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Ferrous ion (Fe2+) can indicate the redox situation of water and also plays an important role in maintaining the ecological balance of water bodies. However, due to the redox-active property of Fe2+, it is still a huge challenge to sensitively and accurately determine Fe2+ especially in interstitial water. Herein, we prepared a ferrozine gel rod for valence fixation during sampling and subsequent smartphone-based detection of Fe2+. The electrode potential of the redox pair can be varied through the formation of Fe2+-ligand complexes, and when Ecomplex was higher than [Formula: see text] , the oxidation of Fe2+ by O2 was hindered, thus achieving the valence fixation of Fe2+. Six ligands were screened, and it was found that ferrozine could effectively increase the redox potential after complexing with Fe2+, and also exhibits an obvious color change while fixing the valence of Fe2+. To facilitate Fe2+ detection, a cross-linked porous polymer gel rod prepared by acrylamide and sodium alginate was used to encapsulate the ferrozine molecules. The ferrozine gel rod enabled fixation the valence of Fe2+ longer than 30 days, and the resulted purple-red color was pictured and analyzed by a smartphone. Ultimately, the developed ferrozine gel rod sensing system was able to achieve sensitive and linear detection of Fe2+ in the range of 1-200 µM with the limit of detection as low as 0.33 µM, and it also exhibited excellent selectivity and anti-interference ability. The accuracy and reliability of the method was verified by the determination of Fe2+ in spiked water samples and certified standard reference water samples. Finally, the ferrozine gel rod sensing system was successfully applied to in-situ detection of Fe2+ in interstitial water, overlying water and upper water of lake and river. This facile system that enabled valence fixation and fast detection is promising for detection of Fe2+ in environmental waters.
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Transition metal-based nanoparticles (NPs) are emerging as potential alternatives to platinum for catalyzing the oxygen reduction reaction (ORR) in zinc-air batteries (ZAB). However, the simultaneous coexistence of single-atom moieties in the preparation of NPs is inevitable, and the structural complexity of catalysts poses a great challenge to identifying the true active site. Herein, by employing in situ and ex situ XAS analysis, we demonstrate the coexistence of single-atom moieties and iron phosphide NPs in the N, P co-doped porous carbon (in short, Fe-N4-Fe2P NPs/NPC), and identify that ORR predominantly proceeds via the atomic-dispersed Fe-N4 sites, while the presence of Fe2P NPs exerts an inhibitory effect by decreasing the site utilization and impeding mass transfer of reactants. The single-atom catalyst Fe-N4/NPC displays a half-wave potential of 0.873 V, surpassing both Fe-N4-Fe2P NPs/NPC (0.858 V) and commercial Pt/C (0.842 V) in alkaline condition. In addition, the ZAB based on Fe-N4/NPC achieves a peak power density of 140.3 mW cm-2, outperforming that of Pt/C-based ZAB (91.8 mW cm-2) and exhibits excellent long-term stability. This study provides insight into the identification of true active sites of supported ORR catalysts and offers an approach for developing highly efficient, nonprecious metal-based catalysts for high-energy-density metal-air batteries.
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The electrocatalytic nitrogen reduction reaction (NRR) is a crucial process in addressing energy shortages and environmental concerns by synthesizing the NH3. However, the difficulty of N2 activation and fewer NRR active sites limit the application of NRR. Therefore, the NRR performance can be improved by rapid electron transport paths to participate in multi-electron reactions and N2 activation. Doping with transition metal element is a viable strategy to provide electrons and electronic channels in the NRR. This study focuses on the synthesis of Fe2(MoO4)3 (FeMo) and x%La-doped FeMo (x = 3, 5, 7, and 10) using the hydrothermal method. La-doping creates electron transport channels Fe2+-O2--Fe3+ and oxygen vacancies, achieving an equal molar ratio of Fe2+/Fe3+. This strategy enables the super-exchange in Fe2+-O2--Fe3+, and then enhances electron transport speed for a rapid hydrogenation reaction. Therefore, the synergistic effect of Fe2+/Fe3+ cycling and oxygen vacancies improves the NRR performance. Notably, 5%La-FeMo demonstrates the superior NRR performance (NH3 yield rate: 29.6 µg h-1 mgcat-1, Faradaic efficiency: 5.8%) at -0.8 V (vs. RHE). This work analyzes the influence of the catalyst electronic environment on the NRR performance based on the effect on different valence states of ions on electron transport.
