首页 | 本学科首页   官方微博 | 高级检索  
相似文献
 共查询到19条相似文献,搜索用时 62 毫秒
1.
Iron oxide(FeO)coated by natural organic matter(NOM)is ubiquitous.The associations of minerals with organic matter(OM)significantly changes their surface properties and reactivity,and thus affect the environmental fate of pollutants,including nutrients(e.g.,phosphorus(P)).In this study,ferrihydrite/goethite-humic acid(FH/GE–HA)complexes were prepared and their adsorption characteristics on P at various p H and ionic strength were investigated.The results indicated that the Fe O–OM complexes showed a decreased P adsorption capacity in comparison with bare Fe O.The maximum adsorption capacity(Q_(max))decreased in the order of FH(22.17 mg/g)FH-HA(5.43 mg/g)GE(4.67 mg/g)GE-HA(3.27 mg/g).After coating with HA,the amorphous FH–HA complex still showed higher P adsorption than the crystalline GE–HA complex.The decreased P adsorption observed might be attributed to changes of the Fe O surface charges caused by OM association.The dependence of P adsorption on the specific surface area of adsorbents suggests that the Fe O component in the complexes is still the main contributor for the adsorption surfaces.The P adsorptions on Fe O–HA complexes decreased with increasing initial p H or decreasing initial ionic strength.A strong dependence of P adsorption on ionic strength and p H may demonstrate that outer-sphere complexes between the OM component on the surface and P possibly coexist with inner-sphere surface complexes between the Fe O component and P.Therefore,previous over-emphasis on the contributions of original minerals to P immobilization possibly over-estimates the P loading capacity of soils,especially in humic-rich areas.  相似文献   

2.
Competitive and cooperative adsorption of arsenate and citrate on goethite   总被引:1,自引:1,他引:0  
The fate of arsenic in natural environments is influenced by adsorption onto metal (hydr)oxides. The extent of arsenic adsorption is strongly a ected by coexisting dissolved natural organic acids. Recently, some studies reported that there existed competitive adsorption between arsenate and citrate on goethite. Humic acid is known to interact strongly with arsenate by forming complexes in aqueous solution, hence it is necessary to undertake a comprehensive study of the adsorption of arsenate/citrate onto goethite in the presence of one another. The results showed that at the arsenate concentrations used in this study (0.006–0.27 mmol/L), citrate decreased arsenate adsorption at acidic pH but no e ect was observed at alkaline pH. In comparison, citrate adsorption was inhibited at acidic pH, but enhanced at alkaline pH by arsenate. This was probably due to the formation of complex between arsenate and citrate like the case of arsenate with humic acid. These results implied that the mechanism of the adsorption of arsenate and citrate onto goethite in the presence of one another involved not only competition for binding sites, but the cooperation between the two species at the watergoethite interface as well.  相似文献   

3.
In order to study the influences of functionalized groups onto the adsorption of tetracycline,we prepared a series of amino and amino–Fe~(3+)complex mesoporous silica adsorbents with diverse content of amino and Fe~(3+)groups(named N,N-SBA15 and Fe-N,N-SBA15).The resulting mesoporous silica adsorbents were fully characterized by X-ray powder diffraction(XRD),Fourier transform infrared spectrometer(FTIR)and N_2adsorption/desorption isotherms.Furthermore,the effects of functionalized groups on the removal of TC were investigated.The results showed that the periodic ordered structure of SBA-15 was maintained after modification of amino/Fe~(3+)groups.The functionalized amino groups decreased the adsorption capacity while the coordinated Fe~(3+)increased the adsorption capacity.The adsorption kinetics of TC fitted pseudo-second-order model well and the equilibrium was achieved quickly.The adsorption isotherms fitted the Langmuir model well and with the Fe~(3+)content increased from 3.93%to 8.26%,the Q_(max)of the adsorbents increased from 102 to 188 mmol/kg.The solution p H affected the adsorption of TC onto amino complex adsorbents slightly while influenced the adsorption onto Fe-amine complex adsorbents greatly.The adsorption of TC on SBA15 and N,N-SBA15 may be related to the formation of outer-sphere surface complexes,while the adsorption of TC onto Fe-N,N-SBA15 was mainly attributed to the inner-sphere surface complexes.This study could offer potential materials that have excellent adsorption behavior for environmental remediation and suggested useful information for the preparing other adsorbents in environmental applications.  相似文献   

