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1.
Bioresour Technol ; 398: 130522, 2024 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-38437965

RESUMO

The enhancement of nitrate reduction in microbial fuel cells (MFCs) by acclimating biocathode potential was studied. An MFC system was started up, and measured by cyclic voltammetry to determine a suitable potential region for acclimating biocathode. The experimental results revealed that potential acclimation could efficiently improve denitrification performance by relieving the phenomenon of nitrite accumulation, and optimum performance was obtained at -0.4 V with a total nitrogen removal efficiency of 87.4 %. Subsequently, the characteristics of electron transfer behaviors were measured, suggesting that a positive correlation between nitrate reduction and the contribution of direct electron transfer emerged. Furthermore, a denitrification mechanism was proposed. The results indicated that potential acclimation was conducive to enhancing denitrifying enzyme activity and that the electron transport system activity could be increased by 5.8 times. This study provides insight into the electron transfer characteristics and denitrification mechanisms in MFCs for nitrate reduction at specific acclimatization potentials.


Assuntos
Fontes de Energia Bioelétrica , Microbiota , Nitratos , Nitritos , Aclimatação , Nitrogênio , Desnitrificação , Eletrodos , Reatores Biológicos
2.
Environ Sci Pollut Res Int ; 31(9): 13175-13184, 2024 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-38240970

RESUMO

The crystal structure has a significant impact on the electrochemical properties of electrode material, and thus influences the electrocatalytic activity of the electrode. In this work, α-, ß-, and γ-MnO2 electrodes were fabricated and applied for investigating the effect of crystal structure on electro-oxidation treatment of N,N-dimethylacetamide (DMAC) containing wastewater. The prepared MnO2 electrodes were characterized by scanning electron microscopy and X-ray diffraction, suggesting that different crystal structures of MnO2 electrodes with the same morphology of stacking-needle structure were successfully prepared. The electrochemical performances, including removal efficiencies of DMAC, chemical oxygen demand (COD) and total nitrogen (TN), and energy consumption, were compared between different MnO2 electrodes. Results indicated that ß-MnO2 electrode presented the excellent electrochemical activity, and could remove 93% DMAC, 62% COD, and 78.9% TN, which was much higher than that of α- and γ-MnO2; moreover, energy consumptions of 11.3, 9.7, and 10.5 kWh/m3 were calculated for α-, ß-, and γ-MnO2, respectively. Additionally, the oxidation mechanism of the MnO2 electrodes was presented, indicating that DMAC was mainly oxidized by hydroxyl radical through reactions of hydroxylation, demethylation, and deamination, and electrode characteristics of specific surface area, oxygen evolution potential, and hydroxyl radical production were the key factors for degrading DMAC on MnO2 electrodes. Finally, an actual DMAC containing wastewater was applied for testing the electrochemical performance of the three electrodes, and ß-MnO2 electrode was verified as the suitable electrode for potential application which achieved removal efficiencies of 100%, 64.5%, and 73% for DMAC, COD, and TN, respectively, after system optimization.


Assuntos
Acetamidas , Óxidos , Poluentes Químicos da Água , Óxidos/química , Águas Residuárias , Compostos de Manganês/química , Radical Hidroxila , Poluentes Químicos da Água/análise , Eletrodos
3.
Environ Res ; 241: 117613, 2024 Jan 15.
Artigo em Inglês | MEDLINE | ID: mdl-37980980

RESUMO

Microbial co-culture has been proven as an effective technique for environmental remediation. In this study, co-culture mechanism of Rhodococcus ruber HJM-8 and Paracoccus communis YBH-X during N,N-dimethylacetamide (DMAC) degradation was studied. The comparison of degradation performance in monoculture and co-culture was presented; due to the efficient cooperation between the two strains via parallel and cascaded degradation, the removal efficiency of total nitrogen (TN) in co-culture could reach 90.1%, which was 1.35 and 1.21 times higher than that of HJM-8 and YBH-X, respectively. Then the communication mode of co-culture during DMAC degradation was determined as contact-independent and contact-dependent interactions between microorganisms. Meanwhile, intercellular nanotube between HJM-8 and YBH-X was found as a unique contact-dependent interaction. The cell staining experiments and RNA sequencing analyses revealed that the nanotube could be used as a bridge to exchange cytoplasmic molecules, and thus improved material transfer and enhanced cell connection in co-culture. The results of KEGG pathway showed that differentially expressed genes in co-culture have an association with cell metabolism, nanotube generation, and genetic material transfer. Furthermore, a mechanism diagram of DMAC biodegradation was proposed for co-culture, indicating that bidirectional cooperation was established between HJM-8 and YBH-X which was mediated by the conversions of acetate and nitrogen. Finally, the co-culture system was validated for treatment of an actual wastewater; results indicated that removal efficiencies of 100% and 68.2% were achieved for DMAC and TN, respectively, suggesting that co-culture had the potential for application.


