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Hexachloroethane dechlorination in sulfide-containing aqueous solutions catalyzed by nitrogen-doped carbon materials
2021
Liu, Na | Hu, Qing | Wang, Chao | Tong, Lizhi | Weng, Chih-Huang | Ding, Longzhen
This study demonstrated that nitrogen-doped carbon materials (NCMs) could effectively catalyze the chlorine elimination process in hexachloroethane (HCA) declorination in sulfide-containing environments for the first time. The kₒbₛ values of HCA dechlorination by sulfide in the presence of 10 mg/L NCMs were higher than that of no mediator at pH 7.3 by one or two orders of magnitude. The catalytic capabilities of NCMs on HCA dechlorination were evident in common ranges of natural pH (5.3–8.9) and it could be accelerated by the increase of pH but be suppressed by the presence of dissolved humic acid. Moreover, NCMs exhibited much better catalytic capability on HCA dechlorination compared to the carbon materials, mainly owing to the combined contributions of pyridine N, including enhanced nucleophilic attack to HCA molecule by generating newborn C–S–S and activation of HCA molecule by elongating C–Cl bonds. The functions of pyridine N in micron-sized NCMs with mesopores were better than in nano-sized NCMs on HCA dechlorination. These findings displayed the potential of NCMs, when released into sulfide-containing environments, may significantly increase the dechlorination of chlorinated aliphatic hydrocarbons.
Show more [+] Less [-]Nano-magnetite supported by biochar pyrolyzed at different temperatures as hydrogen peroxide activator: Synthesis mechanism and the effects on ethylbenzene removal
2020
Yan, Jingchun | Yang, Lei | Qian, Linbo | Han, Lu | Chen, Mengfang
Nano-magnetite supported by biochar (nFe₃O₄/BC) pyrolyzed at temperatures of 300 °C–600 °C was developed to activate hydrogen peroxide (H₂O₂) for the efficient degradation of ethylbenzene in aqueous solution. It was revealed that the degradation efficiency of ethylbenzene and TOC removal were 96.9% and 36.2% respectively after the reaction for 40 min in the presence of initial concentration of 0.1 mmol L⁻¹ ethylbenzene, 2.76 g L⁻¹ nFe₃O₄/BC₅₀₀ with the mass ratio of nFe₃O₄ to BC₅₀₀ of 4:1 and 2.0 mmol L⁻¹ H₂O₂ at pH 7.0. Based on electron paramagnetic resonance (EPR), quenching experiment and X-ray photoelectron spectroscopy (XPS) data, both OH and O₂⁻ radicals were generated in the nFe₃O₄/BC₅₀₀ activated H₂O₂ system, and the OH radicals were the predominant species for the degradation of ethylbenzene. Through electron transfer process, mechanisms of Fe(II), phenolic hydroxyl group and persistent free radicals (PFRs) on BC surfaces accounted for the generation of OH radicals, and Fe(III) in nFe₃O₄ and formed from Fe(II) oxidation responsible for the generation of O₂⁻ radicals in the nFe₃O₄/BC activated H₂O₂ system were proposed.
Show more [+] Less [-]Chemical stability of metallic nanoparticles: A parameter controlling their potential cellular toxicity in vitro
2009
Auffan, Mélanie | Rose, Jerome | Wiesner, Mark R. | Bottero, Jean-Yves
The level of production of nanoparticles will inevitably lead to their appearance in air, water, soils, and organisms. A theoretical framework that relates properties of nanoparticles to their biological effects is needed to identify possible risks to human health and the environment. This paper considers the properties of dispersed metallic nanoparticles and highlights the relationship between the chemical stability of these nanoparticles and their in vitro toxicity. Analysis of published data suggests that chemically stable metallic nanoparticles have no significant cellular toxicity, whereas nanoparticles able to be oxidized, reduced or dissolved are cytotoxic and even genotoxic for cellular organisms. The ability of metallic nanoparticles to be oxidized, reduced or dissolved in biological media can be used to predict their toxicity in vitro.
