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Benzotriazole decorated graphene oxide for efficient removal of U(VI)
2019
Ding, Jie | Yan, Zijun | Feng, Lanqi | Zhai, Fuwan | Chen, Xiao | Xu, Yuwei | Tang, Siqun | Huang, Chao | Li, Laicai | Pan, N. (Ning) | He, Yi | Jin, Yongdong | Xia, Chuanqin
There is a need to develop highly efficient materials for capturing uranium from nuclear wastewater. Here, 5-methylbenzotriazole modified graphene oxide (MBTA-GO) was used to adsorb U(VI) from aqueous solution. By the trials of different conditions, we found that the removal of U(VI) from acidic solution was strongly dependent on pH but independent of ionic strength. The U(VI) adsorption was perfectly conformed to the pseudo-second-order kinetics and the adsorption isotherms were simulated by the Langmuir model well. A high removal capacity (qₘₐₓ = 264 mg/g) for U(VI) at pH 3.5 was obtained. XPS, EXAFS analyses and DFT calculations revealed that the mechanism of uranium capture was ascribed to (i) the surface complexation by benzotriazole and carboxyl groups (providing lone pair electrons) on MBTA-GO and (ii) enhanced synergistic coordination ability of delocalized π-bond of triazole group toward U due to the transfer of electrons from graphene sheet to benzotriazole. DFT calculations further demonstrated that benzotriazole displayed stronger binding with U(VI) compared to carboxyl group due to higher binding energy of [Side/Surface-U-MBTA-GO] (79.745, 54.986 kcal/mol) than [MBTA-GO–COOH–U] (27.131 kcal/mol). This work will provide valuable insight into designing novel nitrogen-containing adsorbents for practical application in wastewater treatment.
Mostrar más [+] Menos [-]A simple method for preparing ultra-light graphene aerogel for rapid removal of U(VI) from aqueous solution
2019
Zhao, Donglin | Wang, Yangyang | Zhao, Siyu | Wakeel, Muhammad | Wang, Zheng | Shaikh, Rehan S. | Hayat, Tasawar | Chen, Changlun
In this study, graphene aerogel (GA) was successfully prepared through a simple hydrothermal method. The resulting GA exhibited a porous network structure with a large specific surface area (350.8 m²/g), ultra-light mass and easy separation from water. The pHIEP value of the GA was estimated to be 3.5. The adsorption process and the factors that affect adsorption capacity were studied. The adsorption could be conducted in a wide pH range from 2.0 to 7.0. The maximum adsorption capacity of GA towards U(VI) at pH 4.0 and T = 298 K was 238.67 mg/g calculated from the Langmuir model. The GA had greatly rapid adsorption property for the removal of U(VI) at pH 4.0. Kinetic data showed good correlation with pseudo-second-order equation. Fourier transform infrared spectroscopy and X-ray photoelectron spectrometry characterizations showed that GA adsorbed U(VI) through chemical interaction by oxygen-containing and nitrogen-containing groups functional groups. The results show that GA has excellent application potential as an adsorbent material for removing U(VI) from aqueous solution.
Mostrar más [+] Menos [-]Graphite particle electrodes that enhance the detoxification of municipal solid waste incineration fly ashes in a three-dimensional electrokinetic platform and its mechanisms
2018
Huang, Tao | Zhang, Shuwen | Liu, Longfei | Xu, Jiaojiao
This paper investigated the application of graphite particle electrodes to the removal of Zn, Pb, Cu, and Cd from municipal solid waste incineration (MSWI) fly ashes in a three-dimensional (3D) electrokinetic reactor. The influences of the voltage gradient, mass ratio of graphite powers to fly ashes, nitric acid concentrations, proposing times, and liquid-solid (L-M) ratios on the remedial efficiencies of MSWI fly ashes were comprehensively studied in an orthogonal deign and a sequential double-factor setup. Significant analysis showed that changes in the mass ratios and nitric acid concentrations both had a statistically significant effect on the removals of Zn and Pb. Proposing times and L-M ratios both remarkably affected the removals of heavy metals (HMs) in a 3D electrochemical system. The graphite powers had a narrower distribution interval and slightly larger surface areas compared with MSWI fly ashes, which relented pH gradients over the time in the electrochemical experiments and minimized the bubble barricade caused by the hydrolysis. The particle electrode had increased the residue factions of Zn, Pb, Cu, and Cd in S1 region by approximately 216%, 136%, 309%, and 950%, respectively, compared with the raw MSWI fly ashes. The addition of graphite powders to a two-dimensional (2D) electrochemical process strengthened hydrolysis reactions, shortened time for the redistribution of pH balance, decreased the tortuosity of migration path, and increased the desorption concentrations of HMs in the sample area.
Mostrar más [+] Menos [-]Pristine graphene induces cardiovascular defects in zebrafish (Danio rerio) embryogenesis
2018
Manjunatha, Bangeppagari | Pak, Sŏng-ho | Kim, Kiwoong | Kundapur, Rajesh R. | Lee, Sang Joon
The multiple effect of pristine graphene (pG) toxicity on cardiovascular developmental defects was assessed using zebrafish as a model. Recently, the nanotoxicity is emerging as a critical issue, and it is more significant in embryogenesis. Especially, graphene and its derivatives have attracted a lot of interest in biomedical applications. However, very little is known about the toxic effects of pG which has been widely used carbon nanomaterial according to concentration and its effects on biological and cardiovascular development. In the present study, we examined the development of zebrafish embryos by exposing to pG (5, 10, 15, 20 and 25 μg/L) under different developmental toxicity end-points such as cardiotoxicity, cardiovascular defect, retardation of cardiac looping, apoptosis and globin expression analysis. For this, the developmental cardiotoxicity of pG at different concentrations and the specific cardiovascular defects thereof were elucidated for the first time. As a result, the exposure to pG was found to be a potential risk factor to cardiovascular system of zebrafish embryos. However, a further study on the variations of physical, molecular properties and mechanisms of nanotoxicity which vary depending on production method and surface functionalization is required. In addition, the potential risks of pG flakes to aquatic organisms and human health should be considered or checked before releasing them to the environment.
