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A new understanding of the microstructure of soot particles: The reduced graphene oxide-like skeleton and its visible-light driven formation of reactive oxygen species
2021
Zhu, Jiali | Shang, Jing | Zhu, Tong
The mechanisms of soot’s photochemistry are still unclear, especially, how the microstructure and composition of soot influence its photoactivity. In the current study, we started with the exploration of the microstructure of soot particles and gained new insights. The elemental-carbon fraction of soot (E-soot), considered the core component of soot and can reflect the intrinsic characteristics of soot, was extracted by organic solvents and characterized in terms of structure and chemical reactivity. The intrinsic structure of E-soot was found to be more analogous to reduced graphene oxide than to graphene, in terms of containing similar levels of defective sites such as oxygen-containing functional groups and environmentally persistent free radicals, as well as exhibiting similar optoelectronic performance. The generation of reactive oxygen species via an electron transfer pathway under visible light suggests that reduced graphene oxide-like E-soot can serve as a potential carbo-photocatalyst, which facilitates elucidating the mechanism of E-soot’s role during soot’s photochemical aging. Our study reveals the intrinsic structure of soot and its role in photo-triggered reactive oxygen species production, which is vital for atmospheric and health effects.
Mostrar más [+] Menos [-]Evaluation of graphenic and graphitic materials on the adsorption of Triton X-100 from aqueous solution
2021
Presently, graphenic nanomaterials are being studied as candidates for wastewater pollutant removal. In this study, two graphite oxides produced from natural graphite with different grain sizes (325 and 10 mesh), their respective reduced graphene oxides and one reduced graphene oxide with nitrogen functional groups were synthesized and tested to remove a surfactant model substrate, Triton X-100, from an aqueous solution. Kinetic experiments were carried out and adjusted to pseudo-first order equation, pseudo-second order equation, Elovich, Chain-Clayton and intra-particle diffusion models. Reduced graphene oxides displayed an instantaneous adsorption due to their accessible and hydrophobic surfaces, while graphite oxides hindered the TX100 adsorption rate due to their highly superficial oxygen content. Results from the adsorption isotherms showed that the Sips model perfectly described the TX100 adsorption behavior of these materials. Higher adsorption capacities were developed with reduced graphene oxides, being maximum for the material produced from the lower graphite grain size (qₑ = 3.55·10⁻⁶ mol/m²), which could be explained by a higher surface area (600 m²/g), a lower amount of superficial oxygen (O/C = 0.04) and a more defected structure (ID/IG = 0.85). Additionally, three commercial high surface area graphites in the range of 100–500 m²/g were evaluated for comparison purposes. In this case, better adsorption results were obtained with a more graphitic material, HSAG100 (qₑ = 1.72·10⁻⁶ mol/m²). However, the best experimental results of this study were obtained using synthesized graphenic materials.
Mostrar más [+] Menos [-]Water-soluble graphitic carbon nitride for clean environmental applications
2021
(Dhinasekaran),
The removal of halogenated dye and sensing of pharmaceutical products in the water bodies with quick purification time is of high need due to the scarcity of drinking water. The present work reported on the preparation of graphitic carbon nitride (g-C₃N₄) for quick time water contaminant adsorption, followed by synthesizing silver nanoparticles decorated graphitic carbon nitride for pharmaceutical product sensing using in-situ SERS technique. The prepared graphitic carbon nitride is used to study the adsorption behavior of water contaminants at room temperature, in the presence of methylene blue (MB) as an adsorbate model. The water-soluble graphitic carbon nitride, even at low concentration, possesses an excellent ability to adsorb halogenated organic dye. As a result, the dyes are found to adsorb within ∼5s even without any additional physical or chemical activation. From the UV–Vis absorption investigations, it has been perceived that in the presence of graphitic carbon nitride (g-C₃N₄) the dye adsorption efficacy is observed nearly 80% with the well fitted linearly of R² = 0.9731. Effective in-situ surface-enhanced Raman scattering (SERS) studies for Ag nanoparticles decorated graphitic carbon nitride has been carried out and the obtained result shows good sensing performance of the material towards acetaminophen drug. This method opens the possibility of the Nobel metal decorated graphitic carbon nitride for real-time sensing of SERS-based drug products along with the development of high-performance sensing of the target analyte in the future.