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The discharge of several pollutants, such as ammonia (NH4+-N), nitrate (NO3--N), and heavy metals, from aquaculture wastewater into the aquatic environment can cause severe pollution issues. In this work, microbial techniques were employed to enable concurrent elimination of NH4+-N and NO3--N by Fe3+/Fe2+ cycling. The greatest NH4+-N and NO3--N removal efficiencies of 96.1 % and 97.6 % were gained by Aquabacterium sp. XL4 at NH4+/NO3- ratio of 1:1, carbon to nitrogen ratio of 4.0, pH of 6.5, and Fe3+ dosage of 20.0 mg L-1. Inhibitor and nitrogen balance assays suggested that nitrogen removal process of strain XL4 was a coupled function of anaerobic ammonia oxidation, ferric reduction driven ammonia oxidation, and iron-based denitrification. Furthermore, under the compound influence of strain XL4 metabolic processes and microbial iron oxide adsorption, the removal efficiencies of Pb2+, Cd2+, and Cu2+ reached above 90 %. This work contributes to theoretical grounding for microbial removal of multiple pollutants.
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The efficiency of photoelectrochemical (PEC) water splitting is hindered by the slow kinetics of the oxygen evolution reaction (OER). This study developed a composite photoanode for water oxidation by incorporating ternary LDHs (ZnCoAl-LDH) onto Ti-Fe2O3 as a cocatalyst. The ZnCoAl-LDH/Ti-Fe2O3 photoanode achieved a photocurrent density of 3.51 mA/cm2 at 1.23 V vs. RHE, which is 9.8 times higher than that of bare Ti-Fe2O3. Through a series of characterizations, the synergistic effects among the three metals were revealed. Furthermore, the addition of Zn can induce the formation of more high-valent Co, increasing the conductivity of CoAl-LDH and significantly reducing the surface charge transfer resistance. These advantages significantly enhance the injection efficiency of ZnCoAl-LDH/Ti-Fe2O3 (82 %), thereby accelerating the OER kinetics of Ti-Fe2O3. Our work introduces new approaches for selecting photoelectrochemical cocatalysts and designing high-performance photoanodes for water splitting.
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Developing hydrogen sensors with parts per billion-level detection limits, high response, and high stability is crucial for ensuring safety across various industries (e.g., hydrogen fuel cells, chemical manufacturing, and aerospace). Despite extensive research on parts per billion-level detection, it still struggles to meet stringent requirements. Here, high performance and ppb-level H2 sensing have been developed with palladium-doped iron oxide nanotubes (Pd@Fe2O3 NTs), which have been prepared by FeCl3·6H2O, PdCl2, and PVP electrospinning and air calcination techniques. Various characterization techniques (FESEM, TEM, XRD, and so forth) were used to prove that the nanotube structure was successfully prepared, and the doping of Pd nanoparticles was realized. The experiments show that palladium doping can significantly improve the gas response of iron oxide nanotubes. Specifically, 0.59 wt % Pd@Fe2O3 NTs have high response (Ra/Rg = 41,000), high selectivity, and excellent repeatability for 200 ppm hydrogen at 300 °C. Notably, there was still a significant response at a low detection limit (LOD) of 50 ppb (Ra/Rg = 16.8). This excellent hydrogen sensing performance may be attributed to the high surface area of the nanotubes, the p-n heterojunction of PdO/Fe2O3, which allows more oxygen to be adsorbed on the surface, and the catalytic action of Pd nanoparticles, which promotes the reaction of hydrogen with surface-adsorbed oxygen.
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The utilization of a heterogeneous nanojunction design has shown significant enhancements in the gas sensing capabilities of traditional metal oxide gas sensors. In this study, a novel room temperature H2S gas sensor employing Fe2O3 functionalized Ti3C2 MXene as the sensing material has been developed. This sensor exhibits a broad detection range (0.01-500 ppm), low detection limit (10 ppb), and rapid response/recovery times (10 s/15 s), making it ideal for ppb-level H2S detection. The exceptional gas sensitivity of Fe2O3/Ti3C2 composite to H2S can be attributed to several key factors. First, the unique layered frame structure of Fe2O3/Ti3C2 significantly amplifies the surface area of the hybrid material, enhancing the absorption and diffusion capabilities of H2S molecules. Second, the abundance of functional groups (-O, -OH, and -F) on the surface of Ti3C2 MXene nanosheets provides additional active sites for H2S adsorption, The density functional theory calculation confirms that the adsorption energy of the Fe2O3/Ti3C2 composite for H2S (-2.93 eV) is significantly lower than that of pure Fe2O3 (-2.37 eV) and Ti3C2 (-0.2 eV). Lastly, the remarkable metal conductivity of Ti3C2 MXene ensures efficient electron transfer, thereby enhancing overall sensing performance.
