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Energy and environmental applications of Sn4+/Ti4+ doped α-Fe2O3@Cu2O/CuO photoanode under optimized photoelectrochemical conditions
2021
Nagappagari, Lakshmana Reddy | Lee, Jaewon | Lee, Hyeonkwon | Jeong, Beomgyun | Lee, Kiyoung
The most promising technique for directly converting solar energy into clean fuels and environmental remediation by organic dye degradation is photoelectrochemical (PEC) process. We introduced Sn⁴⁺/Ti⁴⁺ doped α-Fe₂O₃@CuₓO heterojunction photoanode with complete optimization for PEC hydrogen (H₂) generation and organic dye degradation. Improvement of photocurrent photo and reducing overpotentials under optimized conditions lead to enhancing PEC performances, degradation efficiency of organic compounds, and H₂ generation generation rate. The optimized heterojunction photoanode (5TiFe@CuₓO-D) showed IPCE exceeding 42% compared with pristine hematite (Fe₀.₀₁–800₆ₕ) nanostructures (28%). Additionally, all the optimized photoanodes showed higher PEC stability for 10 h. Time-resolved PL spectra confirm the improved average lifetime for heterojunction photoanodes, supporting the enhanced PEC performance. Optimized 5TiFe@CuₓO-D material achieved PEC H₂ generation of ∼300 μL h⁻¹.cm⁻² which is two times higher than pristine hematite’s activity (150 μL h⁻¹.cm⁻²) and almost 99% degradation efficiency within 120 min of irradiation time. Therefore, a state-of-the-art study has been explored for hematite-based heterojunction photoanodes reflecting the superior PEC performance and hydrogen, methyl orange (MO) dye degradation activities. The improved results were reported because of stable morphology and better crystallinity acquired through systematic investigation of thermal effects and hydrothermal duration, improved electrical properties by Sn/Ti doping into the lattice of α-Fe₂O₃ and optimization of CuₓO deposition methods. The formation of well-defined heterojunction minimizes the recombination of the charge carrier and leads to effective transportation of excited electrons for the enhanced PEC performance.
اظهر المزيد [+] اقل [-]Integration of biochar into Ag3PO4/α-Fe2O3 heterojunction for enhanced reactive oxygen species generation towards organic pollutants removal
2022
Qian, Yifan | Shi, Jun | Yang, Xianni | Yuan, Yangfan | Liu, Li | Zhou, Ganghua | Yi, Jianjian | Wang, Xiaozhi | Wang, Shengsen
A biochar (BC) harbored Ag₃PO₄/α-Fe₂O₃ type-Ⅰ heterojunction (Ag-Fe-BC) was prepared by a hydrothermal-impregnation method to transfer active center of heterojunctions. The electrochemical and spectroscopic tests demonstrated that BC enhanced the catalytic performance of the heterojunction by enhancing photocurrent, reducing fluorescence intensity, and facilitating separation of electron-hole pairs. The photocatalytic activity showed the Ag-Fe-BC (5:1:3) could degrade Rhodamine B (20 mg/L) by up to 92.7%, which was 3.35 times higher than Ag₃PO₄/α-Fe₂O₃. Tetracycline and ciprofloxacin (20 mg/L) were degraded efficiently by 58.3% and 79.4% within 2 h, respectively. Electron paramagnetic resonance and scavenging experiments confirmed the major reactive oxygen species (ROS) consisted of singlet oxygen (¹O₂) and superoxide (·O₂⁻). Excellent RhB adsorption and electrons capturing capacity of BC facilitated electron-hole pairs separation and ROS transferring to target organics followed by elevated degradation. Thus, a facile method was proposed to synthesize a highly efficient visible-light responsive photocatalyst for degradation of various organics in water.
