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1.
J Chromatogr A ; 1635: 461704, 2021 Jan 04.
Article in English | MEDLINE | ID: mdl-33223152

ABSTRACT

In this study, porous covalent organic frameworks (COFs, named as COFs-SWMU) were synthesized for the first time via a facile approach by using 4,4',4''-methylidynetri-anilin and 2,5-dihydroxy-1,4-benzenedicarboxaldehyde as precursors under ambient temperature. The COFs-SWMU were characterized by scanning electron microscopy, Fourier-transform infrared spectroscopy, X-ray diffraction and X-ray photoelectron spectroscopy, thermogravimetric analysis, etc. The COFs-SWMU exhibited a relatively high specific surface area and desirable thermal stability. The adsorption performance of COFs-SWMU towards fluoronitrobenzenes (FNBs, including 1-fluoro-2-nitrobenzene, 1-fluoro-3-nitrobenzene, 1-fluoro-4-nitrobenzene, 2,4-difluoronitrobenzene, 3,4-difluoronitrobenzene, and 3,4-dinitrofluorobenzene) was investigated on the basis of adsorption capacity and partition coefficient (PC). The adsorption kinetics and isotherm of COFs-SWMU for FNBs were studied in detail. Further, a simple, fast and sensitive method which combined COFs-SWMU based extraction with high-performance liquid chromatography-diode array detection, was proposed for the analysis of FNBs in environmental samples. Desirable linearity (R2>0.9998) in the range of 0.1-100 µg•mL-1, low limits of detection (LODs; 0.1‒0.15 µg•mL‒1), low limits of quantitation (LOQs; 0.28‒0.40 µg•mL‒1), and desirable precision (RSDs, 0.24-2.83% for intraday and 1.13-6.92% for interday) are obtained. Finally, the COFs-SWMU were applied to the effective extraction of FNBs from environmental samples, and desirable recovery results were obtained.


Subject(s)
Chromatography, High Pressure Liquid , Environmental Monitoring/methods , Metal-Organic Frameworks/chemical synthesis , Nitrobenzenes/isolation & purification , Solid Phase Extraction , Adsorption , Limit of Detection , Metal-Organic Frameworks/ultrastructure , Spectroscopy, Fourier Transform Infrared , X-Ray Diffraction
2.
Chemosphere ; 247: 125832, 2020 May.
Article in English | MEDLINE | ID: mdl-31931312

ABSTRACT

Anaerobic reduction of nitrobenzene (NB) can be efficiently enhanced bySupplementing withSulfide-modified nanoscale zerovalent iron (S-nZVI). In thisStudy,S/Fe ratio ofS-nZVI was further optimized for enhancing biological NB removal in anaerobicSystem amended withS-nZVI and inoculated by anaerobicSludge. The results indicated that the performance andStability of the coupled anaerobicSystem for NB reduction and aniline formation were remarkably improved byS-nZVI atS/Fe molar ratio of 0.3 (0.3S-nZVI). TheSecretion of extracellular polymericSubstances (EPS), transformation of volatile fatty acids (VFAs), yield of methane and activity ofSeveral key enzymes could be efficiently improved by 0.3S-nZVI. Furthermore,Species related to NB reduction, fermentation, electroactivity and methanogenesis could be enriched in 0.3S-nZVI coupled anaerobicSystem, with remarkable improvement in the biodiversity observed. ThisStudy demonstrated thatSulfidation would be a promising method to improve the performance of nZVI in coupled anaerobicSystems for the removal of recalcitrant nitroaromatic compounds from wastewater.


Subject(s)
Iron/analysis , Nitrobenzenes/isolation & purification , Sulfides/analysis , Water Pollutants, Chemical/metabolism , Anaerobiosis , Extracellular Polymeric Substance Matrix/metabolism , Iron/pharmacology , Methane/biosynthesis , Methane/metabolism , Nitrobenzenes/metabolism , Sulfides/pharmacology , Wastewater/chemistry , Water Pollutants, Chemical/analysis
3.
Environ Int ; 131: 105020, 2019 10.
Article in English | MEDLINE | ID: mdl-31325713