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This study investigated the modification of polyethersulfone (PES) ultrafiltration membranes with TiO2 and Fe2O3-TiO2 nanoparticles to enhance their hydrophilicity and biofouling resistance against the marine microalgae Chlorella vulgaris. It is a common freshwater and marine microalga that readily forms biofilms on membrane surfaces, leading to significant flux decline and increased operational costs in ultrafiltration processes. The microalgae cells and their extracellular polymeric substances (EPS) adhere to the membrane surface, creating a dense fouling layer that impedes water permeation. The modified membranes were characterized using contact angle measurements, scanning electron microscopy, and pure water flux/resistance tests. Short-term ultrafiltration experiments evaluated the membranes' antifouling performance by measuring flux decline, flux recovery ratio, and relative flux reduction during C. vulgaris filtration. The TiO2 membrane showed improved hydrophilicity and antifouling over the pristine PES membrane, while the Fe2O3-TiO2 nanocomposite membrane exhibited the best performance. It reduced the water contact angle and showed only a 5% relative flux reduction compared to 60% for the pristine membrane. SEM images confirmed reduced microalgal deposition on the nanocomposite surface. Long-term tests with microalgal cells under dark and visible light conditions in saline water further assessed the membranes' biofouling resistance. The Fe2O3-TiO2 membrane maintained 59 L/m2 h water flux under visible light after immersion in the microalgal solution, outperforming the pristine (38 L/m2 h) and TiO2 (52 L/m2 h) membranes. This superior antifouling was attributed to photocatalytic generation of reactive oxygen species inhibiting microalgal adhesion. This study demonstrates a promising strategy for mitigating biofouling in membrane-based water treatment and desalination processes.
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Incrustação Biológica , Chlorella vulgaris , Compostos Férricos , Luz , Membranas Artificiais , Polímeros , Sulfonas , Titânio , Ultrafiltração , Incrustação Biológica/prevenção & controle , Titânio/química , Titânio/farmacologia , Polímeros/química , Sulfonas/química , Sulfonas/farmacologia , Ultrafiltração/métodos , Compostos Férricos/química , Compostos Férricos/farmacologia , Chlorella vulgaris/efeitos dos fármacos , Nanopartículas/químicaRESUMO
BACKGROUND: Harmful microorganisms like pathogens significantly impact human health. Meanwhile, industrial growth causes pollution and water contamination by releasing untreated hazardous waste. Effective treatment of these microorganisms and contaminants is essential, and nanocomposites may be a promising solution. The present attempt demonstrates the green synthesis of α-Fe2O3@TiO2 nanocomposites (FTNCs) for the effective treatment of pathogens and organic contaminants. METHODS: The α-Fe2O3@TiO2 nanocomposites (FTNCs) has been synthesized through a green approach utilizing curcumin extract. Curcumin (Turmeric) extract (TEx) was prepared by washing, drying, and crushing 5 g of turmeric, then boiling it in 100 mL distilled water at 70°C for 1 hour. Metal salts (Fe3+/Ti4+, 2:1) were added to 100 mL of TEx under continuous stirring at 70°C for 24 h. The solution was rinsed and dried at 80°C overnight and heated at 300°C for 3 h to remove impurities. RESULTS: Synthesized FTNCs have been tested for the potent antibacterial activity against both Gram-positive (Staphylococcus aureus, Bacillus subtilis, Enterococcus faecalis) and Gram-negative bacteria (Escherichia coli, Salmonella Abony, Pseudomonas sp.). Observations discovered noteworthy inhibition of both Gram-positive and Gramnegative bacteria by FTNCs. Furthermore, the FTNCs system shows the energy band gap of ~2.6 eV which may suppress electron recombination, thereby enhancing photocatalysis and examined against Evans blue (EB) and Congo red (CR) dyes under UV and visible light (125 W) irradiation. The remarkable photocatalytic degradation efficiency (DE) for CR reached ~67.4% in 60 min. CONCLUSION: A simple green approach has been demonstrated for the synthesis of the FTNCs using curcumin-mediated reduction. As prepared FTNCs have been evaluated for potent antibacterial activity against both Gram-positive (Staphylococcus aureus, Bacillus subtilis, Enterococcus faecalis) and Gram-negative bacteria (Escherichia coli, Salmonella Abony, Pseudomonas sp.). OBSERVATIONS: The results show that the highest ZID values have been obtained for 5 mg/mL concertation of FTNCs of ~14, 22,18, 21, and 20 and 29 mm for E. coli, S. abony, S. aureus, B. subtilis, E. faecalis, and Pseudomonas sp., respectively. Additionally, FTNCs demonstrate remarkable photocatalytic degradation efficiency against EB and CR dyes under UV (125 W) irradiation, achieving 56, 67% degradation within 60 minutes for EB and CR. The findings suggest that the FTNCs hold promise for long-term antimicrobial efficacy against various bacteria and offer the potential for addressing water and wastewater contaminants through photocatalysis.