اظهر المزيد [+] اقل [-]Coupled with EDDS and approaching anode technique enhanced electrokinetic remediation removal heavy metal from sludge
2021
Tang, Jian | Qiu, Zhongping | Tang, Hengjun | Wang, Haiyue | Sima, Weiping | Liang, Chao | LIao, Yi | Li, Zhihua | Wan, Shan | Dong, Jianwei
In this work, the novel technology was used to remove heavy metal from sludge. The coupled with biodegradable ethylenediamine disuccinic acid (EDDS) and approaching anode electrokinetic (AA-EK) technique was used to enhance heavy metal removing from sludge. Electric current, sludge and electrolyte characteristics, heavy metal removal efficiency and residual content distribution, and heavy metal fractions percentage of variation were evaluated during the electrokinetic remediation process. Results demonstrated that the coupled with EDDS and AA-EK technique obtain a predominant heavy metal removal efficiency, and promote electric current increasing during the enhanced electrokinetic remediation process. The catholyte electrical conductivity was higher than the anolyte, and electrical conductivity of near the cathode sludge achieved a higher value than anode sludge during the coupled with EDDS and AA-EK remediation process. AA-EK technique can produce a great number of H⁺, which caused the sludge acidification and pH decrease. Cu, Zn, Cr, Pb, Ni and Mn obtain the highest extraction efficiency after the coupled with EDDS and AA-EK remediation, which were 52.2 ± 2.57%, 56.8 ± 3.62%, 60.4 ± 3.62%, 47.2 ± 2.35%, 53.0 ± 3.48%, 54.2 ± 3.43%, respectively. Also, heavy metal fractions analysis demonstrated that the oxidizable fraction percentage decreased slowly after the coupled with EDDS and AA-EK remediation.
اظهر المزيد [+] اقل [-]Comparison of electrokinetic soil remediation methods using one fixed anode and approaching anodes
2007
Shen, Z. | Chen, X. | Jia, J. | Qu, L. | Wang, W.
During the cation exchange membrane (CEM) enhanced electrokinetic (EK) soil remediation, the nearer to the anode, the higher are the H+ concentrations and the redox potentials. As both low pH and high redox potential are helpful to speedup Cd electro-migration, soils near the anode can be quickly remedied. Usually EK process is operated with one fixed anode (FA). A novel CEM enhanced EK method with approaching anodes (AAs) is proposed to accelerate electro-migration effect. Several mesh Ti/Ru anodes were inserted as AAs in the treated soil. They were switched in turn from the anode towards the cathode. Thus high H+ ions concentrations and high redox potentials quickly migrate to the cathode. Consequently, soil remediation is accelerated and nearly 44% of energy and 40% of time can be saved. The mechanism of Cd electro-migration behavior in soils during CEM enhanced EK is described as the elution in an electrokinetically driven chromatogram. During electrokinetic remediation, the nearer to the anode, the higher are the Cd removal velocities. A novel method with approaching anodes is proposed to accelerate remediation effect.
اظهر المزيد [+] اقل [-]Mechanistic insights into soil heavy metals desorption by biodegradable polyelectrolyte under electric field
2022
Wang, Yuchen | Li, Ang | Ren, Binqiao | Han, Zijian | Lin, Junhao | Zhang, Qiwei | Cao, Tingting | Cui, Chongwei
In this study, we firstly used alginate to enhance an electrokinetic technology to remediate soil contaminated with divalent heavy metals (Pb²⁺, Cu²⁺, Zn²⁺). The mechanisms of alginate-associated migration of metal ions in electric field were confirmed. Alginate resulted in a high electrical current during electrokinetic process, and soil conductivity also increased after remediation. Obvious changes in both electroosmotic flow and soil pH were observed. Moreover, these factors were affected by increasing alginate dosage. The highest Cu (95.82%) and Zn (97.33%) removal efficiencies were obtained by introducing 1 wt% alginate. Alginate can desorb Cu²⁺ and Zn²⁺ ions from soil by forming unstable gels, which could be dissociated through electrolysis. However, Pb²⁺ ions did not easily migrate out of the contaminated soil. The density functional theory (DFT) calculations show Pb²⁺ ions could form a more stable coordination sphere in metal complexes than Cu²⁺ and Zn²⁺ ions. The metal removal efficiency was decreased by increasing alginate dosage at a high level. More alginate could provide more carboxyl ligands for divalent metal ions to stabilize gels, which were difficult to dissociate by electrolysis. In summary, the results indicate it is potential for introducing alginate into an electrokinetic system to remediate Cu- and Zn- contaminated soil.