ABSTRACT

Nanoscale zero-valent iron (nZVI), although being increasingly used in anaerobic systems for strengthening the removal of various refractory pollutants, is limited by various inherent drawbacks, such as easy precipitation, passivation, poor mass and electron transfer. To address the above issues, biochar stabilized sulfide-modified nZVI (S-nZVI@BC) was added into an up-flow anaerobic sludge blanket (UASB) to investigate the enhancement of anaerobic biodegradation of nitrobenzene (NB) and its impacts on microbial community structure. The results demonstrated that both NB reduction and aniline formation could be substantially facilitated in S-nZVI@BC coupled system compared to other anaerobic ones coupled with nZVI or S-nZVI. The dosage of S-nZVI@BC resulted in the formation of densely packed aggregates, evidently increased the extracellular polymeric substances content, promoted the volatile fatty acids transformation and stimulated the methane yield. Furthermore, species related to fermentation (Bacteroides and Longilinea), methanogenesis (Methanosarcina and Methanomethylovorans), electroactivity (Pelobacter, Thiobacillus and Phaselicystis) as well as reduction (Desulfovibrio) were considerably enriched in S-nZVI@BC coupled system. The activities of electron transport, total adenosine triphosphate, nitroreductase and NAD(P)H, which were closely related to microbial activity and NB transformation, were increased noticeably in S-nZVI@BC coupled anaerobic system. This study demonstrated the promising potential for long-term operation and full-scale application of S-nZVI@BC coupled system for the treatment of NB containing wastewater.


Subject(s)
Biodegradation, Environmental , Charcoal , Environmental Microbiology , Iron/chemistry , Metal Nanoparticles/chemistry , Nitrobenzenes/isolation & purification , Sulfides/chemistry , Anaerobiosis , Methane , Nitrobenzenes/chemistry , Sewage/chemistry , Wastewater , Water Pollutants, Chemical/analysis
4.
J Chromatogr A ; 1597: 54-62, 2019 Jul 19.
Article in English | MEDLINE | ID: mdl-30929864

ABSTRACT

Silicon nanowire (SiNW) arrays are demonstrated as a suitable platform for the preconcentration of trace nitroaromatic compounds and subsequent desorption via Joule heating of the array. Arrays are fabricated from Si wafers containing an epitaxially grown layer of low conductivity intrinsic Si sandwiched between layers of high conductivity p-type Si. Passage of current through the nanowires results in nanowire temperatures in excess of 200 °C during heating of the arrays as verified by using the temperature-dependent shift of the Si Raman band at ˜520 cm-1. Analyte vapor preconcentration and partial separation is achieved on the array at analyte concentrations nearly two orders-of-magnitude below saturated vapor concentrations at room temperature. The effects of desorption carrier gas flow rate and temperature on the ability to preconcentrate and resolve the analytes of interest are determined. 2,6-dinitrotoluene (2,6-DNT) and 2,4-dinitrotoluene (2,4-DNT) were detected at nominal vapor concentrations of 800 pptv with a 1 min sample time (1.1 ng nominal mass load) and trinitrotoluene (TNT) was detected at a nominal vapor concentration of 65 pptv with a 10 min sample time (1.1 ng nominal mass load).


Subject(s)
Chemistry Techniques, Analytical/methods , Explosive Agents/isolation & purification , Nanowires/chemistry , Nitrobenzenes/isolation & purification , Electric Conductivity , Gases/chemistry , Gases/isolation & purification , Silicon/chemistry , Temperature
5.
Chemosphere ; 223: 375-382, 2019 May.
Article in English | MEDLINE | ID: mdl-30784744

ABSTRACT

The reactivity and delivery of remediants and treatment of organic contaminants in heterogeneous aquifer are particularly challenging issues for injection-based remedial treatments. Our objective was to enhance the reactivity and delivery of nanoscale zero-valent iron (nZVI) and improve the sweeping efficiency of nZVI into low permeable zones (LPZs) to reduce nitrobenzene (NB). This was accomplished by conducting batch and transport experiments that quantified NB degradation by different modified nZVI and the ability of emulsified nZVI (EZVI) or xanthan carried EZVI (XG-EZVI) to penetrate and cover a lens. By incorporating the xanthan and emulsified oil with nZVI, it possessed higher stability and stronger reactivity to reduce NB. Results showed that the stability of EZVI was improved by xanthan, and there were no adverse effects on NB removal in use of XG-EZVI at limited xanthan addition of ≦100 mg L-1. By the injection of XG-EZVI in 2D-tank experiments, the degradation of NB was 8 times that of EZVI added, while NB adsorption on media was only 1/50 of initial NB. 1205 mg of NB totally entered into the tank, the quality of aniline in effluent was approximately 90.0 mg in addition of XG-EZVI at 40 h, but not detected in presence of EZVI. The greater NB reduction by XG-EZVI resulted from higher sweeping efficiency in LPZ. These observations support the couple use of xanthan and emulsified oil for modifying nZVI as a means of achieving greater stability and reactivity and enhancing nZVI delivery into LPZs for the treatment of NB.


