Degradation of ofloxacin using peroxymonosulfate activated by nitrogen-rich graphitized carbon microspheres: Structure and performance controllable study

Nitrogen-rich graphitized carbon microspheres (NGCs) with hierarchically porous were constructed by self-assembly. Under different heat treatment conditions, the structure, morphology and properties of NGCs were studied by using multiple characterization techniques. The results showed that the chemical microenvironments (e.g. surface chemistry, degree of graphitization and defective, etc.) and microstructures properties (e.g. morphology, specific surface area, particle size, etc.) could be delicately controlled via thermal carbonization processes. The degradation of ofloxacin (OFLX) by NGCs activated peroxymonosulfate (PMS) was studied systematically. It was found that the synergistic coupling effect between optimum N or O bonding species configuration ratio (graphitic N and C=O) and special microstructure was the main reason for the enhanced catalytic activity of NGC-800 (calcination temperature at 800°C). Electron paramagnetic resonance (EPR) experiments and radical quenching experiments indicated that the hydroxyl (^?OH), sulfate (SO₄^??) and singlet oxygen (¹O₂) were contributors in the NGC-800/PMS systems. Further investigation of the durability of chemical structures and surface active sites revealed that undergo N bonding species configuration reconstruction and cannibalistic oxidation during PMS activation reaction. The used NGC-800 physicochemical properties could be recovered by heat treatment to achieve the ideal catalytic performance. The findings proposed a valuable insight for catalytic performance and controllable design of construction.     

Comparison of light absorption and oxidative potential of biodiesel/diesel and chemicals/diesel blends soot particles

Soot particles,mainly coming from fuel combustion,affect climate forcing through absorbing light and also result in adverse human health outcomes.Though biodiesel or additives blending with diesel was considered environmentally friendly,the understanding on absorbing and oxidative capacity of soot emitted from them are still unclear.The watersoluble organic carbon(WSOC) content,surface chemical structure,light absorption and oxidative potential(OP~(DTT)) of soot from biodiesel/diesel and chemicals/diesel blends were investigated utilizing total organic carbon analyzer,X-ray photoelectron spectrometer,ultraviolet–visible spectrophotometry and dithiothreitol(DTT) assay.The differences and correlations between soot properties were statistically analyzed.Chemicals/diesel blends soot owned significantly higher WSOC content,ratio of mass absorbing efficiency(MAE) in250 and 365 nm(E_2/E_3),OP~(DTT),and higher surface carbonyl content.Coconut biodiesel/diesel blends soot contained evidently higher aromatic carbon–oxygen single bond(Ar_C–O)content,and higher MAE365.The individual comparison of biodiesel/diesel blends showed20% coconut biodiesel blend owned the lowest WSOC,E_2/E_3 and OP~(DTT),while highest Ar_C–O and MAE365,representing strongest absorbing properties.Association analysis showed OP~(DTT)was significantly positively correlated with WSOC.Further,the evident negative correlation between MAE365 and OP~(DTT) was observed.Our results showed coconut biodiesel/diesel blends soot induced lower levels of oxidative potential,whereas absorption of light was higher,which have far reaching consequences on climate forcing.Therefore,it is important to evaluate the balance point between light-absorbing properties and oxidative potential,under the wide use of biodiesel.     

Effect of lanthanum loading on nanosized CeO2-ZnO solid catalysts supported on cordierite for diesel soot oxidation

We report the application of a solid lanthanum–ceria–zinc catalyst in the catalytic regeneration of diesel particulate filters(DPF) in diesel engines.We synthesized a CeO_2–ZnO–La_2O_3(Ce–Zn–La) mixed oxide by a lactic acid-mediated sol–gel method,which efficiently coated cordierite substrates for soot capture and combustion.We studied the effects of La loading on the physicochemical and catalytic properties of Ce–Zn mixed oxide during lowtemperature soot combustion processes.We characterized the synthesized catalysts by X-ray diffraction(XRD),Fourier-transform infrared spectroscopy(FTIR),N2 adsorption,Raman spectroscopy,oxygen storage capacity(OSC),and scanning and transmission electron microscopy(SEM and TEM).Thermogravimetric and differential thermal analysis(TGA/DTA)confirmed that the catalysts effectively reduced the soot oxidation temperature.The ternary Ce–Zn–La mixed oxide catalyst with Ce/Zn/La atomic ratio of 2:1:0.5 had the highest catalytic activity and promoted soot oxidation at temperatures below 390°C.This indicated that the large number of oxygen vacancies in the catalyst structure generated oxygen species at low temperatures.Raman spectroscopy measurements revealed the presence of oxygen vacancies and lattice defects in Ce–Zn–La samples,which were key parameters concerning the stability and redox properties of the prepared catalysts.     