Assuntos
Interações Microbianas , Nitrogênio , Técnicas de Cocultura , Comunicação
4.
Chemosphere ; 303(Pt 1): 134935, 2022 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-35561776

RESUMO

In this work, Rhodococcus ruber HJM-8 and Paracoccus communis YBH-X were isolated and used to enhance N,N-dimethylacetamide (DMAC) degradation and mineralization efficiencies. The monoculture and co-culture of the two strains for DMAC degradation were compared; results indicated that, a degradation efficiency of 97.62% was obtained in co-culture, which was much higher than that of monocultures of HJM-8 (57.34%) and YBH-X (34.02%). The degradation mechanism showed that co-culture could efficiently improve extracellular polymeric substances production, electron transfer, and microbial activity. Meanwhile, the mineralization mechanism suggested that acetate was the dominant intermediate which had an inhibitory effect on HJM-8, and co-culture was conducive to mineralization due to the high performance of acetate conversion and Na+ K+-ATPase vitality. Besides, a pathway of DMAC biodegradation was proposed for co-culture: DMAC was degraded into acetate by HJM-8, then the accumulated acetate was mineralized by YBH-X. Additionally, the co-culture system was further optimized by Box-Behnken design.


Assuntos
Rhodococcus , Acetamidas , Biodegradação Ambiental , Técnicas de Cocultura , Paracoccus , Rhodococcus/metabolismo
5.
Environ Sci Pollut Res Int ; 29(26): 39441-39450, 2022 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-35103946

RESUMO

In this work, two different types of ZnAl-layered double hydroxide (LDH) mixed metal-oxide composites (CeO2 and SnO2) were synthesized and applied for the photodegradation of 4-chlorophenol (4-CP) in wastewater. The fabricated CeO2/ZnAl-LDH and SnO2/ZnAl-LDH were characterized by X-ray diffraction (XRD), Fourier transform infrared (FTIR) spectroscopy, UV-visible diffuse reflectance spectroscopy (UV-vis DRS), and theoretical density functional theory (DFT) calculations, suggesting that the band gaps of the synthesized hybrid composites were much lower than those of traditional ZnAl-LDH. In addition, the photocatalytic activity for 4-CP degradation and reaction kinetics were investigated to evaluate the catalytic behavior of the prepared composites. The results indicated that the photocatalytic process in this case followed a pseudo-first-order kinetic model, and SnO2/ZnAl-LDH illustrated the optimum performance for 4-CP degradation with an efficiency of 95.2% due to its stability and recyclability. Additionally, the reaction mechanism of 4-CP photodegradation was studied over SnO2/ZnAl-LDH; it presented that 4-CP could be oxidized by hydroxyl radicals, holes, and superoxide radicals, where hydroxyl radicals were identified as the dominant active species during the degradation process. Finally, decomposition intermediates were measured to deduce the reaction pathway of 4-CP, and three tentative pathways were proposed and discussed.


Assuntos
Clorofenóis , Hidróxidos , Catálise , Hidróxidos/química , Óxidos
6.
Environ Sci Pollut Res Int ; 29(33): 49976-49984, 2022 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-35224693

RESUMO

Electro-oxidation is a promising technology for wastewater treatment with biorefractory organic and nitrogen pollutants; however, the high energy demand hinders its wide application. In this study, a novel method by regulating significant parameter during the electro-oxidation process in a timely manner for real dyeing wastewater treatment with energy savings was studied. Operating factors (i.e., flow rate, initial pH value, electrode distance, and current density) were investigated for chemical oxygen demand (COD) and ammonia removal, and the results indicated that current density was the key factor that obviously influenced the electrochemical performance. Indirect oxidation by active chlorine was then confirmed as the main reaction pathway for pollutant oxidation, and the relationship between the current density and the generation of active chlorine was established, suggesting that a large part of the generated active chlorine was not utilized effectively. Subsequently, a novel method of varying the current density in a timely manner based on the reaction mechanism was proposed; the results indicated that, with similar pollutant removal efficiencies, energy consumption could be reduced from 31.6 to 20.5 kWh/m3. Additionally, the novel system was further optimized by Box-Behnken design: The COD removal efficiency could reach 71.8%, and the energy demand could be reduced by 45.6%.


