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Effective treatment of levofloxacin wastewater by an electro-Fenton process with hydrothermal-activated graphite felt as cathode
2020
Liu, Jia-Ming | Ji, Zhi-Yong | Shi, Ya-Bin | Yuan, Peng | Guo, Xiao-Fu | Zhao, Li-Ming | Li, Shuming | Li, Hong | Yuan, Jun-Sheng
The performance of the cathode significantly affects the ability of the electro-Fenton (EF) process to degrade chemicals. In this study, a simple method to modify the graphite felt (GF) cathode was proposed, i.e. oxidizing GF by hydrothermal treatment in nitric acid. The surface physical and electrochemical properties of modified graphite felt were characterized by several techniques: scanning electron microscope (SEM), water contact angle, X-ray photoelectron spectroscopy (XPS), Raman spectroscopy and linear scanning voltammetry (LSV). Compared with an unmodified GF (GF-0), the oxygen reduction reaction (ORR) activity of a modified GF was significantly improved due to the introduction of more oxygen-containing functional groups (OGs). Furthermore, the results showed that GF was optimally modified after 9 h (GF-9) of treatment. As an example, the H₂O₂ generation by GF-9 was 2.26 times higher than that of GF-0. After optimizing the process parameters, which include the initial Fe²⁺ concentration and current density, the apparent degradation rate constant of levofloxacin (LEV) could reach as high as 0.40 min⁻¹. Moreover, the total organic carbon (TOC) removal rate and mineralization current efficiency (MCE) of the modified cathode were much higher than that of the GF-0. Conclusively, GF-9 is a promising cathode for the future development in organic pollutant removal via EF.
Show more [+] Less [-]Simultaneous energy harvest and nitrogen removal using a supercapacitor microbial fuel cell
2020
Cai, Teng | Jiang, Nan | Zhen, Guangyin | Meng, Lijun | Song, Jialing | Chen, Gang | Liu, Yanbiao | Huang, Manhong
The insufficient removal of pollutants and bioelectricity production have become a bottleneck for high-concentration saline wastewater treatment through microbial fuel cell (MFC) technology. Herein, a novel supercapacitor MFC (SC-MFC) was constructed with carbon nanofibers composite electrodes to investigate pollutant removal ability, power generation, and electrochemical properties using real landfill leachate. The possible extracellular electron transfer and nitrogen element conversion pathways in the bioanode were also analyzed. Results showed that the SC-MFC had higher pollutant removal rates (COD: 59.4 ± 1.2%; NH₄⁺-N: 78.2 ± 1.6%; and TN: 77.8 ± 1.2%), smaller internal impedance Rₜ (∼6 Ω), higher exchange current density i₀ (2.1 × 10⁻⁴ A cm⁻²), and a larger catalytic current j₀ (704 μA cm⁻²) with 60% leachate than those with 10% and 20% leachate, resulting in a power output of 298 ± 22 mW m⁻². Ammonium could be incorporated by chemoautotrophic bacteria to produce organic compounds that could be further utilized by heterotrophs to generate power when biodegradable organic matters are depleted. Three conversion pathways of nitrogen might be involved, including NH₄⁺ diffusion from anode to cathode chamber, nitrification, and the denitrification process. Additionally, cyclic voltammetry tests showed that both the direct electron transfer (DET) and the mediator electron transfer in bioanode were involved and dominated by DET. The microbial analysis revealed that the bioanode was dominated by salt-tolerant denitrifying bacteria (38.5%), which was deduced to be the key functional microorganism. The electrochemically active bacteria decreased significantly from 61.7% to 4% over three stages of leachate treatment. Overall, the SC-MFC has demonstrated the potential for wastewater treatment along with energy harvesting and provides a new avenue toward sustainable leachate management.
Show more [+] Less [-]Determination of bisphenol A and bisphenol S by a covalent organic framework electrochemical sensor
2020
Pang, Yue-Hong | Huang, Yu-Ying | Wang, Li | Shen, Xiao-Fang | Wang, Yi Ying
Bisphenol A (BPA) is a widely produced chemical that is mainly used as raw material for manufacturing plastic products. It is an endocrine disruptor and causes irreversible damage to the human body. Bisphenol S (BPS), an alternative to BPA, has low dose effects on toxicology and genotoxicity. Herein, we constructed a highly porous crystalline covalent organic framework (COF, CTpPa-2)-modified glassy carbon electrode (GCE) for the electrochemical sensing of BPA and BPS. The electrochemical properties of the CTpPa-2/GCE were characterized using galvanostatic charge-discharge, cyclic voltammetry and differential pulse voltammetry. The CTpPa-2/GCE exhibited remarkable electrocatalytic activity, and the electrochemical responses for BPA and BPS were found to be linear in the concentration ranges of 0.1–50 μM and 0.5–50 μM with detection limits of 0.02 μM and 0.09 μM (S/N = 3), respectively. Moreover, the fabricated sensor was utilized to determine BPA and BPS in bottle samples with recoveries of 87.0%–92.2% and migration rates of 13.2%–28.0%.