Mercury oxidation and adsorption characteristics of potassium permanganate modified lignite semi-coke

The adsorption characteristics of virgin and potassium permanganate modified lignite semi-coke (SC) for gaseous Hg⁰ were investigated in an attempt to produce more effective and lower price adsorbents for the control of elemental mercury emission. Brunauer-Emmett-Teller (BET) measurements, X-ray powder diffraction (XRD) and X-ray photoelectron spectroscopy (XPS) were used to analyze the surface physical and chemical properties of SC, Mn-SC and Mn-H-SC before and after mercury adsorption. The results indicated that potassium permanganate modification had significant influence on the properties of semi-coke, such as the specific surface area, pore structure and surface chemical functional groups. The mercury adsorption efficiency of modified semi-coke was lower than that of SC at low temperature, but much higher at high temperature. Amorphous Mn⁷⁺, Mn⁶⁺ and Mn⁴⁺ on the surface of Mn-SC and Mn-H-SC were the active sites for oxidation and adsorption of gaseous Hg⁰, which oxidized the elemental mercury into Hg²⁺ and captured it. Thermal treatment reduced the average oxidation degree of Mn^x+ on the surface of Mn-SC from 3.80 to 3.46. However, due to the formation of amorphous MnO_x, the surface oxidation active sites for gaseous Hg⁰ increased, which gave Mn-H-SC higher mercury adsorption efficiency than that of Mn-SC at high temperature.     

Genotoxicity removal of reclaimed water during ozonation

Genotoxicity in wastewater and reclaimed water now is gaining increased attention because of genotoxins' potential damage to the ecosystem and human health. The effect of ozonation on genotoxicity in reclaimed water was investigated. It was found that ozonation decreased the genotoxicy dramatically in three tertiary treatment plants. In the further batch ozonation experiment in laboratory,secondary effluent sample used exhibited the genotoxicity of(41.1 ± 4.1) μg 4NQO/L. Ozonation with a dose of 10 mg O3/L completely removed the genotoxicity in secondary effluent. However,after ozonation, the dissolved organic carbonvalue of the sample didn't change much but the specific ultraviolet absorbance(SUVA) value dropped sharply. With the help of Fourier transform infrared spectroscopy, ozonation was found to change chemical aliphatic carbon and C–O of the dissolved arganic matter, which might be the reason of the significant decreases of SUVA and genotoxicity.     

TOF–SIMS surface analysis of chemical components of size–fractioned urban aerosols in a typical heavy air pollution event in Beijing

Size–fractioned atmospheric aerosol particles were collected during a typical heavy air pollution event in Beijing. The organic and inorganic components on the surfaces of the samples were analyzed using time–of–flight secondary ion mass spectrometry(TOF–SIMS).The variation characteristics of the surface chemical composition and influencing factors were studied, and the possible sources of these chemical compositions were identified through principal component analysis. The results showed that inorganic components such as crustal elements and sulfate, and organic components such as aliphatic hydrocarbons and oxygen–containing organic groups were present. Some surface components, such as polycyclic aromatic hydrocarbons, heavy metals and fluorides may exert adverse effects on human health. The species and relative percentages of the chemical components varied with particle size, diurnal and pollution progress. During a heavy pollution event, the species and relative percentages of secondary components such as oxygen–containing organic groups and sulfurous compounds increased, indicating that particles aged during this event. The surface chemical composition of the aerosol particles was affected mainly by emissions from coal combustion and motor vehicles. In addition, air pollution, meteorological factors, and air mass transport also exerted a significant effect on the surface chemical composition of aerosol particles.     