Mostrar más [+] Menos [-]Comparison of the chronic toxicities of graphene and graphene oxide toward adult zebrafish by using biochemical and phenomic approaches
2021
Audira, Gilbert | Lee, Jiann-Shing | Siregar, Petrus | Malhotra, Nemi | Rolden, Marri Jmelou M. | Huang, Jong-Chin | Chen, Kelvin H.-C. | Hsu, Hua-Shu | Hsu, Yuchun | Ger, Tzong-Rong | Hsiao, Chung-Der
Graphene (GR) and graphene oxide (GO) are widely being used as promising candidates for biomedical applications, as well as for bio-sensing, drug delivery, and anticancer therapy. However, their undesirable side effects make it necessary to assess further the toxicity and safety of using these materials. The main objective of the current study was to investigate the toxicities of GR and GO in predicted environmental relevant concentrations in adult zebrafish (Danio rerio), particularly on their behaviors, and conducted biochemical assays to elucidate the possible mechanism that underlies their toxicities. Zebrafish was chronically (∼14 days) exposed to two different doses of GR (0.1 and 0.5 ppm) or GO (0.1 and 1 ppm). At 14 ± 1 days, a battery of behavioral tests was conducted, followed by enzyme-linked immunosorbent assays (ELISA) test on the following day to inspect the alterations in antioxidant activity, oxidative stress, and neurotransmitters in the treated zebrafish brain. An alteration in predator avoidance behavior was observed in all treated groups, while GR-treated fish exhibited abnormal exploratory behavior. Furthermore, altered locomotor activity was displayed by most of the treated groups, except for the high concentration of the GR group. From the ELISA results, we discovered a high concentration of GR exposure significantly decreased several neurotransmitters and cortisol levels. Meanwhile, elevated reactive oxygen species (ROS) were displayed by the group treated with low and high doses of GR and GO, respectively. These significant changes would possibly affect zebrafish behaviors and might suggest the potential toxicity from GR and GO exposures. To sum up, the present study presented new evidence for the effects of GR and GO in zebrafish behavioral dysregulation. We hope these assessments can contribute to our understanding of graphene and graphene oxide biosafety.
Mostrar más [+] Menos [-]Elucidating the co-transport of bisphenol A with polyethylene terephthalate (PET) nanoplastics: A theoretical study of the adsorption mechanism
2021
Cortés-Arriagada, Diego
Polyethylene terephthalate (PET) is a possible key component of nanoplastics in water environments, which can migrate pollutants through co-transport. In this regard, the co-transport of endocrine disruptors (such as bisphenol A, BPA) by nanoplastics is of emergent concern because of its cytotoxicity/bioaccumulation effects in aquatic organisms. In this work, a computational study is performed to reveal the BPA adsorption mechanism onto PET nanoplastics (nanoPET). It is found that the outer surface of nanoPET has a nucleophilic nature, allowing to increase the mass transfer and intraparticle diffusion into the nanoplastic to form stable complexes by inner and outer surface adsorption. The maximum adsorption energy is similar (even higher) in magnitude with respect to nanostructured adsorbents such as graphene, carbon nanotubes, activated carbon, and inorganic surfaces, indicating the worrying adsorption properties of nanoPET. The adsorption mechanism is driven by the interplay of dispersion (38–49%) and electrostatics effects (43–50%); specifically, dispersion effects dominate the inner surface adsorption, while electrostatics energies dominate the outer surface adsorption. It is also determined that π–π stacking is not a reliable interaction mechanism for aromatics on nanoPET. The formed complexes are also highly soluble, and water molecules behave as non-competitive factors, establishing the high risk of nanoPET to adsorb and migrate pollutants in water ecosystems. Furthermore, the adsorption performance is decreased (but not inhibited) at high ionic strength in salt-containing waters. Finally, these results give relevant information for environmental risk assessment, such as quantitative data and interaction mechanisms for non-biodegradable nanoplastics that establish strong interactions with pollutants in water.