Show more [+] Less [-]Adsorption Mechanisms and Electrochemical Properties of Methyl Blue onto Magnetic NixMgyZn(1-x-y)Fe2O4 Nanoparticles Fabricated Via the Ethanol-Assisted Combustion Process
2020
Yu, Lulu | Li, You | Pan, Shuai | Huang, Wei | Liu, Ruijiang
Magnetic NiₓMgyZn₍₁₋ₓ₋y₎Fe₂O₄ nanoparticles were fabricated via the ethanol-assisted combustion process. The characterizations of the nanoparticles were illuminated by SEM, EDS, XRD, and VSM. The specific surface area and pore diameter distribution were measured by the Brunauer–Emmett–Teller (BET) measurement. Magnetic Ni₀.₄Mg₀.₃Zn₀.₃Fe₂O₄ nanoparticles calcined at 400 °C for 2 h with anhydrous ethanol of 20 mL were chosen to remove methyl blue (MB), and their adsorption performances for removal of MB from water environment were evaluated. Adsorption kinetics and adsorption isotherm experiments had been carried out; the adsorption mechanisms were well demonstrated by the pseudo-second-order kinetics model and Temkin isotherm model, respectively, which indicated that the removal of MB by Ni₀.₄Mg₀.₃Zn₀.₃Fe₂O₄ adsorbent was multimolecular layer chemisorption mechanism. The pH effect of the dye solutions was explored to reveal that the adsorption capacity remained a solidly high level when pH was above 5. After three times of recycling, the relative removal activity of MB onto the nanoparticles remained above 97.6% of its original removal activity. The adsorption process of MB removed by Ni₀.₄Mg₀.₃Zn₀.₃Fe₂O₄ adsorbent was further illuminated by cyclic voltammetry (CV) and electrochemical impedance spectra (EIS). Graphical Abstract Magnetic Ni₀.₄Mg₀.₃Zn₀.₃Fe₂O₄ nanoparticles were fabricated by the ethanol-assisted combustion method, and they were chosen to remove methyl blue. Adsorption experiments were performed, and the pseudo-second-order kinetics model and the Temkin isotherm model fitted well with the experimental data. When pH was above 5, the adsorption capacity remained at a solidly high level. After three times of recycling, the relative removal activity of the nanoparticles remained above 97.6% of its original removal activity. The adsorption process was further illuminated by CV and EIS.
Show more [+] Less [-]Electroactive Manganese Oxide–Reduced Graphene Oxide Interfaced Electrochemical Detection of Urea
2020
Ramasami Sundhar Baabu, Priyannth | Gumpu, Manju Bhargavi | Nesakumar, Noel | Rayappan, John Bosco Balaguru | Kulandaisamy, Arockia Jayalatha
Urea, being a nitrogen fertilizer, is crucial for plant growth but when excessively provided (above biuret 2% levels specified by the World Health Organization), plant characteristics are deeply affected. A real-time sensor to check the presence of excess urea in plants is therefore necessary. Towards this goal, a manganese oxide–reduced graphene oxide composite was synthesized by modified Hummer’s method and precipitation techniques, which was subsequently used as a nano-interface to immobilize urease enzyme for specific detection of urea. The synthesized nanocomposite helped in shuttling of electrons between the redox species and in enhanced electron transfer rate due to their high surface area, vindicated by their structural and morphological characterization using X-ray diffractometer (XRD), scanning electron microscope (SEM), and X-ray photoelectron spectrometer (XPS), and electrochemical characterization using cyclic voltammetry and amperometry, respectively. The fabricated biosensor for urea exhibited a linear range of 5–100 μM with a sensitivity of 9.7 × 10⁻³ μA μM⁻¹, limit of detection of 14.693 μM, and a response time of 118 s.