Subject(s)
Environmental Restoration and Remediation/methods , Groundwater/chemistry , Iron/chemistry , Nitrobenzenes/isolation & purification , Polysaccharides, Bacterial/chemistry , Emulsions/chemistry , Reducing Agents , Water Pollutants, Chemical/isolation & purification
6.
Environ Sci Pollut Res Int ; 25(27): 27112-27121, 2018 Sep.
Article in English | MEDLINE | ID: mdl-30022388

ABSTRACT

To investigate the activity of iron carbonate precipitates produced by long-term operation of Fe0 permeable reactive barriers, three kinds of precipitates, namely Fe6(OH)12CO3, Fe2(OH)2CO3, and FeCO3, were prepared to reduce the pollutant nitrobenzene. We studied the reduction effects of these iron carbonate precipitates on nitrobenzene by considering three factors, namely the initial nitrobenzene concentration, initial pH, and precipitate dosage, and established the kinetic degradation using pseudo-first-order kinetics model. The results showed that all three precipitates can reduce nitrobenzene, and the order of reducing capability is Fe6(OH)12CO3 > Fe2(OH)2CO3 > FeCO3; moreover, the removal efficiency values of nitrobenzene are 68.08, 53.00, and 50.29%. A high initial nitrobenzene concentration and high pH value are beneficial to nitrobenzene reduction, and removal efficiency was increased when pH was increased from 4 to 9. In addition, the increased precipitate addition in the Fe6(OH)12CO3 and Fe2(OH)2CO3 systems increased removal efficiency. Furthermore, the dosage did not significantly influence the removal rate in the FeCO3 system. Fe6(OH)12CO3 and Fe2(OH)2CO3 mainly relied on the precipitate itself with the structural Fe(II) to reduce nitrobenzene, and FeCO3 mainly relied on the dissolved Fe2+. The reaction of all three precipitates in reducing nitrobenzene followed the first-order reaction kinetics.


Subject(s)
Carbonates/chemistry , Iron/chemistry , Nitrobenzenes/chemistry , Carbonates/chemical synthesis , Chemical Precipitation , Ferric Compounds/chemical synthesis , Kinetics , Nitrobenzenes/isolation & purification , Oxidation-Reduction , Water Pollutants, Chemical/isolation & purification
7.
J Environ Manage ; 223: 771-778, 2018 Oct 01.
Article in English | MEDLINE | ID: mdl-29986324

ABSTRACT

Nitrobenzene (NB) is a kind of persistent organic pollutant. A ubiquitous and cost-effective substance spent black tea (SBT) was investigated for the removal of nitrobenzene from aqueous media. The maximum uptake potential of dried biomass (SBT) for NB was found to be 14.86 mg per gram (qmax) in a batch experimental set-up. Equilibration time for NB sorption was about 50 min, and optimal removal efficiency was achieved at a dosage of 2 g/L with an initial concentration of 100 mg/L of NB. Findings revealed that NB uptake increased with an increase in the temperature from 273 K to 353 K. Sorption was also found to be pH sensitive, sorption improved as the pH value changes from alkaline to acidic (from 10 to 2). Different isotherm (Langmuir, Freundlich, Temkin and Dubinin Radushkevich) and kinetic models (pseudo-1st order, pseudo-2nd order and Elovich models) were applied to experimental results; the sorption mechanism was well described by the Freundlich and pseudo-2nd order models. Moreover, Scanning electron micrographs, ATR-FTIR spectra and the results of elemental analysis also supported the efficacy of SBT as an efficient bio-sorbent for the elimination of NB from water.