Show more [+] Less [-]Remediation of a chlorinated aromatic hydrocarbon in water by photoelectrocatalysis
2009
Nissen, Silke | Alexander, B. D. (Bruce D) | Dawood, Ilyas | Tillotson, Martin | Wells, Richard P.K. | Macphee, D. E. (Donald E) | Killham, Kenneth
Photoelectrocatalysis driven by visible light offers a new and potentially powerful technology for the remediation of water contaminated by organo-xenobiotics. In this study, the performance of a visible light-driven photoelectrocatalytic (PEC) batch reactor, applying a tungsten trioxide (WO3) photoelectrode, to degrade the model pollutant 2,4-dichlorophenol (2,4-DCP) was monitored both by toxicological assessment (biosensing) and chemical analysis. The bacterial biosensor used to assess the presence of toxicity of the parent molecule and its breakdown products was a multicopy plasmid lux-marked E. coli HB101 pUCD607. The bacterial biosensor traced the removal of 2,4-DCP, and in some case, its toxicity response suggests the identification of transient toxic intermediates. The loss of the parent molecule, 2,4-DCP determined by HPLC, corresponded to the recorded photocurrents. Photoelectrocatalysis offers considerable potential for the remediation of chlorinated hydrocarbons, and that the biosensor based toxicity results identified likely compatibility of this technology with conventional, biological wastewater treatment. Visible light-driven photoelectrocatalysis has potential as a remediation technology in wastewater treatment.
Show more [+] Less [-]Catalytic air pollution control
1995
Heck, Ronald M. | Farrauto, Robert J.
Reduction of nitrobenzene with sulfides catalyzed by the black carbons from crop-residue ashes
2014
Gong, Wenwen | Liu, Xinhui | Tao, Li | Xue, Wei | Fu, Wenjun | Cheng, Dengmiao
In this paper, three types of black carbons (BCs) named R-BC, W-BC, and C-BC were derived from rice straw ashes, wheat straw ashes, and corn straw ashes, respectively. Under room temperature and in an anaerobic aqueous solution, these three types of BCs could catalyze the reduction of nitrobenzene (NB) by sulfides rather than only act as the superabsorbent. The catalytic activities of BCs derived from different crop-residue ashes were very different and in the order of R-BC > W-BC > C-BC, since the reaction rate constants (k ₒbₛ) of NB with the BCs in the presence of 3 mM sulfides were 0.0186, 0.0063, and 0.0051 h⁻¹, respectively. The key catalytic active sites for NB reduction were evaluated, with four types of modified BCs and two types of tailored graphite as the model catalysts. The results indicated that BCs probably had two types of active sites for NB reduction, the microscopic graphene moieties and the surface oxygen functional groups. Since the sulfides and BCs often coexist in the environment, this BC-catalyzed reduction technology of NACs may be applied as an in situ remediation technique without the need for reagent addition.
Show more [+] Less [-]Decomposition of NO in automobile exhaust by plasma–photocatalysis synergy
2014
Chen, Meng | Jin, Lisheng | Liu, Yanhua | Guo, Xiurong | Chu, Jiangwei
The combination of plasma discharge and TiO₂ photocatalysis exhibits high performances in the removal of nitrogen monoxide (NO). This article is aimed at elucidating the relationships between NO decomposition efficiency and various experimental parameters, including voltages, humidity and temperature. The experimental results indicate that the efficiency of NO removal by synergic plasma-catalyst coupling is significantly higher than plasma only or photocatalyst only systems. Moreover, the NO removal efficiency improves with the increase of applied voltage. Meanwhile, a higher humidity results in a reduced number of electron–hole pairs at the surface of TiO₂ photocatalyst, leading to lower synergic purification efficiencies. Finally, the efficiency of NO removal is raised with the increase of temperature due to the fact that the adsorption of NO and water by nano-TiO₂ is affected by environmental temperature.