Show more [+] Less [-]Novel Electrochemical Sensor Based on Nylon 6,6-Modified Graphite HB Pencil Electrode for Chlorothalonil Determination by Differential Pulse Cathodic Stripping Voltammetry
2020
Thanalechumi, Paramalinggam | Yusoff, Abdull Rahim Mohd | Yusop, Zulkifli
Mercury-based electrode was the choice of electrode material for many years, and it has been extensively used in voltammetry studies. Nonetheless, alternative electrode materials are highly preferred in voltammetry studies due to the toxicity of mercury. This work introduces a novel green sensor, nylon 6,6-modified graphite HB pencil electrode (Nyl-MHBPE) as electrochemical method for chlorothalonil determination by differential pulse cathodic stripping voltammetry (DPCSV). The Nyl-MHBPE was significantly improved electroactivity towards the reduction of chlorothalonil, under the optimal conditions (at pH 8.0). It was clearly observed that nylon 6,6 revealed as an efficient modifier for enhancing stripping signal for voltammetric analysis. Moreover, the developed sensor showed great feature such as a remarkably low detection limit in nanomolar level (0.94 × 10⁻⁸ M) with a linear range from 1 to 26 × 10⁻⁷ M. It presented excellent repeatability with high sensitivity and selectivity. Besides, analysis of chlorothalonil in real water samples was successfully carried out with good recovery values (92.5–103%) and relative standard deviation (RSD) values < 2.2%. The performance of Nyl-MHBPE was also compared to bare pencil electrode (HBPE). Another significant feature of this work is that the conductivity properties of the Nyl-MHBPE were superior as compared to hanging mercury drop electrode (HMDE). The present study provides admirable merits that make the Nyl-MHBPE selected as a promising electrochemical sensor to perform routine analysis of chlorothalonil.
Show more [+] Less [-]Enhancement of NOx photo-oxidation by Fe- and Cu-doped blue TiO2
2020
Martínez Oviedo, Adriana | Ray, Schindra Kumar | Joshi, Bhupendra | Lee, Soo Wohn
The present work is focused on the removal of NOx with reduced blue TiO₂ with Fe (blue Fe-TiO₂)- and Cu (blue Cu-TiO₂)-doped photocatalyst. TiO₂ was reduced via lithium in EDA (blue TiO₂). Fe and Cu ions were doped in the reduced TiO₂ (blue Fe-TiO₂ and blue Cu-TiO₂). The material resulted in a core-shell structure of amorphous and anatase phase. XPS suggests the existence of Ti³⁺ species and oxygen vacancies within the structure of TiO₂. Additionally, valence bond (VB)-XPS shows the generation of intermediate levels at the band edge of the doped photocatalyst. Photocurrent, electrochemical impedance spectroscopy and cyclic voltammetry confirmed the enhanced charge-separation process in doped reduced TiO₂. The photocatalysts were tested for the photo-oxidation of NOx. Blue Fe-TiO₂ reveals the efficiency of 70% for NO elimination and 44.74% for NO₂ formation. The improved efficiency of the doped photocatalyst is related to the re-engineered structure with Ti³⁺ species, oxygen vacancies, and charge traps. Electron spin resonance (ESR) measurement was carried out for blue Fe-TiO₂ to confirm the formation of reactive oxygen species (ROS). Furthermore, ion chromatography was used to investigate the mechanism of NOx oxidation. In conclusion, the doped blue TiO₂ has a strong tendency to photo-oxidize NOx gasses.
Show more [+] Less [-]Treatment of mixed dairy and dye wastewater in anode of microbial fuel cell with simultaneous electricity generation
2020
Tajdid Khajeh, Rana | Aber, Soheil | Nofouzi, Katayoon | Ebrahimi, Sirous
Microbial fuel cell (MFC) is a green technology that converts the stored chemical energy of organic matter to electricity; therefore, it can be used for wastewater purification and energy production simultaneously. In this study, three kinds of dairy products, including milk, cheese water, and yogurt water, were mixed with Acid orange 7 (AO7) as the model wastewater and used as the anolyte of an MFC. The capability of the system in energy production and dye removal was also investigated. The FESEM images were used to investigate the biofilms attachment to the anodes. Moreover, the polarization curves, electrochemical impedance spectroscopy, cyclic voltammetry (CV), voltage–time profiles, and coulombic efficiency were used to evaluate the electrochemical activity of the MFCs. Based on the CV results, the biofilm formation significantly improved the electrochemical activity of the electrodes. Maximum power density, voltage, and coulombic efficiency were obtained as 44.05 mW.m⁻², 332.4 mV, and 1.76%, respectively, for cheese water + AO7 anolyte, but the milk + AO7 MFC produced a stable voltage for a long time and its performance was similar to the cheese water + AO7 anolyte. Maximum COD removal and decolorization efficiencies were obtained equal to 84.57 and 92.18% for yogurt water + AO7 and cheese water + AO7 anolytes, respectively.
