antibióticos Antineoplásicos/farmacologia , Antibióticos Antineoplásicos/administração & dosagem , Antibióticos Antineoplásicos/químicaRESUMO
Herein we present a catalytic cross-coupling strategy between C-radicals and Si-radicals, enabling the efficient, gentle, and versatile synthesis of dibenzylic silanes from para-quinone methides and silanecarboxylic acids as the stable silyl radical precursors. The reaction is facilitated by an inexpensive organophotocatalyst and exhibits broad compatibility with various electron-donating and electron-withdrawing functional groups. Notably, mechanistic investigations suggest the involvement of dibenzylic and silyl radicals, underscoring a novel radical coupling mechanism that introduces a fresh perspective on C-Si bond formation.
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Although the synthesis of polycyclic (hetero)aromatics via the [4 + 2] benzannulation process has been thoroughly explored, the restricted availability of energy sources (including thermal, light, and electrical energy) mandates the utilization of substantial quantities of organic solvents, inevitably leading to environmental pollution, resource wastage, and low reaction efficiency. Herein, we report a new method for the synthesis of polycyclic (hetero)aromatics from diazonium salts and alkynes under ball-milling conditions. This mechanochemical approach requires only substoichiometric amounts of DMSO as a liquid-assisted grinding additive and furnishes the desired product in a short time.
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The consumption of disposable surgical masks (DSMs) considerably increased during the coronavirus pandemic in 2019. Herein, we explored the spread of antibiotic resistance genes (ARGs) and the potential risks of antibiotic resistant bacteria (ARB) on DSMs. At environmentally relevant concentrations, the conjugate transfer frequency (CTF) of ARGs increased by 1.34-2.37 folds by 20 µg/m3 of atmospheric water-soluble inorganic ions (WSIIs), and it increased by 2.62-2.86 folds by 80 ng/m3 of polycyclic aromatic hydrocarbons (PAHs). Total suspended particulates (TSP) further promoted the CTF in combination with WSIIs or PAHs. Under WSII and PAH exposure, gene expression levels related to oxidative stress, cell membrane, and the adenosine triphosphate (ATP) were upregulated. WSIIs predominantly induced cellular contact, while PAHs triggered ATP formation and membrane damage. Molecular dynamics simulations showed that WSIIs and PAHs reduced membrane lipid fluidity and increased membrane permeability through interactions with the phosphatidylcholine bilayer. DSM filtering performance decreased, and the CTF of ARGs increased with the wearing time. The gut simulator test showed that ARB disrupted the human gut microbial community and increased total ARG abundance but did not change the ARG abundance carried by ARB themselves. A mathematical model showed that long-term WSII and PAH exposure accelerated ARG dissemination in DSMs.
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Máscaras , Hidrocarbonetos Policíclicos Aromáticos , Humanos , Poluentes Atmosféricos , Resistência Microbiana a Medicamentos/genética , COVID-19 , SARS-CoV-2RESUMO
Fluorosilicone rubber is essential for sealing in extreme temperatures and non-polar environments due to its exceptional adaptability. However, achieving a high yield of fluorosilicone polymers with medium and high fluorine content remains a challenge. Herein, a facile gradient strategy is developed that involves modifying the method of cyclic monomer addition based on the rate of ring-opening polymerization (ROP), to improve yield and adjust fluorine content precisely. The polymerization process is designed and tailored based on the reaction rates of anionic ring-opening polymerization (AROP) and cationic ring-opening polymerization (CROP) via an efficient gradient strategy. The effects of the polymerization process on the viscosity and yield of vinyl fluorosilicone polymers and hydrofluorosilicone polymers are investigated and optimized. Notably, the as-prepared vinyl-terminated fluoromethylsilane with 60% fluorine content (FMS-Vi-60F) has a high yield (86.6%) and high viscosity (150 000 mPa·s) in a short reaction time, which is superior to previous methods. Clearly, the gradient ring-opening method developed in this work provides a facile and efficient synthesis for fabricating fluorosilicone polymers with a high yield and tunable fluorine content.