Mostrar más [+] Menos [-]A novel modified Fe–Mn binary oxide graphite felt (FMBO-GF) cathode in a neutral electro-Fenton system for ciprofloxacin degradation
2021
Huang, Anqi | Zhi, Dan | Zhou, Yaoyu
A graphite felt (GF) cathode was firstly modified by Fe–Mn binary oxide (FMBO), active carbon (AC), carbon black (CB), and polytetrafluoroethylene (PTFE), which exhibits satisfactory ciprofloxacin (CIP) removal efficiency at neutral pH value in electro-Fenton (EF) system. Morphological data showed that modified cathodes have larger surface area and volume pore as well as more active sites. And electrochemical properties have proved stronger current response after modification. In compassion to the unmodified GF, the FMBO/AC/CB modified GF (FMBO-GF) has wider pH range and higher CIP removal efficiency due to its unique nanoparticles structure. The CIP removal efficiency achieved 95.40% in 30 min, and the removal efficiency of total organic carbon (TOC) achieved 93.77% in 2 h when conditions were optimal (25 mg/L initial CIP concentration, 2 mA/cm² current density, FMBO/AC: CB: PTFE of 1:1:5, and 7 initial pH value) in this study. The results of great degradation and mineralization of CIP in this study indicate that the FMBO-GF cathode has huge potential on antibiotics removals in neutral environment.
Mostrar más [+] Menos [-]Multigenerational selection towards longevity changes the protective role of vitamin C against graphene oxide-induced oxidative stress in house crickets
2021
Flasz, Barbara | Dziewięcka, Marta | Kędziorski, Andrzej | Tarnawska, Monika | Augustyniak, Jan | Augustyniak, Maria
This research was designed to investigate changes that can arise in an invertebrate organism due to stress caused by a strong prooxidant, graphene oxide (GO), and a potent antioxidant, vitamin C. The study aimed to investigate if vitamin C may support convalescence after chronic GO intoxication. We investigated the toxicity of chronic dietary graphene oxide administration in house cricket (Acheta domesticus) types: wild and selected for longevity (with a better developed antioxidant system, conducive to long life). Vitamin C was applied immediately after cessation of graphene oxide intoxication to check if it can support the remedial effect. The condition of cells, DNA stability, catalase activity, and the reproduction potential, measured as the Vitellogenin (Vg) protein expression level, were investigated in control and GO treated groups, recovery groups (-GO), and recovery groups with Vit. C (-GO + Vit.C). In this study vitamin C had no evident remedial effect on the house crickets exposed to graphene oxide. Most probably, the mechanism of vitamin C action, in case of intoxication with nanoparticles, is much more complicated. In the context of the results obtained, it is worth considering whether Vit. C, applied after GO intoxication, causes further disturbance of homeostasis in terms of the cells' redox potential.
Mostrar más [+] Menos [-]Monitoring of glyphosate-DNA interaction and synergistic genotoxic effect of glyphosate and 2,4-dichlorophenoxyacetic acid using an electrochemical biosensor
2021
Congur, Gulsah
Glyphosate (GLY) is a broad-spectrum herbicide used worldwide to control broadleaf sedge, and grass weeds to control non-specific vegetation. Although it was evaluated as non-toxic agent in 20ᵗʰ century, its carcinogenic and genotoxic potential has being intensively investigated all over the world in the last decade. Moreover, the combination of GLY and 2,4-dichlorophenoxyacetic acid (2,4-D) has been widely applied. Although genotoxicity of GLY has been evaluated in vivo studies, there is no report in the literature for the monitoring of in vitro biointeraction of GLY and double stranded DNA, or how effect the combination of GLY and 2,4-D onto DNA. Herein, an electrochemical biosensor platform was developed for detection of the pesticide-DNA interaction by using disposable pencil graphite electrodes (PGEs). First, voltammetric detection of the interaction between GLY and DNA was investigated and the electrochemical characterization of the interaction was achieved. Taking a step further, the synergistic genotoxic effect of the mixture of GLY and 2,4-dichlorophenoxyacetic acid (2,4-D) or the mixture of their herbicide forms onto DNA could be monitored. This effect was concentration dependent, and the herbicide of GLY or the use of mixture of herbicides of GLY and 2,4-D had more genotoxic effect than analytical grade of the active molecules, GLY and 2,4-D. The single-use PGEs provided to fabricate robust, eco-friendly and time saver recognition platform for monitoring of herbicide-DNA interaction with the sensitive and reliable results. It is expected that this study will lead to be designed miniaturized lab-on-a chip platforms for on-line analysis of the pesticide-nucleic acid interactions.