Subject(s)
Nitrobenzenes/isolation & purification , Tea , Water Pollutants, Chemical/isolation & purification , Adsorption , Hydrogen-Ion Concentration , Kinetics , Nitrobenzenes/chemistry , Thermodynamics , Water , Water Pollutants, Chemical/chemistry
8.
Environ Sci Pollut Res Int ; 25(8): 7916-7923, 2018 Mar.
Article in English | MEDLINE | ID: mdl-29299866

ABSTRACT

Three polystyrene (PS) resin microspheres supported nanoscale zero-valent iron (nZVI), i.e., nZVI@PS, nZVI@PS-Cl, and nZVI@PS-N, were prepared and characterized by FT-IR, XPS, SEM, EDS, and weighing method. The functional groups on the carriers showed obvious influence on the loading quantity, the micro morphology, and the reduction efficiency of these supported nZVI. The best hybrid reducer was nZVI@PS-N. The load quantity of nZVI was 0.2476 g/g, and some of them were dispersed and the others remained as particles (≤ 50 nm). At optimal reaction conditions, i.e., initial solution pH = 3, 25 °C, 100 r/min stirring, 99% nitrobenzene (NB) in 250 mL 123.1 mg/L NB solution could be totally reduced into AN by 1.31 g fresh nZVI@PS-N within 20 min. The excellent reduction efficiency and fast degradation rate of nZVI@PS-N were mainly attributed to the synergistic effects between the good adsorption property of its carrier and the high reduction activity of nZVI particles. NZVI@PS-N was reproducible and recycled, and 90.6% degradation ratio of NB was till obtained at its seventh recycle. The results showed that nZVI@PS-N had high potential practical application value in the reductive degradation and emergency rescue of nitrobenzene pollutant.


Subject(s)
Iron/chemistry , Microspheres , Nitrobenzenes/chemistry , Polystyrenes/chemistry , Water Pollutants, Chemical/chemistry , Adsorption , Hydrogen-Ion Concentration , Nitrobenzenes/isolation & purification , Recycling , Temperature , Water Pollutants, Chemical/isolation & purification
9.
J Chromatogr A ; 1529: 107-112, 2017 Dec 22.
Article in English | MEDLINE | ID: mdl-29132825

ABSTRACT

Typical trace vapor analysis involves sorbent trapping, followed by desorption and chromatographic separation. This communication describes a method for streamlining this process by combining sorbent sampling/preconcentration with partial separation achieved through temperature-programmed thermal desorption. A novel sorbent trap was formulated in which tubular glass liners for a programmable-temperature gas chromatograph inlet were coated with a sol-gel based polymer stationary phase synthesized from methyltrimethoxysilane precursor and installed into the inlet, which was directly connected to a mass-selective detector by a fused silica capillary transfer line. This method is shown to achieve partial separation of two nitroaromatic vapors in a total 3-5min analysis time, which represents a tenfold improvement in speed in terms of the overall cycle time compared to an analogous conventional vapor analysis method. Both analytes proved to have a high dynamic range and loading capacity, with nitrobenzene achieving both high and low sampling extremes (0.32ng-4µg sampling concentration) with only a slight compromise in peak broadening. The multivariate curve resolution by alternating least squares algorithm (MCR-ALS) was shown to successfully resolve the overlapped elution profiles of the two nitroaromatic test vapors examined in this study.


Subject(s)
Chemistry Techniques, Analytical/methods , Gases/isolation & purification , Silanes/chemistry , Chromatography, Gas , Gases/chemistry , Gels/chemistry , Nitrobenzenes/chemistry , Nitrobenzenes/isolation & purification , Polymers/chemistry , Silicon Dioxide/chemistry , Temperature
10.
Metabolism ; 70: 107-115, 2017 05.
Article in English | MEDLINE | ID: mdl-28403934

ABSTRACT

OBJECTIVE: The extracts of Nitraria genus are composed of Nitraria alkaloids and have been used traditionally as a hypoglycemic medicine. However, the efficacy and precise mechanism of Nitraria alkaloids remain largely unknown. METHODS: Previously, we reported the total synthesis of (+)-isonitramine, one of Nitraria alkaloids. In this study, we investigated the anti-diabetic potential of isonitramine in diabetes mellitus and its underlying molecular mechanism in carbohydrate catabolism in vitro and in vivo. RESULTS: Isonitramine exerted significant inhibitory effect on α-glucosidases but not α-amylase in vitro. In zebrafish, isonitramine alleviated the streptozotocin (STZ)-induced postprandial hyperglycemia and protected the pancreatic damages against alloxan-induced oxidative stress in vivo. Also, isonitramine induced insulin without any toxicities and downregulated phosphoenolpyruvate carboxykinase (PEPCK), which catalyzes the first committed step in gluconeogenesis. CONCLUSION: Taken together, isonitramine inhibited α-glucosidase activity and PEPCK expression, while increased insulin expression, resulting in attenuating the postprandial hyperglycemia. Also, isonitramine protected the pancreas from ROS-mediated toxicities. Therefore, isonitramine may be a new drug candidate for the treatment of diabetes mellitus.