اظهر المزيد [+] اقل [-]Electrocoagulation applied for textile wastewater oxidation using iron slag as electrodes
2022
De Maman, Rafaela | da Luz, Vilson Conrado | Behling, Laura | Dervanoski, Adriana | Dalla Rosa, Clarissa | Pasquali, Gean Delise Leal
The indigo blue dye is widely used in the textile industry, specifically in jeans dyeing, the effluents of which, rich in organic pollutants with recalcitrant characteristics, end up causing several environmental impacts, requiring efficient treatments. Several pieces of research have been conducted in search of effective treatment methods, among which is electrocoagulation. This treatment consists of an electrochemical process that generates its own coagulant by applying an electric current on metallic electrodes, bypassing the use of other chemical products. The purpose of this study was to evaluate the potential use of iron slag in the electrocoagulation of a synthetic effluent containing commercial indigo blue dye and the effluent from a textile factory. The quantified parameters were color, turbidity, pH, electrical conductivity, sludge generation, phenol removal, chemical oxygen demand (COD), and total organic carbon (TOC). The electrocoagulation treatment presented a good efficiency in removing the analyzed parameters, obtaining average removal in the synthetic effluent of 85% of color and 100% of phenol after 25 min of electrolysis. For the effluent from the textile factory, average reductions of 80% of color reaching 177.54 mg Pt CoL⁻¹, 91% of turbidity reaching 93.83 NTU (nephelometric turbidity unit), 100% of phenol, 55% of COD with a final concentration of 298.8 mg O₂ L⁻¹, and 73% of TOC with a final concentration of 56.21 mg L⁻¹, in 60 min of electrolysis. The reduced time for removal of color and phenolic compounds in synthetic effluent demonstrates the complexity of treating the real effluent since to obtain removals of the same order a 60-min period of electrolysis was necessary. The results obtained demonstrate the potential of using iron slag as an electrode in the electrocoagulation process in order to reuse industrial waste and reduce costs in the treatment and disposal of solid waste. Thus, the slag can be seen as an alternative material to be used in electrocoagulation processes for the treatment of effluents from the textile industry under the experimental conditions presented, its only limitation being the fact that it is a waste and therefore does not have a standardization in the amounts of iron present in the alternative electrodes.
اظهر المزيد [+] اقل [-]Photocatalytic degradation of imidacloprid by optimized Bi2WO6/NH2-MIL-88B(Fe) composite under visible light
2022
Chen, Mao-Long | Lu, Tian-Hui | Li, Shan-Shan | Wen, Li | Xu, Zhou | Cheng, Yun-Hui
Imidacloprid as a widely used neonicotinoid insecticide can cause harmful pesticide residue inevitably. Metal-organic frameworks (MOFs) were innovatively composited to improve the light absorption and degradation performance of Bi₂WO₆ semiconductor, which expanded the photodegradation application in solving environmental problems. Based on the synergistic effect of Bi₂WO₆ and NH₂-MIL-88B(Fe), a Bi₂WO₆/NH₂-MIL-88B(Fe) (BNM) heterojunction photocatalyst with high-performance of photocatalytic degradation activities was successfully synthesized. The optimized BNM catalyst had a good degradation rate under visible light, which was mainly caused by generation of the active ·OH. Transient photocurrent response and electrochemical impedance tests verified that 1:2 BNM exhibits a highest charge separation and a lowest carrier recombination rate which were favorable to the photocatalytic activity. Cycle experiments show that the composite photocatalyst had good reusability and stability which were very important for potential industry applications.