Mostrar más [+] Menos [-]Nickel decorated manganese oxynitride over graphene nanosheets as highly efficient visible light driven photocatalysts for acetylsalicylic acid degradation
2021
Mohan, Harshavardhan | Yoo, Suhwan | Thimmarayan, Srivalli | Oh, Hyeon Seung | Kim, Gitae | Seralathan, Kamala-Kannan | Shin, Taeho
In this work, we prepared nanocomposites of nickel-decorated manganese oxynitride on graphene nanosheets and demonstrated them as photocatalysts for degradation of acetylsalicylic acid (ASA). The catalyst exhibited a high degradation efficiency over ASA under visible light irradiation and an excellent structural stability after multiple uses. Compared to manganese oxide (MnO) and manganese oxynitride (MnON) nanoparticles, larger specific surface area and smaller band gap were observed for the nanocomposite accounting for the enhanced photocatalytic efficiency. Besides the compositional effect of the catalyst, we also examined the influence of various experimental parameters on the degradation of ASA such as initial concentration, catalyst dose, initial pH and additives. The best performance was obtained for the nanocomposite when the catalyst dose was 10 mg/mL and the initial pH 3. Detection of intermediates during photocatalysis showed that ASA undergoes hydroxylation, demethylation, aromatization, ring opening, and finally complete mineralization into CO₂ and H₂O by reactive species. For practical applications as a photocatalyst, cytotoxicity of the nanocomposite was also evaluated, which revealed its insignificant impact on the cell viability. These results suggest the nanocomposite of nickel-decorated manganese oxynitride on graphene nanosheets as a promising photocatalyst for the remediation of ASA-contaminated water.
Mostrar más [+] Menos [-]Biochemical toxicity, lysosomal membrane stability and DNA damage induced by graphene oxide in earthworms
2021
Zhao, Shulan | Wang, Yanli | Duo, Lian
With the growing production and use of carbon nanomaterials (CNMs), the risk of their releases to the environment has drawn much attention. However, their potential effect on soil invertebrates has not yet been systematically assessed. Herein, the toxic effects of graphene oxide (GO) on earthworms (Eisenia fetida) were thoroughly investigated. Exposure to different doses of GO (0, 5, 10, 20, and 30 g kg⁻¹) was conducted for 7, 14, 21, and 28 days. The results showed that enzymatic activity was stimulated at the early stages of exposure (7 days and 14 days) and inhibited after 14 days for catalase (CAT) and after 21 days for peroxidase (POD) and superoxide dismutase (SOD), especially at high GO doses. The content of MDA showed an increasing trend over the whole exposure period and was significantly elevated by GO from 21 days except at the dose of 5 g kg⁻¹on day 21. Lysosomal membrane stability and DNA damage presented dose- and time-dependent relationships. Graphene oxide remarkably decreased lysosomal membrane stability except at the dose of 5 g kg⁻¹ on day 7. The tail DNA%, tail length and olive tail moment increased with increasing GO dose throughout the exposure duration, reaching maximum values at the end of exposure (28 days). These findings suggest that GO induces oxidative stress and genotoxicity in Eisenia fetida, resulting in lipid peroxidation, decreased lysosomal membrane stability and DNA damage. Therefore, attention should be paid to the potential pollution and risk associated with graphene oxide application. The results can provide valuable information for environmental safety assessment of graphene nanomaterials in soil.
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