Assuntos
Poluentes Químicos da Água , Purificação da Água , Análise da Demanda Biológica de Oxigênio , Corantes , Eletrodos , Oxirredução , Eliminação de Resíduos Líquidos/métodos , Águas Residuárias , Purificação da Água/métodos
7.
Artigo em Inglês | MEDLINE | ID: mdl-35055672

RESUMO

In this work, an electrochemical method for chemical oxygen demand (COD) and total nitrogen (TN, including ammonia, nitrate, and nitrite) removal from wastewater using a divided electrolysis cell was developed, and its process optimization was investigated. This process could effectively relieve the common issue of NO3-/NO2- over-reduction or NH4+ over-oxidation by combining cathodic NO3-/NO2- reduction with anodic COD/NH4+ oxidation. The activity and selectivity performances toward pollutant removal of the electrode materials were investigated by electrochemical measurements and constant potential electrolysis, suggesting that Ti electrode exhibited the best NO3-/NO2- reduction and N2 production efficiencies. In-situ Fourier transform infrared spectroscopy was used to study the in-situ electrochemical information of pollutants conversion on electrode surfaces and propose their reaction pathways. The effects of main operating parameters (i.e., initial pH value, Cl- concentration, and current density) on the removal efficiencies of COD and TN were studied. Under optimal conditions, COD and TN removal efficiencies from simulated wastewater reached 92.7% and 82.0%, respectively. Additionally, reaction kinetics were investigated to describe the COD and TN removal. Results indicated that COD removal followed pseudo-first-order model; meanwhile, TN removal followed zero-order kinetics with a presence of NH4+ and then followed pseudo-first-order kinetics when NH4+ was completely removed. For actual pharmaceutical wastewater treatment, 79.1% COD and 87.0% TN were removed after 120 min electrolysis; and no NH4+ or NO2- was detected.


Assuntos
Poluentes Químicos da Água , Purificação da Água , Análise da Demanda Biológica de Oxigênio , Eletrólise , Nitrogênio/química , Oxirredução , Eliminação de Resíduos Líquidos/métodos , Águas Residuárias/química , Poluentes Químicos da Água/química
8.
Chemosphere ; 281: 130718, 2021 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-34044302

RESUMO

Multi walled carbon nanotubes (MWCNTs) have attracted more and more attention as adsorbents due to their excellent adsorption properties. By loading metal particles on MWCNTs, the chemical reduction ability of adsorbed pollutants could be provided, so as to achieve the purpose of adsorption and degradation of pollutants. Therefore, the removal process of NO3--N by Fe-Pd-Fe3O4/MWCNTs was studied, including rapid adsorption of initial pollutants, gradual reduction of intermediate products and re-adsorption of final products. The results showed that Fe-Pd-Fe3O4/MWCNTs completely removed NO3--N within 2 h, 39% and 25% of which were converted into NO2--N and NH4+-N. The adsorption efficiency, kinetics, capacity and adsorption energy all followed the order of NH4+-N > NO2--N > NO3--N. With the recoverability and reusability of Fe-Pd-Fe3O4/MWCNTs having been confirmed in 5 consecutive cycles, the removal rate of NO3--N still reached 43%. It has been shown that MWCNTs prolonged the reducing power for NO3--N, due to avoiding the aggregation of metal particles. The rapid adsorption of initial pollutants, effective stepwise reduction and convenient recovery processes were of great value for the rehabilitation of polluted water.