Subject(s)
Alkaloids/pharmacology , Aniline Compounds/pharmacology , Hyperglycemia/drug therapy , Insulin-Secreting Cells/drug effects , Nitrobenzenes/pharmacology , Alkaloids/isolation & purification , Aniline Compounds/isolation & purification , Animals , Carbohydrate Metabolism/drug effects , Cell Line , Cricetinae , Glycoside Hydrolase Inhibitors , Humans , Hypoglycemic Agents/isolation & purification , Hypoglycemic Agents/pharmacology , Nitrobenzenes/isolation & purification , Phosphoenolpyruvate Carboxykinase (ATP)/drug effects , Plant Extracts/chemistry , Protective Agents/isolation & purification , Protective Agents/pharmacology , Rats , Swine , Zebrafish
11.
Analyst ; 141(7): 2303-7, 2016 Apr 07.
Article in English | MEDLINE | ID: mdl-26887641

ABSTRACT

Halonitrobenzenes (HNBs) are a class of molecules that are highly toxic to human health and the ecological environment. Thus, effective and efficient approaches capable of monitoring and detecting HNBs are greatly desired. We report herein a simple and sensitive method for the detection of HNBs. The detection was based on the indium tin oxide (ITO) electrodes modified with a binary assembly of highly ordered surfactant micelles (OSMs) and silica mesochannels (SMs). The SMs have a diameter of 2-3 nm and a vertical orientation, which provide a hard support to stabilize soft OSMs. Moreover, each OSM consists of a hydrophobic core due to the organized assembly of surfactant hydrocarbon chains, which can selectively extract and concentrate lipophilic HNBs from aqueous media, allow their transport to the underlying ITO electrode surface and therein their detection by voltammetry. As a proof-of-concept experiment, 1-chloro-3-nitrobenzene, 1-chloro-4-nitrobenzene, 1-bromo-4-nitrobenzene and 2,4-dinitrobromobenzene were analyzed in aqueous solutions. A simple and fast detection was achieved in all cases, with a wide linear dynamic range, a high sensitivity and a low limit of detection at the ppb level. Apart from the extraction ability, the OSMs also prohibited the access of and surface contamination by unwanted substances, showing excellent anti-fouling and anti-interference power. Indeed, as we demonstrated, the sensor could be employed for direct electrochemical detection of HNBs in complex samples, such as lake water and soil dispersion, without any pre-treatment, indicating its potential usefulness in practical analysis.


Subject(s)
Chemical Fractionation/methods , Limit of Detection , Micelles , Nitrobenzenes/analysis , Nitrobenzenes/isolation & purification , Surface-Active Agents/chemistry , Environmental Pollutants/analysis , Environmental Pollutants/chemistry , Environmental Pollutants/isolation & purification , Nitrobenzenes/chemistry
12.
Environ Sci Pollut Res Int ; 23(10): 9972-83, 2016 May.
Article in English | MEDLINE | ID: mdl-26865481

ABSTRACT

A laboratory-scale bio-permeable reactive barrier (bio-PRB) was constructed and combined with enclosed in-well aeration system to treat nitrobenzene (NB) and aniline (AN) in groundwater. Batch-style experiments were first conducted to evaluate the effectiveness of NB and AN degradation, using suspension (free cells) of degrading consortium and immobilized consortium by a mixture of perlite and peat. The NB and AN were completely degraded in <3 days using immobilized consortium, while 3-5 days were required using free cells. The O2 supply efficiency of an enclosed in-well aeration system was assessed in a box filled with perlite and peat. Dissolved O2 (DO) concentrations increased to 8-12 mg L(-1) in 12 h for sampling ports within 12 cm of the aeration well. A diffusion coefficient as 33.5 cm(2) s(-1) was obtained. The DO concentration was >4 mg L(-1) when the aeration system was applied into the bio-PRB system. The NB and AN were effectively removed when the aeration system was functional in the bio-PRB. The removal efficiency decreased when the aeration system malfunctioned for 20 days, thus indicating that DO was an important factor for the degradation of NB and AN. The regain of NB and AN removal after the malfunction indicates the robustness of degradation consortium. No original organics and new formed by-products were observed in the effluent. The results indicate that NB and AN in groundwater can be completely mineralized in a bio-PRB equipped with enclosed in-well aeration system and filled with perlite and peat attached with degrading consortium.