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OBJECTIVE: Physical exercise has the potential to mitigate addictive behaviors and relevant health issues. However, the nighttime exercise has not been studied regarding this research topic. This study aims to explore the association between nocturnal physical exercise and problematic smartphone use before sleep, as well as related health issues. METHODS: To explore the association between nighttime physical exercise and problematic smartphone use before sleep as well as related health issues, we conducted a cross-sectional survey among 1,334 college students. Their daily exercise behaviors (including timeframe, rationale, frequency, and duration), smartphone use before sleep, sleep quality, smartphone addiction, anxiety, and depression were measured by questionnaires. The associations were assessed using generalized linear models. RESULTS: Our findings indicate that nearly 70% of participants chose to perform exercise at nighttime. Among these individuals who exercised at nighttime, the frequency and duration of nighttime exercise were significantly associated with decreased probabilities of smartphone use before sleep. Additionally, the frequency and duration of nighttime exercise were associated with lower levels of smartphone addiction and anxiety disorders. CONCLUSION: Nighttime Exercise behaviors can effectively reduce sleep delays caused by problematic smartphone use before bedtime. These findings contribute to understanding the potential effects of nighttime exercise on problematic smartphone use and relevant health issues. Future research should employ more precise methodologies to examine these associations.
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Ansiedade , Smartphone , Humanos , Estudos Transversais , Ansiedade/epidemiologia , Transtornos de Ansiedade , SonoRESUMO
Verbena officinalis L. as a medical plant has been used to treat many diseases. However, the quality control underlying V. officinalis remains to be studied. HPLC fingerprint analysis and the qualitative and quantitative analysis of water extract from V. officinalis were carried out, and it was found that the quality varies according to habitat and batch. Verbenalin could be a crucial component in the quality evaluation of V. officinalis. This study contributes to better understanding of quality control for V. officinalis.
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Extratos Vegetais , Verbena , Cromatografia Líquida de Alta Pressão/métodos , Extratos Vegetais/química , Extratos Vegetais/análise , Verbena/química , Reprodutibilidade dos Testes , Espectrometria de Massas/métodos , Modelos Lineares , Limite de Detecção , Espectrometria de Massa com Cromatografia LíquidaRESUMO
CuO nanoparticles with good water solubility and uniform particle size were successfully prepared. Interestingly, the oxidase-like activity of CuO NPs was continuously enhanced by the addition of thiourea (TU), and the enzyme activity was further enhanced by the addition of aluminum ion (Al3+). By systematically exploring and optimizing the experimental conditions, including the key parameters such as temperature, reaction time, and pH, a fluorescence-colorimetric dual-mode sensing system based on CuO nanoparticles was constructed. The detection range of TU and Al3+ were 1-100 µM and 1-100 µM, respectively, and the selectivity and precision of detection were further improved. In addition, the catalytic mechanism of CuO NPs as oxidase-like catalysts and the specific process in the reaction were investigated. Finally, the nano-sensing system was successfully applied to the analysis of three real environmental samples, namely, tap water, lake water and river water, which provided an effective new strategy for the future development of nano-sensing technology for TU and Al3+.
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In this study, a new polyionic polymer inhibitor, TIL-NH2, was developed to address the instability of shale gas horizontal wells caused by water-based drilling fluids. The structural characteristics and inhibition effects of TIL-NH2 on mud shale were comprehensively analyzed using infrared spectroscopy, NMR spectroscopy, contact angle measurements, particle size distribution, zeta potential, X-ray diffraction, thermogravimetric analysis, and scanning electron microscopy. The results demonstrated that TIL-NH2 significantly enhances the thermal stability of shale, with a decomposition temperature exceeding 300 °C, indicating excellent high-temperature resistance. At a concentration of 0.9%, TIL-NH2 increased the median particle size of shale powder from 5.2871 µm to over 320 µm, effectively inhibiting hydration expansion and dispersion. The zeta potential measurements showed a reduction in the absolute value of illite's zeta potential from -38.2 mV to 22.1 mV at 0.6% concentration, highlighting a significant decrease in surface charge density. Infrared spectroscopy and X-ray diffraction confirmed the formation of a close adsorption layer between TIL-NH2 and the illite surface through electrostatic and hydrogen bonding, which reduced the weakly bound water content to 0.0951% and maintained layer spacing of 1.032 nm and 1.354 nm in dry and wet states, respectively. Thermogravimetric analysis indicated a marked reduction in heat loss, particularly in the strongly bound water content. Scanning electron microscopy revealed that shale powder treated with TIL-NH2 exhibited an irregular bulk shape with strong inter-particle bonding and low hydration degree. These findings suggest that TIL-NH2 effectively inhibits hydration swelling and dispersion of shale through the synergistic effects of cationic imidazole rings and primary amine groups, offering excellent temperature and salt resistance. This provides a technical foundation for the low-cost and efficient extraction of shale gas in horizontal wells.