Assuntos
Nanotubos de Carbono , Poluentes Químicos da Água , Adsorção , Cinética , Nitratos , Óxidos de Nitrogênio , Poluentes Químicos da Água/análise
9.
Environ Sci Pollut Res Int ; 28(35): 48718-48727, 2021 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-33913111

RESUMO

Sulfur-containing wastewater is very common as an industrial waste, yet a high-efficiency composite microbial agent for sulfur-containing wastewater treatment is still lacking. In this work, three novel and efficient desulfurizing bacteria were isolated from the sewage treatment tank of Zhejiang Satellite Energy Co., Ltd. They were identified as Brucella melitensis (S1), Ochrobactrum oryzae (S8), and Achromobacter xylosoxidans (S9). These three strains of bacteria were responsible for the oxidative metabolism of sodium sulfide via a similar polythionate pathway, which could be expressed as follows: S2-→S2O32-/S0→SO32-→SO42-. Activated carbon, wheat bran, and diatomite at 1:1:1 ratio are used as carriers to construct a composite microbial agent containing the three bacteria. The desulfurization efficiency of 95% was predicted by response surface methodology under the following optimum conditions: the dosage of the inoculum was 3 g/L, pH 7.86, and temperature of 39 °C. Additionally, the impact resistance was studied in the anaerobic sequencing batch reactor. The removal capacity of microbial agent reached 98%. High-throughput analysis showed that composite microbial agent increased bacterial evenness and diversity, and the relative abundance of Brucellaceae increased from 5.04 to 8.79% in the reactor. In the process of industrial wastewater transformation, the transformation rate of sulfide by composite microbial agent was maintained between 70 and 81%. The composite microbial agent had potential for the treatment of sulfur-containing wastewater.


Assuntos
Microbiota , Esgotos , Anaerobiose , Reatores Biológicos , Biotransformação , Ochrobactrum , Sulfetos , Eliminação de Resíduos Líquidos , Águas Residuárias
10.
Bioresour Technol ; 327: 124785, 2021 May.
Artigo em Inglês | MEDLINE | ID: mdl-33582520

RESUMO

Aiming at the accumulation of NO2--N and N2O during denitrification process, this work focused to improve the denitrification performance by Pd-Fe embedded multi-walled carbon nanotubes (MWCNTs). The main conclusions were as follows: 30 mg/L Pd-Fe/MWCNTs have shown an excellent promotion on denitrification (completely TN removal at 36 h). Meanwhile, enzyme activity results indicated that the generation of NO2--N, NH4+-N by Pd-Fe/MWCNTs led the occur of short-cut denitrification by increasing 203.9% the nitrite reductase activity. Furthermore, electrochemical results and index correlation analysis confirmed that the electron exchange capacity (1.401 mmol eg-1) of Pd-Fe/MWCNTs was positively related to nitrite reductase activity, indicating its crucial role in electron transport activity (0.46 µg O2/(protein·min) at 24 h) during denitrification process by Pd-Fe/MWCNTs played a role of chemical reductant and redox mediator.


Assuntos
Alcaligenes , Nanotubos de Carbono , Desnitrificação , Transporte de Elétrons , Oxirredução
11.
Environ Sci Pollut Res Int ; 28(21): 26479-26487, 2021 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-33486682

RESUMO

5-Chloro-2-(2,4-dichlorophenoxy) phenol (triclosan, TCS) is a potential threat to the environment and human health, and it needs appropriate approaches for its removal. A new modified PbO2 electrode, Al-PbO2 based on TiO2 nanotubes (NTs), was successfully prepared for TCS electrochemical oxidation. Scanning electron microscopy indicated a compact coating layer on the anode. TCS removal on Ti/TiO2 NTs/Al-PbO2 anode followed a pseudo-first-order kinetics. The electrical efficiency per log order (EE/O) for oxidation was decreased from 14.79 to 12.90 kWh m-3 order-1 after TiO2 NTs on Ti material and decreased to 8.27 kWh m-3 order-1 after Al3+ doping. The effects of current density, pH value, and electrolyte concentration were investigated. Intermediate organo-chlorinated compounds were detected by gas chromatography coupled with mass spectrometry, high-performance liquid chromatography, and ion chromatography. Finally, ecotoxicity assessment revealed that the degradation of TCS by electrooxidation system with Ti/TiO2 NTs/Al-PbO2 anode could yield a smaller toxicity compared with parent compounds.