Show more [+] Less [-]Potentiometric polyphenol oxidase biosensor for sensitive determination of phenolic micropollutant in environmental samples
2020
Yashas, Shivamurthy Ravindra | Sandeep, Shadakshari | Shivakumar, Ballagere Puttaraju | Swamy, Ningappa Kumara
The present study demonstrates the development of polyphenol oxidase (PPO) biosensor for the detection of catechol using strontium copper oxide (SrCuO₂) and polypyrrole nanotubes (PPyNT) matrix. The SrCuO₂ micro-seeds, a perovskite compound, are synthesized by co-precipitation under pH 8.0. The as-synthesized micro-seeds are characterized by scanning electron microscopy (SEM), field emission scanning electron microscopy (FE-SEM), energy-dispersive X-ray spectroscopy (EDX), and X-ray diffraction spectroscopy (XRD). The proposed sensor is fabricated on pencil graphite (P-Gr) by successive deposition of PPyNT, SrCuO₂, and PPO enzyme. The developed PPO/SrCuO₂/PPyNT/P-Gr sensor is characterized by cyclic voltammetry (CV), differential pulse voltammetry (DPV), and electrochemical impedance spectroscopy (EIS) techniques. The PPO/SrCuO₂/PPyNT/P-Gr displayed excellent electrocatalytic activity towards the oxidation and detection of catechol. The as-developed sensor showed sensitive response ascribing to limit of detection (LOD) of 0.15 μM and sensitivity of 15.60 μA μM⁻¹ cm⁻². The fabricated sensor exhibited excellent repeatability and longer shelf life. The proposed biosensor finds its application within the broad linear range of 1–50 μM. Real sample analysis of mineral water, tap water, and domestic wastewater using developed sensor showed acceptable recovery. Hence, the biosensor endeavors its application in environmental monitoring and protection.
Show more [+] Less [-]Fabrication of multi-walled carbon nanotubes and carbon black co-modified graphite felt cathode for amoxicillin removal by electrochemical advanced oxidation processes under mild pH condition
2020
Pan, Guifang | Sun, Xiuping | Sun, Zhirong
Hydrogen peroxide (H₂O₂) electrogenerated via two-electron oxygen reduction reaction at cathode plays an important role in electrochemical advanced oxidation processes for organic pollutants removal from wastewater. Herein, multi-walled carbon nanotubes and carbon black co-modified graphite felt electrode (MWCNTs-CB/GF) was prepared as an efficient cathode for H₂O₂ electrogeneration and amoxicillin removal by anodic oxidation with hydrogen peroxide (AO-H₂O₂) and electro-Fenton (EF) under mild pH condition. Besides, the physicochemical and electrochemical properties of MWCNTs-CB/GF were characterized by scanning electron microscopy, N₂ adsorption and desorption experiment, contact angle measurement, X-ray photoelectron spectroscopy, and linear sweep voltammetry. Compared with GF, MWCNTs-CB/GF showed a higher H₂O₂ generation of 309.0 mg L⁻¹ with a current efficiency of 60.9% (after 120 min) and more effective amoxicillin removal efficiencies of 97.5% (after 120 min) and 98.7% (after 30 min) in AO-H₂O₂ and EF (with 0.5 mM Fe²⁺) processes, under the condition of current density 12 mA cm⁻² and initial pH 5.5. Meanwhile, the TOC removal efficiency was 45.2% during EF process after 120 min. Anodic oxidation, H₂O₂ oxidation, and methanol capture indicated that ∙OH generated via electro-activation reaction at MWCNTs-CB/GF and Fenton reaction in solution played the dominant role in amoxicillin removal. Moreover, the TOC removal was associated with ∙OH generated during Fenton reaction in the solution. The major intermediates of AMX degradation by EF process were identified using LC-MS and the possible degradation pathways were proposed containing of β-lactam ring opening, hydroxylation reaction, decarboxylation reaction, methyl groups in the thiazolidine ring oxidation reaction, bond cleavage, and rearrangement processes. All of the above results proved that MWCNTs-CB/GF was an excellent cathode for AMX degradation under mild pH condition.
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