Subject(s)
Aniline Compounds/isolation & purification , Groundwater/analysis , Nitrobenzenes/isolation & purification , Water Pollutants, Chemical/isolation & purification , Water Purification/instrumentation , Aerobiosis , Biodegradation, Environmental , Microbial Consortia , Oxygen/analysis , Soil Microbiology , Water Purification/methods
13.
Water Sci Technol ; 73(1): 153-60, 2016.
Article in English | MEDLINE | ID: mdl-26744946

ABSTRACT

The efficiency of Fenton-like catalysis using nano zerovalent iron (nZVI) is limited by nZVI aggregation and activity loss due to inactive ferric oxide forming on the nZVI surface, which hinders electron transfer. A novel iron-carbon composite catalyst consisting of nZVI and granular activated carbon (GAC), which can undergo internal iron-carbon microelectrolysis spontaneously, was successfully fabricated by the adsorption-reduction method. The catalyst efficiency was evaluated in nitrobenzene (NB) removal via the Fenton-like process (H2O2-nZVI/GAC). The results showed that nZVI/GAC composite was good for dispersing nZVI on the surface of GAC, which permitted much better removal efficiency (93.0%) than nZVI (31.0%) or GAC (20.0%) alone. Moreover, iron leaching decreased from 1.28 to 0.58 mg/L after reaction of 240 min and the oxidation kinetic of the Fenton-like reaction can be described well by the second-order reaction kinetic model (R2=0.988). The composite catalyst showed sustainable catalytic ability and GAC performed as a medium for electron transfer in internal iron-carbon microelectrolysis to promote Fe2+ regeneration and Fe3+/Fe2+ cycles. Therefore, this study represents an important method to design a low cost and high efficiency Fenton-like catalyst in practical application.


Subject(s)
Charcoal/chemistry , Hydrogen Peroxide/chemistry , Iron/chemistry , Nitrobenzenes/isolation & purification , Water Pollutants, Chemical/isolation & purification , Adsorption , Catalysis , Ferric Compounds , Kinetics , Oxidation-Reduction
14.
PLoS One ; 10(8): e0132878, 2015.
Article in English | MEDLINE | ID: mdl-26266532

ABSTRACT

The combination of surfactant enhanced soil washing and degradation of nitrobenzene (NB) in effluent with persulfate was investigated to remediate NB contaminated soil. Aqueous solution of sodium dodecylbenzenesulfonate (SDBS, 24.0 mmol L-1) was used at a given mass ratio of solution to soil (20:1) to extract NB contaminated soil (47.3 mg kg-1), resulting in NB desorption removal efficient of 76.8%. The washing effluent was treated in Fe2+/persulfate and Fe2+/H2O2 systems successively. The degradation removal of NB was 97.9%, being much higher than that of SDBS (51.6%) with addition of 40.0 mmol L-1 Fe2+ and 40.0 mmol L-1 persulfate after 15 min reaction. The preferential degradation was related to the lone pair electron of generated SO4•-, which preferably removes electrons from aromatic parts of NB over long alkyl chains of SDBS through hydrogen abstraction reactions. No preferential degradation was observed in •OH based oxidation because of its hydrogen abstraction or addition mechanism. The sustained SDBS could be reused for washing the contaminated soil. The combination of the effective surfactant-enhanced washing and the preferential degradation of NB with Fe2+/persulfate provide a useful option to remediate NB contaminated soil.


Subject(s)
Electrons , Nitrobenzenes/isolation & purification , Sodium Compounds/chemistry , Soil Pollutants/isolation & purification , Soil/chemistry , Sulfates/chemistry , Surface-Active Agents/chemistry , Benzenesulfonates/chemistry , Environmental Restoration and Remediation/methods , Humans , Hydrogen/chemistry , Nitrobenzenes/chemistry , Oxidation-Reduction , Soil Pollutants/chemistry
15.
Bioresour Technol ; 189: 23-29, 2015.
Article in English | MEDLINE | ID: mdl-25864027

ABSTRACT

A novel thermophilic bioelectrochemical system (TBES) based on electrical stimulation was established for the enhanced treatment of p-fluoronitrobenzene (p-FNB) wastewater. p-FNB removal rate constant in the TBES was 78.6% higher than that of the mesophilic BES (MBES), the elevation of which owing to high-temperature overtook the rate improvement of 50.8% in the electrocatalytic system (ECS). Additionally, an overwhelming mineralization efficiency of 91.96% ± 5.70% was obtained in the TBES. The superiority of TBES was attributed to the integrated role of electrical stimulation and high-temperature. Electrical stimulation provided an alternative for the microbial growth independent energy requirements, compensating insufficient energy support from p-FNB metabolism under the high-temperature stress. Besides, electrical stimulation facilitated microbial community evolution to form specific thermophilic biocatalysis. The uniquely selected thermophilic microorganisms including Coprothermobacter sp. and other ones cooperated to enhance p-FNB mineralization.