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Background: Neuroblastoma (NB) is one of the most devastating malignancies in children, accounting for a high mortality rate due to limited treatment options. This study is aimed at elucidating the role of the ferroptosis-related EIF2S1 gene in NB pathogenesis and exploring its potential as a therapeutic target. Methods: We conducted comprehensive bioinformatics analyses utilizing the FerrDb database and NB-related transcriptomics data to investigate the role of EIF2S1 in NB. Changes in EIF2S1 expression were subsequently validated in NB tissues and cell lines. Loss-of-function experiments were performed in SK-N-SH and IMR-32 cell lines through shRNA-mediated EIF2S1 knockdown. The impact of EIF2S1 knockdown on the tumorigenesis of SK-N-SH cells was assessed in nude mice. Results: Bioinformatics analyses revealed a significant association between elevated EIF2S1 expression and poor prognosis in NB patients. The increased levels of EIF2S1 expression were confirmed in NB tissues and cancerous cell lines. Furthermore, EIF2S1 overexpression was linked to translational regulation and immune cell infiltration modulation. Silencing of EIF2S1 resulted in the suppression of cell proliferation, migration, and tumorigenicity in NB cells. Additionally, EIF2S1 knockdown led to an accumulation of iron and oxidative stress, as well as a reduction in GPX4 and SLC7A11 expression. Conclusion: Our findings indicate that EIF2S1 appears to facilitate the progression of NB by protecting tumor cells from ferroptosis through modulating GPX4 and SLC7A11 expression. Consequently, EIF2S1 may serve as a potential therapeutic target for the management of NB.
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Developing efficient and environmentally benign heterogeneous catalysts that activate peroxymonosulfate (PMS) for the degradation of persistent organic contaminants remains a challenge. Metal-organic frameworks (MOFs)-derived metal oxide catalysts in advanced oxidation processes (AOPs) have received considerable attention research fraternity. Herein, we report an innovative magnetic trimetallic MOF-derived Fe-Mn-Sn oxide heterostructure (FeMnO@Sn) with adjustable morphology, size and Sn content, prepared through an impregnation-calcination strategy. The formation of a novel magnetic Fe2O3/Fe3O4/Mn3O4 heterostructure induces the generation of abundant Fe2+ and Mn2+ sites on the FeMnO@Sn surface. Meanwhile, the introduction of SnO2 into the Fe2O3/Fe3O4/Mn3O4 heterostructure facilitates the cleavage of the OO bond in adsorbed PMS. The synergy among the different functionalities of each metal oxide plays a vital role in the swift and effective degradation of pollutants. In addition, the uniquely designed catalyst exhibits magnetic properties that facilitate easy recycling and repeated use, thereby meeting environmental protection requirements. Overall, this research highlights the design of heterogeneous catalysts for the effective activation of PMS and provides valuable insights for the advancement of future environmental catalysts.
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The synthesis and characterization of iron oxide nanostructures, specifically snowflake architecture, are investigated for their potential applications in electrochemical sensing systems. A Raman spectroscopy analysis reveals phase diversity in the synthesized powders. The pH of the synthesis affects the formation of the hematite (α-Fe2O3) and goethite (α-FeOOH). Scanning electron microscopy (SEM) images confirm the distinct morphologies of the particles, which are selectively obtained through recrystallization during the elongated reaction time. An electrochemical analysis demonstrates the differing behaviors of the particles, with synthesis pH affecting the electrochemical activity and surface area differently for each shape. Cyclic voltammetry measurements reveal reversible dopamine detection processes, with snowflake iron oxide showing lower detection limits than a mixture of snowflakes and cube-like particles. This research contributes to understanding the relationship between iron oxide nanomaterials' structural, morphological, and electrochemical properties. It offers practical insights into their potential applications in sensor technology, particularly dopamine detection, with implications for biomedical and environmental monitoring.