اظهر المزيد [+] اقل [-]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.
اظهر المزيد [+] اقل [-]Removal of Rhodamine 6G from Aqueous Effluents by Electrocoagulation in a Batch Reactor: Assessment of Operational Parameters and Process Mechanism
2014
Zaleschi, Laura | Secula, Marius Sebastian | Teodosiu, Carmen | Stan, Corneliu Sergiu | Cretescu, Igor
The aim of the present study is to investigate the effects of operating conditions and establish the mechanism of xanthene dye removal from aqueous solutions by electrocoagulation (EC) using a batch-stirred cell operated under galvanostatic regime. The influence of the operating parameters such as: initial pH and dye concentration, electrolysis time, current density, electrode configuration, and electrical current type on the EC performances was investigated. EC tests were performed at current density values ranging from 45 to 109 A/m, initial dye concentrations ranged between 0.1 and 1 g/L, and initial pH values adjusted in the range from 3 to 9. The effects of several electrode configurations (aluminum–aluminum, mild steel–mild steel, and aluminum–mild steel) and current regimes (direct current and alternating pulsed current) on the removal efficiency and energy and material consumption are also discussed. Total organic carbon (TOC) analysis, UV–vis spectroscopy, Fourier transform infrared spectroscopy (FTIR), and cyclic voltammetry (CV) were employed in order to elucidate the decolorization mechanism of Rhodamine 6G (R6G) dye by EC in aqueous solutions. With this aim in view, chemical coagulation tests were also carried out. The best performance was obtained when the EC process was conducted with iron-based electrode configuration in alternative pulse current (APC) mode. It was found that the removal of R6G is due to the co-precipitation of polymeric iron flocs with the phenyl-xanthene radicals remained in the bulk solution after the demethylation and deamination processes. Furthermore, the flocs are separated by flotation with the support of the molecular hydrogen generated at the cathode (in particular at relatively high values of current density) or by sedimentation.
اظهر المزيد [+] اقل [-]Study of the performance of a cylindrical flow-through electro-Fenton reactor using different arrangements of carbon felt electrodes: effect of key operating parameters
2022
García-Espinoza, Josué Daniel | Robles, Irma | Durán-Moreno, Alfonso | Godínez, Luis A.
In this work, a cylindrical flow-through electro-Fenton reactor containing graphite felt electrodes and an Fe(II) loaded resin was evaluated for the production of the Fenton reaction mixture and for the degradation of amoxicillin (AMX) and fecal coliforms containing aqueous solutions. First, the influence of several factors such as treatment time, current intensity, flow rate, and electrode position was investigated for the electrogeneration of H₂O₂ and the energetic consumption by means of a factorial design methodology using a 2⁴ factorial matrix. Electric current and treatment time were found to be the pivotal parameters influencing the H₂O₂ production with contributions of 40.2 and 26.9%, respectively. The flow rate had low influence on the responses; however, 500 mL min⁻¹ (with an average residence time of 1.09 min obtained in the residence time distribution analysis) allowed to obtain a better performance due to the high mass transport to and from the electrodes. As expected, polarization was also found to play an important role, since for the cathode-to-anode flow direction, lower H₂O₂ concentrations were observed when compared with the anode-to-cathode flow arrangement, indicating that part of the H₂O₂ produced in the cathode was destroyed at the anode. A fluorescence study of hydroxyl radical production, on the other hand, showed that higher yields were obtained using an anode-to-cathode flow direction (up to 3.88 µM), when compared with experiments carried out using a cathode-to-anode flow path (3.11 µM). The removal of a commercial formulation of the antibiotic AMX was evaluated in terms of total organic carbon, achieving up to 57.9% and 38.63% of pollutant mineralization using synthetic and real sanitary wastewater spiked, respectively. Finally, the efficiency of the process on the inactivation of fecal coliforms in sanitary wastewater samples was assessed, reducing 90% of the bacteria after 5 min of electrolysis.
اظهر المزيد [+] اقل [-]