Subject(s)
Bacteria/metabolism , Nitrobenzenes/metabolism , Temperature , Adenosine Triphosphatases/metabolism , Bacteria/enzymology , Biocatalysis , Biodegradation, Environmental , Electric Stimulation , Electrochemical Techniques , Fluorides/analysis , Halogenation , Minerals/chemistry , Nitrobenzenes/isolation & purification , Oxidoreductases/metabolism
16.
Environ Technol ; 36(13-16): 1847-54, 2015.
Article in English | MEDLINE | ID: mdl-25650667

ABSTRACT

4-Chloronitrobenzene (4-CNB) is one of the highly toxic contaminants that may lead to acute, chronic or persistent physiological toxicity to ecology and environment. Conventional methods for removing 4-CNB from aquatic environment may be problematic due to inefficiency, high cost and low sustainability. This study develops a pilot-scale bioelectrochemical system (BES, effective volume of 18 L) and examines its performance of bioelectrochemical transformation of 4-CNB to 4-chloroaniline (4-CAN) under continuous operation. The results demonstrate that the initial 4-CNB concentration in the influent and hydraulic retention time (HRT) has a significant impact on 4-CNB reduction and 4-CAN formation. Compared with the conventional anaerobic process in the absence of external power supplied, the 4-CNB conversion efficiency can be enhanced with power supplied due to microbial-mediated electron transfer at the negative cathode potential. At a voltage of 0.4 V and HRT of 48 h, the 4-CNB reduction and 4-CAN formation efficiency reached 99% and 94.1%, respectively. Based on a small external voltage applied, the pilot-scale BES is effective in the conversion of 4-CNB to 4-CAN, an intermediate that is of less toxicity and higher bioavailability for subsequent treatment. This study provides a new strategy and methods for eliminating 4-CNB, making wastewater treatment more economical and more sustainable.


Subject(s)
Bioelectric Energy Sources/microbiology , Electrochemistry/instrumentation , Nitrobenzenes/isolation & purification , Nitrobenzenes/metabolism , Water Pollutants, Chemical/isolation & purification , Water Purification/instrumentation , Bioreactors/microbiology , Electrochemistry/methods , Electrodes , Electrolysis/instrumentation , Electrolysis/methods , Energy Transfer , Equipment Design , Equipment Failure Analysis , Pilot Projects , Water Pollutants, Chemical/metabolism , Water Purification/methods
17.
J Sep Sci ; 38(3): 368-73, 2015 Feb.
Article in English | MEDLINE | ID: mdl-25402743

ABSTRACT

A novel on-site sampling and sample-preparation approach was developed and evaluated in the present work. In this procedure, hollow-fiber/graphene bars (HF/GBs) were used for sampling and sample preparation. A handheld battery-operated electric egg beater was utilized to support the HF/GBs and stir the sample solution to facilitate extraction at the sampling site. Four nitrobenzene compounds (nitrobenzene, o-nitrophenol, m-nitrophenol, and p-nitrophenol) were used as model compounds. Several factors affecting performance, including types and amount of graphene used and extraction and desorption times, were investigated and optimized in the laboratory. Under optimized conditions, the enrichment factors of the four nitrobenzene compounds ranged from 46 to 69. Good linearities of 0.01-10 µg/mL with regression coefficients between 0.9917 and 0.9973 were obtained for all analytes. The LOD of the method was 0.3 ng/mL. Satisfactory recoveries (98-102%) and precision (1.0-5.8%) were also achieved. The ultrastructures and extraction mechanism of the HF/GBs were characterized and analyzed. The proposed approach coupled with high-performance liquid chromatography was successfully applied in the extraction and determination of trace nitrobenzene compounds in lake water. Experimental results showed that the approach is simple, convenient, rapid, and practical for routine environmental monitoring.