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Fenpropathrin (FPT) is a synthetic pyrethroid insecticide, the persistence and accumulation in water of which could cause harmful effects on vulnerable groups like aquatic creatures, particularly posing significant risks to fish immune systems. This study aimed to investigate how environmentally relevant FPT concentrations (10-1000 µ/M) affect lipid peroxidation and Fe2+ metabolism in Cyprinus carpio head kidney lymphocytes, and its relationship with oxidative stress and immunotoxicity. Firstly, CCK-8 results demonstrated that FPT caused a significant increase in lymphocyte death. Secondly, lymphocytes exposed to FPT could lead ferroptosis in lymphocytes, accompanied by evidence of the Fe2+ transporter imbalance, lipid peroxidation, Fe2+ accumulation and ferroptosis related protein increment. Thirdly, we found that FPT esposure leads to a decrease in ATP, mitochondrial DNA and NADPH/NADP+ levels, and the mRNA associated with mitochondrial function-related genes (Fis1, Drp1, and OPA1) in lymphocytes. Additionally, FPT induced the increased the levels of inflammatory genes (TNF-α, IFN-γ, and IL-6) in head kidney lymphocytes. Importantly, exposure to FPT induced oxidative stress to produce intracellular ROS, disrupting the function of the CncC signaling pathway and expression disorder of xenobiotics detoxification (CYP 450 family) genes. Notably, Treatment with NAC (a ROS inhibitor, 5 µM) demonstrated that inhibiting ROS alleviated FPT-induced lymphocyte ferroptosis and inflammatory response via the ROS/CncC-xenobiotics signaling pathway. These findings not only introduces a novel approach to investigating the immunotoxicity of FPT but also offers critical insights into mitigating the adverse effects of FPT on aquatic animal health.
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Carpas , Peroxidação de Lipídeos , Linfócitos , Piretrinas , Espécies Reativas de Oxigênio , Transdução de Sinais , Animais , Carpas/metabolismo , Linfócitos/efeitos dos fármacos , Linfócitos/metabolismo , Piretrinas/toxicidade , Piretrinas/farmacologia , Transdução de Sinais/efeitos dos fármacos , Espécies Reativas de Oxigênio/metabolismo , Peroxidação de Lipídeos/efeitos dos fármacos , Inseticidas/toxicidade , Inseticidas/farmacologia , Ferro/metabolismo , Estresse Oxidativo/efeitos dos fármacos , Xenobióticos/toxicidade , Xenobióticos/metabolismo , Ferroptose/efeitos dos fármacosRESUMO
Excessive Fe2+ in coastal aquaculture source water will seriously affect the aquaculture development. This study used manganese sand to investigate the removal potential and mechanism of Fe2+ in coastal aquaculture source water by column experiments. The pseudo-first-order kinetic model could better describe Fe2+ removal process with R2 in the range of 0.9451-0.9911. More than 99.7% of Fe2+ could be removed within 120 min while the removal rate (k) was positively affected by low initial concentration of Fe2+, high temperature, and low pH. Logistic growth (S-shaped growth) model could better fit the concentration variation of Fe2+ in the effluent of the column (R2>0.99). The Fe2 breakthrough curve could be fitted by Bohart-Adams, Yoon-Nelson, and Thomas models (R2>0.95). Smooth slices with irregular shapes existed on the surface of manganese sand after the reaction while Fe content increased significantly on the surface of manganese sand after the column experiment. Moreover, FeO (OH) was mainly formed on the surface of manganese sand after the reaction. PRACTITIONER POINTS: Fe2+ in coastal aquaculture source water could be removed by manganese ores. The pseudo-first-order kinetic model better described the Fe2+ removal process. FeO (OH) was mainly formed on the surface of manganese sand after the reaction.