Show more [+] Less [-]Using iron-loaded sepiolite obtained by adsorption as a catalyst in the electro-Fenton oxidation of Reactive Black 5
2013
Iglesias, O. | Fernández de Dios, M. A. | Pazos, M. | Sanromán, M. A.
This study explores the possibility of using iron-loaded sepiolite, obtained by recovering iron from polluted water, as a catalyst in the electro-Fenton oxidation of organic pollutants in textile effluents. The removal of iron ions from aqueous solution by adsorption on sepiolite was studied in batch tests at iron concentrations between 100 and 1,000 ppm. Electro-Fenton experiments were carried out in an electrochemical cell with a working volume of 0.15 L, an air flow of 1 L/min, and 3 g of iron-loaded sepiolite. An electric field was applied using a boron-doped diamond anode and a graphite sheet cathode connected to a direct current power supply with a constant potential drop. Reactive Black 5 (100 mg/L) was selected as the model dye. The adsorption isotherms proved the ability of the used adsorbent. The removal of the iron ion by adsorption on sepiolite was in the range of 80-100 % for the studied concentration range. The Langmuir and Freundlich isotherms were found to be applicable in terms of the relatively high regression values. Iron-loaded sepiolite could be used as an effective heterogeneous catalyst for the degradation of organic dyes in the electro-Fenton process. Successive batch processes were performed at optimal working conditions (5 V and pH 2). The results indicate the suitability of the proposed combined process, adsorption to iron remediation followed by the application of the obtained iron-loaded sepiolite to the electro-Fenton technique, to oxidize polluted effluents.
Show more [+] Less [-]Ag/ZnO hollow sphere composites: reusable photocatalyst for photocatalytic degradation of 17α-ethinylestradiol
2014
Li, Yi | Wang, Yuming | Liu, Linhua | Wang, Dawei | Zhang, Wenlong
Characterizations of Ag/ZnO hollow sphere by scanning electron microscopy, X-ray diffraction, X-ray photoelectron spectra, and UV–vis absorption spectra have been made after its synthesis. The results showed that the composite was hollow structure with diameters of about 1–4 μm. The samples synthesized were tested and identified as silver doped ZnO, which have extended and boosted the spectral absorption. The photocatalytic activity of Ag/ZnO hollow spheres was assessed using 17α-ethinylestradiol aqueous solution under UV irradiation. It has been observed that the 17α-ethinylestradiol absorption efficiency and degradation rate is higher for Ag/ZnO hollow spheres. As reusable photocatalysts, Ag/ZnO hollow spheres which could be easily separated from a suspension will facilitate their application in wastewater treatment with enhanced photostability.
Show more [+] Less [-]H2S photocatalytic oxidation over WO3/TiO 2 Hombikat UV100
2014
Alonso-Tellez, Angela | Robert, Didier | Keller, Valérie | Keller, Nicolas
Hydrogen sulfide (H₂S) is a toxic, corrosive and malodorous compound with damaging effects even when present at a low concentration in air. Consequently, the development of efficient and environmentally friendly remediation technologies as an alternative to conventional techniques is justified for environmental reasons and public concern over human health and well-being. In the context of indoor air quality control, the use of photocatalysis over semi-conductor oxides could be a valuable alternative purification technology due to its wide-ranging effect and its easy way of implementation. The superiority of the TiO₂Hombikat UV100 photocatalyst in comparison with the Aeroxide© TiO₂P25 standard was already apparent in the UV-A photocatalytic oxidation of H₂S. We report here on the first use of WO₃/TiO₂UV100 photocatalysts for this reaction. Associating WO₃to TiO₂UV100 was not beneficial in terms of semiconductor coupling and of charge transfer between both phases. Even if such coupled wide band-gap oxide semi-conductor photocatalysts suffered from on-flow deactivation due to the formation of poisoning sulfates as ultimate reaction products continuously stored at the surface, by contrast, their ability to strongly lower and delay the release of SO₂to the gas phase was very positive for maintaining a weak selectivity into the unwanted SO₂by-product.
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