Subject(s)
Graphite/chemistry , Lakes/chemistry , Liquid Phase Microextraction , Nitrobenzenes/isolation & purification , Water Pollutants, Chemical/isolation & purification , Chromatography, High Pressure Liquid , Nitrobenzenes/chemistry , Particle Size , Porosity , Surface Properties , Water Pollutants, Chemical/chemistry
18.
Bioresour Technol ; 172: 104-111, 2014 Nov.
Article in English | MEDLINE | ID: mdl-25247250

ABSTRACT

p-Fluoronitrobenzene (p-FNB) is a toxic compound and tends to accumulate in the environment. p-FNB can be effectively removed and defluorinated in a single-chamber bioelectrochemical system (BES). To verify the suppositionally integrated reductive and oxidative metabolism mechanism in the BES, an oxygen-limited environment was used, with pure oxygen and nitrogen environments used as two controls. Under the oxygen-limited condition, the most excellent performance was achieved. The defluorination rate and mineralization efficiency were 0.0132h(-1) and 72.99±5.68% after 96h, with 75.4% of fluorine in the form of the fluoride ion. This resulted from the unique environment that allowed conventionally integrated reductive and oxidative catabolism. Moreover, the oxidation-reduction potential (ORP) had a significant effect on microbial communities, which was also an important reason for performance diversity. These results provide a new method for complete p-FNB treatment and a control strategy by ORP regulation for optimal system performance.


Subject(s)
Bioelectric Energy Sources , Minerals/chemistry , Nitrobenzenes/chemistry , Oxygen/pharmacology , Bacteria/drug effects , Bacteria/growth & development , Biodegradation, Environmental/drug effects , Bioelectric Energy Sources/microbiology , Carbon/isolation & purification , Catalysis/drug effects , Denaturing Gradient Gel Electrophoresis , Electrochemical Techniques , Electrodes , Halogenation/drug effects , Nitrobenzenes/isolation & purification , Oxidation-Reduction/drug effects
19.
J Hazard Mater ; 280: 450-7, 2014 Sep 15.
Article in English | MEDLINE | ID: mdl-25194813

ABSTRACT

Biochars' performance as the sorbent to pollutants is dependent on their compositions and surface characteristics, which are then related to the feedstock used for biochar preparation. The objective of this work is to probe the feedstock's influence on biochar's sorption property through a comparative study on biochars from lignin, cellulose and wood prepared at 400°C and 600°C, respectively. Elemental and spectral analyses demonstrated that the wood biochar had a composition and carbonization degree close to the cellulose biochar but much different from the lignin biochar prepared at the same temperature, suggesting that lignin is not dominant to properties of plant-derived biochars. The lignin biochar showed a sorption capacity comparable to both cellulose and wood biochars as the sorbent to nitrobenzene, with a higher partition contribution to the total sorption due to the lower carbonization of lignin. In general, the lignin biochar is a good candidate of sorbent to aromatic pollutants, and is advantageous over the other two species with its efficient carbon utilization.


Subject(s)
Charcoal/chemistry , Lignin/chemistry , Nitrobenzenes/isolation & purification , Water Pollutants, Chemical/isolation & purification , Wood/chemistry , Adsorption , Surface Properties
20.
Biosens Bioelectron ; 53: 250-6, 2014 Mar 15.
Article in English | MEDLINE | ID: mdl-24144555

ABSTRACT

Two-dimensional ordered mesoporous carbon nitride (OMCN) has been successfully prepared for the first time using SBA-15 mesoporous silica and melamine as template and precursor respectively, by a nano hard-templating approach. A series of OMCN-x samples with different pyrolysis temperatures have been reported. The formation of these composite materials was verified by detailed characterization (e.g., Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, N2 adsorption, X-ray diffraction, scanning electron microscopy, and transmission electron microscopy). The results showed that the materials were structurally well ordered with two-dimensional porous structure, high surface area and large pore volume. The influence of BET surface area and different amounts of N-bonding configurations formed at different pyrolysis temperatures of OMCN-x for the electrocatalysis towards hydrogen peroxide, nitrobenzene, and nicotinamide adenine dinucleotide were investigated in detail. Results indicated that OMCN treated at 800°C with largest BET surface area and highest amounts of pyrindinic N showed improved electrocatalytic activity for H2O2, nitrobenzene, and NADH in neutral solution.


Subject(s)
Biosensing Techniques/methods , Hydrogen Peroxide/isolation & purification , NAD/isolation & purification , Nitrobenzenes/isolation & purification , Nitriles/chemistry , Porosity , Silicon Dioxide/chemistry , Surface Properties , X-Ray Diffraction
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