Assuntos
Nanotubos , Triclosan , Poluentes Químicos da Água , Eletrodos , Cromatografia Gasosa-Espectrometria de Massas , Humanos , Oxirredução , Óxidos , Titânio , Poluentes Químicos da Água/análise
12.
Sci Total Environ ; 754: 142109, 2021 Feb 01.
Artigo em Inglês | MEDLINE | ID: mdl-32898784

RESUMO

The fungus Penicillium citrinum WXP-2 and the bacterium Citrobacter freundii WXP-9 were isolated and found to have poor denitrification performance. Surprisingly, co-culture of the two strains which formed fungus-bacterium pellets (FBPs) promoted the removal efficiency of nitrate (NO3--N; 95.78%) and total nitrogen (TN; 81.73%). Nitrogen balance analysis showed that excess degraded NO3--N was primarily converted to N2 (77.53%). Moreover, co-culture increased the dry weight to 0.74 g/L. The diameter of pellets and cell viability also increased by 1.49 and 1.78 times, respectively, indicating that the co-culture exerted a synergistic effect to promote growth. The increase in electron-transmission system activity [99.01 mg iodonitrotetrazolium formazan/(g·L)] and nitrate reductase activity [8.65 mg N/(min·mg protein)] were responsible for denitrification promotion. The FBPs also exhibited the highest degradation rate at 2:1 inoculation ratio and 36 h delayed inoculation of strain WXP-9. Finally, recycling experiments of FBP demonstrated that the high steady TN removal rate could be maintained for five cycles.


Assuntos
Desnitrificação , Nitrogênio , Reatores Biológicos , Técnicas de Cocultura , Elétrons , Fungos , Nitratos
13.
Chemosphere ; 253: 126739, 2020 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-32464773

RESUMO

Biological denitrification is a promising and green technology for air pollution control. To investigate the nitric oxide reductase (NOR) that dominates NO reduction efficiency in biological purification, the heterologous prokaryotic expression system of the norB gene, which encodes the core peptide of the catalytic reduction structure in the NOR from Achromobacter denitrificans strain TB, was constructed in Escherichia coli BL21 (DE3). Results showed that the 1218 bp-long norB gene was expressed at the highest level under 1.0 mM IPTG for 5 h at 30 °C, and the relative expression abundance of norB in recombinant E. coli was increased by 16.6 times compared with that of the wild-type TB. However, the NO reduction efficiency and NOR activity of strain TB was 2.7 and 1.83 times higher than those of recombinant E. coli, respectively. On the basis of genomic reassembly and protein structure modeling, the core peptide of the NOR catalytic reduction structure from Achromobacter sp. TB can independently exert NO reduction. The low NO degradation efficiency of recombinant E. coli may be due to the lack of a NorC-like structure that increases the enzyme activity of the NorB protein. The results of this study can be used as basis for further research on the structure and function of NOR.


Assuntos
Achromobacter denitrificans/metabolismo , Oxirredutases/metabolismo , Catálise , Desnitrificação , Escherichia coli/metabolismo , Óxido Nítrico/metabolismo , Peptídeos
14.
Ecotoxicol Environ Saf ; 199: 110727, 2020 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-32446101

RESUMO

Sulfonamides (SAs) are antibiotics widely used in clinical practice, livestock and poultry production, and the aquaculture industry. The compounds enter the soil environment largely through livestock and poultry manure application to farmland. SAs not only affect plant growth, but also pose a potential threat to human health through SA residues in plant tissues. In particular, sulfamethoxazole (SMZ) has been classified as a Category 3 carcinogen by the World Health Organization, and thus its soil ecological toxicity and possible health risks are of concern. Using A. thaliana as a model plant, stress responses and biological residues of sulfadiazine (SD), sulfametoxydiazine (SMD), and SMZ were investigated in the present study. Root length and aboveground plant biomass were significantly inhibited by the three types of SA, whereas lateral roots exposed to SMD grew vigorously. The contents of chlorophyll a and chlorophyll b and photosystem II maximum photochemical quantum yield declined with increase in drug concentration, which indicated that exposure to SAs affected photosynthesis and inhibited chlorophyll synthesis in A. thaliana. With increase in drug concentration, reactive oxygen species (ROS) accumulation in the leaves increased significantly. Activities of the antioxidant enzymes superoxide dismutase (SOD) and catalase (CAT) were activated at low SA concentrations, but increased lipid peroxidation occurred with increase in SA concentration. Of the three compounds, SMZ was the most toxic to A. thaliana, followed by SD, and SMD was the least toxic. The results indicated that the risk of SMD entering an organism through the food chain is greater than that for SMZ and SD.