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Aquicultura , Ferro , Manganês , Poluentes Químicos da Água , Manganês/química , Ferro/química , Poluentes Químicos da Água/química , Cinética , Purificação da Água/métodos , Água do Mar/químicaRESUMO
Aqueous iron-ion batteries with reversible storage of Fe2+ have undergone rapid development in recent years. Consistently throughout these studies, metallic iron is selected as the anode material. However, the large overpotential (250 mV) associated with the plating/stripping process of iron in aqueous solutions leads to unsatisfactory energy efficiency of the battery, although high capacity and Coulomb efficiency can be achieved. Herein, an iron-free anode material, 9,10-anthraquinone (AQ) is proposed in aqueous iron-ion batteries, which shows a low reaction potential and minimal polarization during storing iron ions. The organic anode exhibits favorable specific capacity of 106 mAh g-1 at 0.5 A g-1 and excellent cycling stability (92.6% retention after 500 cycles). In addition, an aqueous full iron-ion battery is constructed using AQ as the anode and 9,10-phenanthraquinone (PQ) as the cathode. The full battery demonstrates an enhanced energy efficiency of 72%, which is 206% higher than that of metal iron anode, and shows excellent cycling stability and Coulombic efficiency. This work provides a viable route to overcome the high polarization of metallic iron anode and promote the development of aqueous iron-ion batteries.
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Increased intramitochondrial free iron is a key feature of various liver diseases, leading to oxidative stress, mitochondrial dysfunction, and liver damage. Polydatin is a polyphenol with a hepatoprotective effect, which has been attributed to its ability to enhance mitochondrial oxidative metabolism and antioxidant defenses, thereby inhibiting reactive oxygen species (ROS) dependent cellular damage processes and liver diseases. However, it has not been explored whether polydatin is able to exert its effects by protecting the phospholipid cardiolipin against damage from excess iron. Cardiolipin maintains the integrity and function of electron transport chain (ETC) complexes and keeps cytochrome c bound to mitochondria, avoiding uncontrolled apoptosis. Therefore, the effect of polydatin on oxidative lipid damage, ETC activity, cytochrome levels, and ROS production was explored in iron-exposed rat liver mitochondria. Fe2+ increased lipid peroxidation, decreased cardiolipin and cytochromes c + c1 and aa3 levels, inhibited ETC complex activities, and dramatically increased ROS production. Preincubation with polydatin prevented all these effects to a variable degree. These results suggest that the hepatoprotective mechanism of polydatin involves the attenuation of free radical production by iron, which enhances cardiolipin levels by counteracting membrane lipid peroxidation. This prevents the loss of cytochromes, improves ETC function, and decreases mitochondrial ROS production.
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Cardiolipinas , Glucosídeos , Peroxidação de Lipídeos , Mitocôndrias Hepáticas , Espécies Reativas de Oxigênio , Estilbenos , Animais , Cardiolipinas/metabolismo , Glucosídeos/farmacologia , Peroxidação de Lipídeos/efeitos dos fármacos , Espécies Reativas de Oxigênio/metabolismo , Ratos , Mitocôndrias Hepáticas/metabolismo , Mitocôndrias Hepáticas/efeitos dos fármacos , Estilbenos/farmacologia , Masculino , Transporte de Elétrons/efeitos dos fármacos , Sobrecarga de Ferro/metabolismo , Ferro/metabolismo , Estresse Oxidativo/efeitos dos fármacos , Antioxidantes/farmacologia , Antioxidantes/metabolismo , Citocromos c/metabolismo , Ratos Wistar , Complexo de Proteínas da Cadeia de Transporte de Elétrons/metabolismoRESUMO
Carbon nanotubes (CNTs) had room temperature response, large surface area, and excellent mechanical properties, making them favorable for the design of flexible, wearable, and portable gas sensors. However, CNTs were lacking in response and selective response to different gases, such as H2S. Here, we demonstrated a flexible H2S ppb-level gas sensor based on a carbon nanotube/amorphous Fe2O3 (CNT/Fe2O3) film at room temperature, which was fabricated via a simple one-step solvent-thermal method. The CNT/Fe2O3 film gas sensor exhibited a high selective response to H2S (with a response of 55.1% to 100 ppb H2S), rapid reversible response at room temperature (with a response time of â¼127 s to 100 ppb H2S), and low limit of detection to about 2 ppb. Additionally, the CNT/Fe2O3 film maintained good sensing performance under various bending conditions and could be further fabricated into the fiber gas sensor device via wet stretching, retaining response at the ppb level (with a response of 18.6% to 100 ppb H2S). This research on a flexible gas sensor device based on the CNT film/fiber opened up new possibilities for wearable portable electronic device applications.