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Cancer, a chronic disease characterized by uncontrolled cell development, kills millions of people globally. The WHO reported over 10 million cancer deaths in 2020. Anticancer medications destroy healthy and malignant cells. Cancer treatment induces neuropathy. Anticancer drugs cause harm to spinal cord, brain, and peripheral nerve somatosensory neurons, causing chemotherapy-induced neuropathic pain. The chemotherapy-induced mechanisms underlying neuropathic pain are not fully understood. However, neuroinflammation has been identified as one of the various pathways associated with the onset of chemotherapy-induced neuropathic pain. The neuroinflammatory processes may exhibit varying characteristics based on the specific type of anticancer treatment delivered. Neuroinflammatory characteristics have been observed in the spinal cord, where microglia and astrocytes have a significant impact on the development of chemotherapy-induced peripheral neuropathy. The patient's quality of life might be affected by sensory deprivation, loss of consciousness, paralysis, and severe disability. High cancer rates and ineffective treatments are associated with this disease. Recently, histone deacetylases have become a novel treatment target for chemotherapy-induced neuropathic pain. Chemotherapy-induced neuropathic pain may be treated with histone deacetylase inhibitors. Histone deacetylase inhibitors may be a promising therapeutic treatment for chemotherapy-induced neuropathic pain. Common chemotherapeutic drugs, mechanisms, therapeutic treatments for neuropathic pain, and histone deacetylase and its inhibitors in chemotherapy-induced neuropathic pain are covered in this paper. We propose that histone deacetylase inhibitors may treat several aspects of chemotherapy-induced neuropathic pain, and identifying these inhibitors as potentially unique treatments is crucial to the development of various chemotherapeutic combination treatments.
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Antineoplásicos , Inibidores de Histona Desacetilases , Neuralgia , Neuralgia/tratamento farmacológico , Neuralgia/induzido quimicamente , Humanos , Inibidores de Histona Desacetilases/farmacologia , Animais , Antineoplásicos/efeitos adversos , Neoplasias/tratamento farmacológico , Qualidade de VidaRESUMO
Plant-enriched environments, the most common terrestrial landscapes, are usually coded as "green space" in urban studies. To understand how these natural environments can benefit human health, many theories have been developed, such as the well-known Attention Restoration Theory. Nowadays, more theories are emerging with regard to various and complex health dimensions. In this context, we searched online databases (from 2000 to 2022) and conducted a narrative review aiming to introduce relevant theories concerning psychological (e.g. Perceptual Fluency Account and Conditioned Restoration Theory), physiological (e.g. volatile organic compounds and environmental microbiomes), and behavioural (e.g. physical activity and social contact) perspectives. We also slightly mentioned some limitations and directions to be considered when using these theories. These results may offer general readers insights into the value of nature exposure and also help relevant researchers with study design and result interpretation.
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Meio Ambiente , Exercício Físico , HumanosRESUMO
To examine the mediatory role of nature connectedness between tree visibility through windows and mental wellbeing, we conducted a questionnaire survey and examined the mediation effect using both cross-sectional and semi-longitudinal mediation models. We evaluated nature connectedness using the Inclusion of Nature in Self (INS) scale and the Connectedness to Nature Scale (CNS) and measured mental wellbeing using the WHO-5 wellbeing index. Our results showed that participants who could see at least three trees through their windows reported higher levels of both nature connectedness and mental wellbeing compared to those without such visibility. Nature connectedness significantly mediated the relationship between the visibility of trees through windows and mental wellbeing, albeit with a somewhat limited effect. More broadly, this study provides additional evidence in support of the "3" component of the 3-30-300 "rule" for equitable access to greenspace in cities.