Mostrar más [+] Menos [-]Metal-free catalysis of persulfate activation and organic-pollutant degradation by nitrogen-doped graphene and aminated graphene
2016
Chen, Hao | Carroll, Kenneth C.
We evaluated three types of functionalized, graphene-based materials for activating persulfate (PS) and removing (i.e., sorption and oxidation) sulfamethoxazole (SMX) as a model emerging contaminant. Although advanced oxidative water treatment requires PS activation, activation requires energy or chemical inputs, and toxic substances are contained in many catalysts. Graphene-based materials were examined herein as an alternative to metal-based catalysts. Results show that nitrogen-doped graphene (N-GP) and aminated graphene (NH2-GP) can effectively activate PS. Overall, PS activation by graphene oxide was not observed in this study. N-GP (50 mg L−1) can rapidly activate PS (1 mM) to remove >99.9% SMX within 3 h, and NH2-GP (50 mg L−1) activated PS (1 mM) can also remove 50% SMX within 10 h. SMX sorption and total removal was greater for N-GP, which suggests oxidation was enhanced by increasing proximity to PS activation sites. Increasing pH enhanced the N-GP catalytic ability, and >99.9% SMX removal time decreased from 3 h to 1 h when pH increased from 3 to 9. However, the PS catalytic ability was inhibited at pH 9 for NH2-GP. Increases in ionic strength (100 mM NaCl or Na2SO4) and addition of radical scavengers (500 mM ethanol) both had negligible impacts on SMX removal. With bicarbonate addition (100 mM), while the catalytic ability of N-GP remained unaltered, NH2-GP catalytic ability was inhibited completely. Humic acid (250 mg L−1) was partially effective in inhibiting SMX removal in both N-GP and NH2-GP systems. These results have implications for elucidating oxidant catalysis mechanisms, and they quantify the ability of functionalization of graphene with hetero-atom doping to effectively catalyze PS for water treatment of organic pollutants including emerging contaminants.
Mostrar más [+] Menos [-]Graphene-based porous nanohybrid architectures for adsorptive and photocatalytic abatement of volatile organic compounds
2022
Vēlāyutan̲, T. A. | Rizwan, Komal | Rahdar, Abbas | Badran, Mohamed Fathy | Iqbal, Hafiz M.N.
Volatile organic compounds (VOCs) represent a considerable threat to humans and ecosystems. Strategic remediation techniques for the abatement of VOCs are immensely important and immediately needed. Given a unique set of optical, mechanical, electrical, and thermal characteristics, inimitable surface functionalities, porous structure, and substantial specific surface area, graphene and derived nanohybrid composites have emerged as exciting candidates for abating environmental pollutants through photocatalytic degradation and adsorptive removal. Graphene oxide (GO) and reduced graphene oxide (rGO) containing oxygenated function entities, i.e., carbonyl, hydroxyl, and carboxylic groups, provide anchor and dispersibility of their surface photocatalytic nanoscale particles and adsorptive sites for VOCs. Therefore, it is meaningful to recapitulate current state-of-the-art research advancements in graphene-derived nanostructures as prospective platforms for VOCs degradation. Considering this necessity, this work provides a comprehensive and valuable insight into research progress on applying graphene-based nanohybrid composites for adsorptive and photocatalytic abatement of VOCs in the aqueous media. First, we present a portrayal of graphene-based nanohybrid based on their structural attributes (i.e., pore size, specific surface area, and other surface features to adsorb VOCs) and structure-assisted performance for VOCs abatement by graphene-based nanocomposites. The adsorptive and photocatalytic potentialities of graphene-based nanohybrids for VOCs are discussed with suitable examples. In addition to regeneration, reusability, and environmental toxicity aspects, the challenges and possible future directions of graphene-based nanostructures are also outlined towards the end of the review to promote large-scale applications of this fascinating technology.
Mostrar más [+] Menos [-]Carbon nanomaterials for the detection of pesticide residues in food: A review
2022
Mishra, Smriti | Mishra, Shivangi | Patel, Shiv Singh | Singh, Sheelendra Pratap | Kumar, Pradip | Khan, Mohd Akram | Awasthi, Himani | Singh, Shiv
In agricultural fields, pesticides are widely used, but their residual presence in the environment poses a threat to humans, animals, insects, and ecosystems. The overuse of pesticides for pest control, enhancement of crop yield, etc. leaves behind a significant residual amount in the environment. Various robust, reliable, and reusable methods using a wide class of composites have been developed for the monitoring and controlling of pesticides. Researchers have discovered that carbon nanomaterials have a wide range of characteristics such as high porosity, conductivity and easy electron transfer that can be successfully used to detect pesticide residues from food. This review emphasizes the role of carbon nanomaterials in the field of pesticide residue analysis in different food matrices. The carbon nanomaterials including carbon nanotubes, carbon dots, carbon nanofibers, graphene/graphene oxides, and activated carbon fibres are discussed in the review. In addition, the review examines future prospects in this research area to help improve detection techniques for pesticides analysis.
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.
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