Spectroscopic study on transformations of dissolved organic matter in coal-to-liquids wastewater under integrated chemical oxidation and biological treatment process

A large amount of wastewater containing various toxic organic contaminants is produced during coal-to-liquids process. In this study, several spectroscopic methods were used to monitor the transformation of organic pollutants during an integrated chemical oxidation and biological process. The results showed that the hydrophobic acid fraction increased after Fenton oxidation, which was likely due to the production of small-molecule organic acids. Soluble microbial products were generated during biological treatment processes,which were degraded after ozonation; meanwhile, the hydrophilic base and acid components increased. Ultraviolet-visible spectroscopic analysis indicated that peaks at the absorption wavelengths of 280 and 254 nm, which are associated with aromatic substances, were detected in the raw water. The aromatic substances were gradually removed, becoming undetectable after biological aeration filter(BAF) treatment. Fourier transform infrared spectroscopy analysis revealed that the functional groups of phenols;benzene, toluene, ethylbenzene, and xylene(BTEX); aromatic hydrocarbons; aliphatic acids;aldehydes; and esters were present in raw wastewater. The organic substances were oxidized into small molecules after Fenton treatment. Aromatic hydrocarbons were effectively removed through bioadsorption and biodegradation after BAF process.Biodegradable organic matter was reduced and finally became undetectable after anoxic–oxic treatment in combination with a membrane bioreactor. Four fluorescent components were fractionated and obtained via excitation–emission matrix parallel factor analysis(EEM-PARAFAC). Dissolved organic matter fractionation in conjunction with EEM-PARAFAC was able to monitor more precisely the evolution of characteristic organic contaminants.     

Trihalomethane formation potential of organic fractions in secondary effluent

Organic matter is known to be the precursor of numerous chlorination by-products. Organic matter in the secondary e uent from the Wenchang Wastewater Treatment Plant (Harbin, China) was physically separated into the following fractions: particulate organic carbon (1.2–0.45 m), colloidal organic carbon (0.45–0.1 m), fine colloidal organic carbon (0.1–0.025 m), and dissolved organic carbon (DOC) (< 0.025 m). Moreover, < 0.45 m fraction was chemically separated into hydrophobic acid (HPO-A), hydrophobic neutral (HPO-N), transphilic acid (TPI-A), transphilic neutral (TPI-N), and hydrophilic fraction (HPI). The chlorine reactivity of these organic fractions obtained from both size and XAD fractionations were evaluated. The structural and chemical compositions of the HPO-A, HPO-N, TPI-A, and TPI-N isolates were characterized using elemental analysis (C, H, O, and N), Fourier transform infrared spectroscopy (FT-IR), and proton nuclear magnetic resonance spectroscopy (1H-NMR). Results showed that DOC was dominant in terms of total concentration and trihalomethane formation potential (THMFP), and there was no statistical di erence in both specific THMFP (STHMFP) and specific ultraviolet light absorbance among the 0.45, 0.1, and 0.025 m filtrates. HPO-A had the highest STHMFP compared to other chemical fractions. HPO-A, HPO-N, TPI-A, and TPI-N contained 3.02%–3.52% of nitrogen. The molar ratio of H/C increased in the order of HPO-A < HPO-N < TPI-A < TPI-N. The O/C ratio was relatively high for TPI-N as compared to those for the other fractions. 1H-NMR analysis of the four fractions indicated that the relative content of aromatic protons in HPO-A was significantly higher than those in the others. The ratio of aliphatic to aromatic protons increased in the order of HPO-A < HPO-N < TPI-A < TPI-N. FT-IR analysis of the four fractions showed that HPO-A had greater aromatic C==C content whereas HPO-N, TPI-A, and TPI-N had greater aliphatic C–H content. TPI-N contained more oxygen-containing functional groups than the other fractions.     