Assuntos
Antibacterianos/toxicidade , Arabidopsis/efeitos dos fármacos , Estresse Oxidativo/efeitos dos fármacos , Poluentes do Solo/toxicidade , Sulfanilamidas/toxicidade , Antioxidantes/metabolismo , Arabidopsis/enzimologia , Arabidopsis/crescimento & desenvolvimento , Clorofila/metabolismo , Clorofila A/metabolismo , Peroxidação de Lipídeos/efeitos dos fármacos , Fotossíntese/efeitos dos fármacos , Complexo de Proteína do Fotossistema II/metabolismo , Folhas de Planta/efeitos dos fármacos , Folhas de Planta/crescimento & desenvolvimento , Folhas de Planta/metabolismo , Raízes de Plantas/efeitos dos fármacos , Raízes de Plantas/crescimento & desenvolvimento , Raízes de Plantas/metabolismo , Espécies Reativas de Oxigênio/metabolismo
15.
Bioprocess Biosyst Eng ; 43(5): 811-820, 2020 May.
Artigo em Inglês | MEDLINE | ID: mdl-31915960

RESUMO

A novel and efficient facultative anaerobic denitrifying bacterium was isolated and identified as Pseudomonas citronellolis WXP-4. The strain WXP-4 could achieve 100% nitrate and nitrite removal efficiency utilizing sodium succinate as a carbon source, C/N ratio 7, pH 7.0, and temperature 40 °C under both aerobic and anaerobic conditions. The bacterium could tolerate a wide range of NO3--N concentrations from 100 to 1000 mg/L with a maximum nitrogen removal rate of 32.05 mg/(L h). An interesting phenomenon was found that no N2O emission occurred during the denitrifying process under anaerobic conditions, while there was 0.06 mg/L under aerobic conditions. This phenomenon had been confirmed by fluorescence quantitative PCR and the results showed that the relative abundance of nosZ gene increased by 17-fold based on the ratio of anaerobic to aerobic, and thus, nosZ gene could encode more nitrous oxide reductase to accelerate the conversion of N2O under anaerobic conditions. Moreover, the narG, nirK, and norB genes were also identified in the denitrifying pathway of the strain WXP-4. This investigation has demonstrated enormous potential for the future application in wastewater treatment systems.


Assuntos
Proteínas de Bactérias/metabolismo , Desnitrificação , Nitratos/metabolismo , Óxido Nitroso/metabolismo , Pseudomonas/metabolismo , Aerobiose , Anaerobiose , Proteínas de Bactérias/genética , Pseudomonas/genética , Pseudomonas/isolamento & purificação
16.
Environ Sci Pollut Res Int ; 26(36): 36933-36941, 2019 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-31745767

RESUMO

Conversion of FeII(EDTA)-NO or FeIII(EDTA) into FeII(EDTA) is a key process in a wet flue gas denitrification technology with FeII(EDTA) solution. In this work, the stoichiometry, kinetics, and thermodynamics of FeII(EDTA)-NO reduction by Mn powder were investigated. We first studied the FeII(EDTA)-NO reduction and product distribution to speculate a possible stoichiometry of FeII(EDTA)-NO reduction by Mn powder. Then, the effects of major influencing factors, such as pH value, temperature, and Mn concentration, were studied. The pseudo-second-order model was established to describe the FeII(EDTA)-NO reduction. Simultaneously, according to Arrhenius and Eyring-Polanyi equations, the reaction activation energy (Ea), enthalpy of activation (∆H‡), and entropy of activation (∆S‡) were calculated as 23.68 kJ/mol, 21.148 kJ/mol, and - 149.728 J/(k mol), respectively. Additionally, simultaneous reduction of FeIII(EDTA) and FeII(EDTA)-NO was investigated to better study the mechanism of FeII(EDTA) regeneration, suggesting that there was a competition between the two reduction processes. Finally, a simple schematic mechanism of NO absorption by FeII(EDTA) combined with regeneration of manganese ion and ammonium was proposed. These fundamental researches could offer a valuable guidance for wet flue gas denitrification technology with FeII(EDTA) solution.