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Compostos Férricos , Sulfeto de Hidrogênio , Nanotubos de Carbono , Temperatura , Nanotubos de Carbono/química , Compostos Férricos/química , Sulfeto de Hidrogênio/análise , Limite de Detecção , Dispositivos Eletrônicos VestíveisRESUMO
Detecting hydrogen sulfide (H2S) odor gas in the environment at parts-per-billion-level concentrations is crucial. However, a significant challenge is the rapid deactivation caused by SO42- deposition. To address this issue, we developed a sensing material comprising Fe2O3-decorated WO3 nanowires (FWO) with strong interfacial interaction. During the H2S sensing process, important oxygen vacancies (OVs) are generated in situ and are recyclable on the surface of the Fe2O3 cluster. This sensor achieves a response of 140 (Ra/Rg) toward 50 ppm of H2S at 250 °C, with an experimentally measured detection limit of 1 ppb. It also exhibits remarkable stability, with no significant change observed over a long period of 150 days. Based on a combination of in situ DRIFT and DFT calculations, we have identified that the overactivation of O2 is the key step in the formation of SO42-. This overactivation can be partially modulated by the synergistic effect of Fe2O3 decoration and the in situ generated OVs, regulating the oxidation product to SO2 rather than the toxic SO42-. Furthermore, the continuous generation of OVs compensates for the loss of active sites pertaining to SO42- deposition, thereby contributing to the excellent stability of the sensor. This study underscores the beneficial impact of in situ OV generation in FWO for H2S sensing, offering a dynamic strategy to enhance sensor performance, particularly in terms of stability.
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Compostos Férricos , Sulfeto de Hidrogênio , Nanofios , Óxidos , Oxigênio , Tungstênio , Tungstênio/química , Nanofios/química , Oxigênio/química , Óxidos/química , Sulfeto de Hidrogênio/análise , Sulfeto de Hidrogênio/química , Compostos Férricos/química , Limite de Detecção , Teoria da Densidade FuncionalRESUMO
2-ketoglutarate (2-KG)/Fe2+-dependent dioxygenases can catalyze the highly specific regio- and stereoselective functionalization of C(sp3)-H bond of complex compounds under mild reaction conditions. Hyoscyamine 6ß-hydroxylase (H6H), a member of these dioxygenases, catalyzes two consecutive oxidation reactions in the synthesis of scopolamine. The first reaction is the hydroxylation of hyoscyamine to 6ß-hydroxyhyoscyamine and the second is epoxidation of 6ß-hydroxyhyoscyamine. This paper introduces the catalytic mechanism, substrate scope, and application of H6H and evaluates the possibility of this enzyme as a biocatalyst for the functionalization of C(sp3)-H bond in complex compounds with different structural characteristics via hydroxylation or epoxidation, providing a theoretical basis for modification and application of this enzyme.
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Oxigenases de Função Mista , Oxigenases de Função Mista/metabolismo , Oxigenases de Função Mista/química , Escopolamina , Oxirredução , HidroxilaçãoRESUMO
This study aims to explore the n-FeO and p-α-Fe2O3 semiconductor nanoparticles in hydrogen (HER) and oxygen (OER) evolution reactions and a combined full cell electrocatalyst system to electrolyze the water. We have observed a distinct electrocatalytic performance for both HER and OER by tuning the interplay between iron oxidation states Fe2+ and Fe3+ and utilizing phase-transformed iron oxide nanoparticles (NPs). The Fe2+ rich n-FeO NPs exhibited superior HER performance compared to p-α-Fe2O3 and Fe(OH)x NPs, which is attributed to the enhancement in n-type semiconducting nature under HER potential, facilitating the electron transfer for the reduction in H+ ions. In contrast, p-α-Fe2O3 NPs demonstrated excellent OER activity. An H-cell constructed using n-FeO||p-α-Fe2O3 NPs as cathode and anode achieved a cell voltage of 1.87 V at a current density of 50 mA/cm2. The cell exhibited remarkable stability after 30 h of activation and maintained the high current density of 100 mA/cm2 for 80 h with a negligible increase in cell voltage. This work highlights the semiconducting properties of n-FeO and p-α-Fe2O3 for the electrochemical water splitting system using the band bending phenomenon under the applied potential.