Preparation of activated carbon from cattail and its application for dyes removal

Activated carbon was prepared from cattail by H3PO4 activation. The effects influencing the surface area of the resulting activated carbon followed the sequence of activated temperature activated time impregnation ratio impregnation time. The optimum condition was found at an impregnation ratio of 2.5, an impregnation time of 9 hr, an activated temperature of 500°C, and an activated time of 80 min. The Brunauer-Emmett-Teller surface area and average pore size of the activated carbon were 1279 m2/g and 5.585 nm, respectively. A heterogeneous structure in terms of both size and shape was highly developed and widely distributed on the carbon surface. Some groups containing oxygen and phosphorus were formed, and the carboxyl group was the major oxygen-containing functional group. An isotherm equilibrium study was carried out to investigate the adsorption capacity of the activated carbon. The data fit the Langmuir isotherm equation, with maximum monolayer adsorption capacities of 192.30 mg/g for Neutral Red and 196.08 mg/g for Malachite Green. Dye-exhausted carbon could be regenerated effectively by thermal treatment. The results indicated that cattail-derived activated carbon was a promising adsorbent for the removal of cationic dyes from aqueous solutions.     

CuO-modified activated carbon for the improvement of toluene removal in air

We used an impregnation method to prepare CuO/AC(activated carbon) composite materials of different CuO content and characterized them via scanning electron microscope(SEM), Brunauer–Emmett–Teller(BET), and Fourier transform infrared spectroscopy(FT-IR).The effect of CuO content on toluene adsorption/desorption was evaluated.We explored the reusability of AC and AC03(CuO modified AC with CuO loading 0.3 wt.%) adsorbents via toluene adsorption/desorption cycle testing.We used quasi-firstand quasi-second-order models, the Bangham model, and the Weber–Morris model to fit the toluene adsorption data.The introduction of CuO species evidently improved the adsorption performance of activated carbon toward toluene.The CuO content markedly affected the specific surface area, CuO dispersal, the numbers of oxygen-containing functional groups on the surface, and adsorption performance of the prepared composite adsorbents.Low CuO content was not favorable for the formation of active adsorption sites,while high content greatly reduced the specific surface area, and even covered active adsorption sites.The toluene adsorption performance varied in the order AC03 AC02 AC05 AC08 AC01(AC03, AC02, AC05, AC08 and AC01 are CuO modifying AC with CuO loading 0.3, 0.2, 0.5 0.8 and 0.1 wt.%, respectively).The breakthrough time and toluene adsorption capacity of the AC03 composite adsorbent were 94 min and 701.8 mg/g,respectively, and the recycling efficiency was 92.8% after thermal desorption at 200°C.The adsorption process was best described by the Bangham model and adsorption could be divided into three stages.     

Toxic effects of acetochlor, methamidophos and their combination on nifH gene in soil

Toxic effects of two agrochemicals on nifH gene in agricultural black soil were investigated using denaturing gradient gel electrophoresis （DGGE） and sequencing approaches in a microcosm experiment. Changes of soil nifH gene diversity and composition were examined following the application of acetochlor, methamidophos and their combination. Acetochlor reduced the nifH gene diversity （both in gene richness and diversity index values） and caused changes in the nifH gene composition. The effects of acetochlor on nifH gene were strengthened as the concentration of acetochlor increased. Cluster analysis of DGGE banding patterns showed that nifH gene composition which had been affected by low concentration of acetochlor （50 mg/kg） recovered firstly. Methamidophos reduced nifH gene richness that except at 4 weeks. The medium concentration of methamidophos （150 mg/kg） caused the most apparent changes in nifH gene diversity at the first week while the high concentration of methamidophos （250 mg/kg） produced prominent effects on nifH gene diversity in the following weeks. Cluster analysis showed that minimal changes of nifH gene composition were found at 1 week and maximal changes at 4 weeks. Toxic effects of acetochlor and methamidophos combination on nifH gene were also apparent. Different nifH genes （bands） responded differently to the impact of agrochemicals： four individual bands were eliminated by the application of the agrochemicals, five bands became predominant by the stimulation of the agrochemicals, and four bands showed strong resistance to the influence of the agrochemicals. Fifteen prominent bands were partially sequenced, yielding 15 different nifH sequences, which were used for phylogenetic reconstructions. All sequences were affiliated with the alpha- and beta-proteobacteria, showing higher similarity to eight different diazotrophic genera.     