Assuntos
Desnitrificação , Ácido Edético/metabolismo , Cinética , Manganês , Compostos Férricos , Compostos Ferrosos , Ferro , Modelos Químicos , Oxirredução , Pós , Temperatura , Termodinâmica
17.
Artigo em Inglês | MEDLINE | ID: mdl-31443230

RESUMO

To mitigate the potential environmental risks caused by nitrogen compounds from industrial wastewater, residual ammonia after conventional wastewater treatment should be further eliminated. In this work, an electrochemical oxidation process for converting ammonia to nitrogen in actual dyeing wastewater was investigated. The effects of the main operating parameters, including initial pH value, applied current density, NaCl concentration, and flow, were investigated on ammonia removal and products distribution. Experimental results indicated that, under optimal conditions of an initial pH value of 8.3, applied current density of 20 mA cm-2, NaCl concentration of 1.0 g L-1, and flow of 300 mL min-1, the ammonia could be completely removed with N2 selectivity of 88.3% in 60 min electrolysis. A kinetics investigation using a pseudo-first-order model provided a precise description of ammonia removal during the electro-oxidation process. Experimental functions for describing the relationships between kinetic constants of ammonia removal and main operating parameters were also discussed. Additionally, the mechanisms and economic evaluation of ammonia oxidation were conducted. All these results clearly proved that this electro-oxidation process could efficiently remove ammonia and achieve high N2 selectivity.


Assuntos
Amônia/química , Corantes/química , Eletrólise/métodos , Nitrogênio/química , Eliminação de Resíduos Líquidos/métodos , Águas Residuárias/química , Poluentes Químicos da Água/química , Oxirredução
18.
Sci Total Environ ; 687: 198-205, 2019 Oct 15.
Artigo em Inglês | MEDLINE | ID: mdl-31207510

RESUMO

Paired electrolysis can take advantage of both anodic oxidation and cathodic reduction, and thus improve current efficiency for electrochemical wastewater treatment. In this work, differential control of anode/cathode potentials of paired electrolysis for simultaneous removal of chemical oxygen demand (COD) and total nitrogen (TN, including ammonia, nitrate, and nitrite) was studied. We first determined the optimal potentials for anodic oxidation of COD/NH4+ or cathodic reduction of NO3-/NO2- (minimization of over-oxidation or over-reduction) by preliminary cyclic voltammetry and constant-potential electrolysis experiments, i.e., 1.6 V for anodic oxidation and -1.26 V for cathodic reduction in this case. The optimal working potential of the cathode was achieved at appropriate current density in the paired electrolysis system, the working potential of the anode was independently controlled by adjusting the ratio of its surface area to that of the cathode. In this way, both the cathode and anode could work under optimal potentials. At an optimized cathodic current density of 5.0 mA cm-2 and cathode/anode surface area ratio of 2:1, the removal efficiencies of COD and TN from simulated wastewater reached 91.9% and 86.2%, respectively. Additionally, the developed paired electrolysis system was validated by treating an actual pharmaceutical wastewater, results for which showed that a total current efficiency of 84.8% was achieved, which was at least twice as high as that of traditional electrochemical processes.

19.
Environ Sci Pollut Res Int ; 23(18): 18288-95, 2016 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-27278066

RESUMO

Effluents after biochemical treatment contain pollutants that are mostly non-degradable. Based upon previous pilot-scale test results, an industrial-scale electro-oxidation device was built to decompose these refractory materials in the effluent from a park wastewater treatment plant. The electro-oxidation device comprised a ditch-shaped plunger flow electrolysis cell, with mesh-plate Ti/PbO2 electrodes as the anode and the same size mesh-plate Ti as the cathode. Wastewater flowed vertically through electrodes; the effective volume of the cell was 2.8 m(3), and the surface-to-volume ratio was 17.14 m(2) m(-3). The optimal current density was 100 A m(-2), and a suitable flow velocity was 14.0 m h(-1). The removal efficiencies for chemical oxygen demand and color in the effluent were over 60.0 and 84.0 %, respectively. In addition, the electro-oxidation system offered a good disinfection capability. The specific energy consumption for this industrial-scale device was 43.5 kWh kg COD(-1), with a current efficiency of 32.8 %, which was superior to the pilot-scale one. To meet the requirements for emission or reuse, the operation cost was $0.44 per ton of effluent at an average price for electricity of $0.11 kWh(-1).


Assuntos
Eletroquímica/métodos , Eliminação de Resíduos Líquidos/métodos , Águas Residuárias/química , Poluentes Químicos da Água/análise , Análise da Demanda Biológica de Oxigênio , Eletroquímica/instrumentação , Eletrodos , Eletrólise , Oxirredução , Eliminação de Resíduos Líquidos/instrumentação
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