Arsenic uptake by arbuscular mycorrhizal maize （Zea mays L.） grown in an arsenic-contaminated soil with added phosphorus

The effects of arbuscular mycorrhizal (AM) fungus (Glomus mosseae) and phosphorus (P) addition (100 mg/kg soil) on arsenic (As) uptake by maize plants (Zea mays L.) from an As-contaminated soil were examined in a glasshouse experiment.Non-mycorrhizal and zero-P addition controls were included.Plant biomass and concentrations and uptake of As,P,and other nutrients,AM colonization,root lengths,and hyphal length densities were determined.The results indicated that addition of P significantly inhibited root colonization and development of extraradical mycelium.Root length and dry weight both increased markedly with mycorrhizal colonization under the zero-P treatments,but shoot and root biomass of AM plants was depressed by P application.AM fungal inoculation decreased shoot As concentrations when no P was added,and shoot and root As concentrations of AM plants increased 2.6 and 1.4 times with P addition,respectively.Shoot and root uptake of P,Mn,Cu,and Zn increased,but shoot Fe uptake decreased by 44.6%,with inoculation, when P was added.P addition reduced shoot P,Fe,Mn,Cu,and Zn uptake of AM plants,but increased root Fe and Mn uptake of the nonmycorrhizal ones.AM colonization therefore appeared to enhance plant tolerance to As in low P soil,and have some potential for the phytostabilization of As-contaminated soil,however,P application may introduce additional environmental risk by increasing soil As mobility.     

Degradation of metabolites accumulated of benzo[a]pyrene by coupling Penicillium Chrysogenum with KMnO4

Several main metabolites of benzo[a]pyrene （BaP） formed by Penicillium chrysogenum, Benzo[a]pyrene-1,6-quinone （BP 1,6- quinone）, trans-7,8-dihydroxy-7,8-dihydrobenzo[a]pyrene （BP 7,8-diol）, 3-hydroxybenzo[a]pyrene （3-OHBP）, were identified by high-performance liquid chromatography （HPLC）. The three metabolites were liable to be accumulated and were hardly further metabolized because of their toxicity to microorganisms. However, their further degradation was essential for the complete degradation of BaP. To enhance their degradation, two methods, degradation by coupling Penicillium chrysogenum with KMnO4 and degradation only by Penicillium chrysogenum, were compared; Meanwhile, the parameters of degradation in the superior method were optimized. The results showed that （1） the method of coupling Penicillium chrysogenum with KMnO4 was better and was the first method to be used in the degradation of BaP and its metabolites; （2） the metabolite, BP 1,6-quinone was the most liable to be accumulated in pure cultures; （3） the effect of degradation was the best when the concentration of KMnO4 in the cultures was 0.01% （w/v）, concentration of the three compounds was 5 mg/L and pH was 6.2. Based on the experimental results, a novel concept with regard to the bioremediation of BaP-contaminated environment was discussed, considering the influence on environmental toxicity of the accumulated metabolites.     

Impact of atrazine and nitrogen fertilizers on the sorption of chlorotoluron in soil and model sorbents

Sorption of chlorotoluron in ammonium sulfate, urea and atrazine multi-solutes system was investigated by batch experiments. The results showed application of nitrogen fertilizers to the soil could affect the behavior of chlorotoluron. At the same concentration of N, sorption of chlorotoluron decreased as the concentration of atrazine increased on the day 0 and 6 in soil, respectively. The sorption of chlorotoluron increased from 0 to 6 d when soils were preincubated with deionized water, ammonium sulfate and urea solution for 6 d. That indicated incubation time was one of the most important factors for the sorption of chlorotoluron in nitrogen fertilizers treatments. The individual sorption isotherms of chlorotoluron in rubbery polymer and silica were strictly linear in single solute system, but there were competition sorption between pesticides or between pesticides and nitrogen fertilizers. That indicated the sorption taken place by concurrent solid-phase dissolution mechanism and sorption on the interface of water-organic matter or water-mineral matter.     

Distribution and ecological effect of mercury in Laogang landfill, Shanghai, China

Laogang landfill near Shanghai is the largest landfill in China, and receives about 10000 t of daily garbage per day, Samples of topsoil and plants were analyzed to evaluate mercury pollution from the landfill. For topsoil samples, there were significant correlations among total mercury （HgT）, combinative mercury （Hgc） and gaseous mercury （HgG）, and content of total organic carbon （TOC）, but, no significantly relationship was found between Hg content and filling time. Hg content changes in vertical profiles with time showed that the average Hgv of profiles 1992, 1996, and 2000 was similar, but their average HgG was quite different. HgT was significantly correlated with Hgc in profile 1992 and 2000, and Hgv was significantly correlated with Hg6 in profile 1996. HgG/Hgv ratio in profile samples decreased in the order of （HgG,/HgT）1992〉（HgG/HgT）1996〉〉（HgG/HgT）2000. A simple outline of Hg release in landfill could be drawn： with increasing of filling time, degradation undergoes different biodegradation, accordingly, gaseous mercury goes through small, more, and small proportion to total mercury. Distribution of Hg in plants was inhomogeneous, following the order of leaf〉root〉stem. The highest value of leaf may be associated with higher atmospheric Hg from landfill. Ligneous plants （e.g. Phyllostachys glanca, Prunus salicina and Ligustrum lucidum） are capable of enriching more Hg than herbaceous plants.     

EDTA-enhanced phytoremediation of lead contaminated soil by Bidens maximowicziana

Phytoremediation is a potential cleanup technology for the removal of heavy metals from contaminated soils.Bidens maximowicziana is a new Pb hyperaccumulator,which not only has remarkable tolerance to Pb but also extraordinary accumulation capacity for Pb.The maximum Pb concentration was 1509.3 mg/kg in roots and 2164.7 mg/kg in overground tissues.The Pb distribution order in the B. maximowicziana was:leaf>stem>root.The effect of amendments on phytoremediation was also studied.The mobility of soil Pb and the Pb concentrations in plants were both increased by EDTA application.Compared with CK(control check),EDTA application promoted translocation of Pb to overground parts of the plant.The Pb concentrations in overground parts of plants was increased from 24.23-680.56 mg/kg to 29.07-1905.57 mg/kg.This research demonstrated that B.maximowicziana appeared to be suitable for phytoremediation of Pb contaminated soil,especially,combination with EDTA.     

Potential of plant polyphenol oxidases in the decolorization and removal of textile and non-textile dyes

In this study an effort has been made to use plant polyphenol oxidases; potato （Solanum tuberosum） and brinjal （Solanum melongena）, for the treatment of various important dyes used in textile and other industries. The ammonium sulphate fractionated enzyme preparations were used to treat a number of dyes under various experimental conditions. Majority of the treated dyes were maximally decolorized at pH 3.0. Some of the dyes were quickly decolorized whereas others were marginally decolorized. The initial first hour was sufficient for the maximum decolorization of dyes. The rate of decolorization was quite slow on long treatment of dyes. Enhancement in the dye decolorization was noticed on increasing the concentration of enzymes. The complex mixtures of dyes were treated with both preparations of polyphenol oxidases in the buffers of varying pH values. Potato polyphenol oxidase was significantly more effective in decolorizing the dyes to higher extent as compared to the enzyme obtained from brinjal polyphenol oxidase. Decolorization of dyes and their mixtures, followed by the formation of an insoluble precipitate, which could be easily removed simply by centrifugation.     

Decomposition of alachlor by ozonation and its mechanism

Decomposition and corresponding mechanism of alachlor, an endocrine disruptor in water by ozonation were investigated. Results showed that alachlor could not be completely mineralized by ozone alone. Many intermediates and final products were formed during the process, including aromatic compounds, aliphatic carboxylic acids, and inorganic ions. In evoluting these products, some of them with weak polarity were qualitatively identified by GC-MS. The information of inorganic ions suggested that the dechlorination was the first and the fastest step in the ozonation of alachlor.     

Enzymatic oxidation of aqueous pentachlorophenol

The influence of the nonionic surfactant Tween 80 on pentachlorophenol （PCP） oxidation catalyzed by horseradish peroxidase was studied. The surfactant was tested at concentrations below and above its critical micelle concentration （CMC）. Enhancement of PCP removal was observed at sub-CMCs. The presence of Tween 80 in the reaction mixture reduced enzyme inactivation which occurred through a combination of free radical attack and sorption by precipitated products. A simple first-order model was able to simulate time profiles for enzyme inactivation in the presence or absence of Tween 80. At supra-CMCs, the surfactant caused noticeable reductions in PCP removal, presumably through micelle partitioning of PCP which precluded the hydrophobic PCP molecule from interacting with the enzyme.     

Removal of heavy metals from sewage sludge by low costing chemical method and recycling in agriculture

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