4.
The adsorption of phosphorus(P) onto three industrial solid wastes(fly ash, red mud and ferric–alum water treatment residual(FAR)) and their modified materials was studied systematically via batch experiments. Compared with two natural adsorbents(zeolite and diatomite), three solid wastes possessed a higher adsorption capacity for P because of the higher Fe, Al and Ca contents. After modification(i.e., the fly ash and red mud modified by FeCl_3 and FARs modified by HCl), the adsorption capacity increased, especially for the modified red mud, where more Fe bonded P was observed. The P adsorption kinetics can be satisfactorily fitted using the pseudo-second-order model. The Langmuir model can describe well the P adsorption on all of the samples in our study. p H and dissolved organic matter(DOM) are two important factors for P adsorption. Under neutral conditions, the maximum adsorption amount on the modified materials was observed. With the deviation from pH 7, the adsorption amount decreased, which resulted from the change of P species in water and surface charges of the adsorbents. The DOM in water can promote P adsorption, which may be due to the promotion effects of humic-Fe(Al) complexes and the pH buffer function exceeds the depression of competitive adsorption.  相似文献   

5.
The massive production and wide use of surfactants have resulted in a large amount of surfactant residuals being discharged into the environment,which could have an impact on arsenic behavior.In the present study,the influence of the anionic surfactant sodium dodecyl benzene sulfonate(SDBS) and nonionic surfactant polyethylene glycol octylphenyl ether(Triton X-100) on arsenic behavior was investigated in batch and column tests.The presence of SDBS and Triton X-100 reduced arsenic retention onto ferrihydrite(FH),enhanced arsenic transport through FH coated sand(FH-sand) columns and promoted arsenic release from the FH surface.With coexisting surfactants in solution,the equilibrium adsorbed amount of arsenic on FH decreased by up to 29.7% and the adsorption rate decreased by up to 52.3%.Pre-coating with surfactants caused a decrease in the adsorbed amount and adsorption rate of arsenic by up to 15.1% and 58.3%,respectively.Because of the adsorption attenuation caused by surfactants,breakthrough of As(Ⅴ) and As(Ⅲ) with SDBS in columns packed with FH-sand was 23.8% and 14.3%faster than that in those without SDBS,respectively.In columns packed with SDBS-coated FH-sand,transport of arsenic was enhanced to a greater extent.Breakthrough of As(Ⅴ) and As(Ⅲ) was 52.4% and 43.8% faster and the cumulative retention amount was 44.5% and 57.3% less than that in pure FH-sand column systems,respectively.Mobilization of arsenic by surfactants increased with the increase of the initial adsorbed amount of arsenic.The cumulative release amount of As(Ⅴ) and As(Ⅲ) from the packed column reached 10.8% and 36.0%,respectively.  相似文献   

6.
Asymmetric flow-field flow fractionation-inductively-coupled plasma-mass spectrometry was used to determine whether colloidal arsenic(As) exists in soil pore water and soil extract samples at two arsenic-contaminated abandoned gold mines(Montague and Goldenville, Nova Scotia). Colloidal arsenic was found in 12 out of the 80 collected samples(= 15%), and was primarily associated with iron(Fe) in the encountered colloids. The molar Fe/As ratios indicate that the colloids in some samples appeared to be discrete iron–arsenic minerals, whereas in other samples, they were more consistent with As-rich iron(oxy)hydroxides. Up to three discrete size fractions of colloidal As were encountered in the samples, with mean colloid diameters between 6 and 14 nm. The pore water samples only contained one size fraction of As-bearing colloids(around 6 nm diameter), while larger As-bearing colloids were only encountered in soil extracts.  相似文献   

7.
The adsorption behavior of p-aminobenzoic acid and o-aminobenzoic acid onto the different polymeric adsorbents was systematically investigated as a function of the solution concentration and temperature.Experimental results indicated that the equilibrium adsorption data of the four polymeric adsorbents fitted well in the Freundlich isotherm.The adsorption capacity of multi-functional polymeric adsorbent NJ-99 was the highest,which might be attributed to the strong hydrogen-bonding interaction between the amino groups on the resin and the carboxyl group of aminobenzoic acid.The adsorption capacity of o-aminobenzoic acid onto any adsorbent was higher than p-aminobenzoic acid.Thermodynamic studies suggested the exothermic,spontaneous physical adsorption process.Adsorption kinetics results showed that the adsorption followed the pseudo-second-order kinetics model and the intraparticle mass transfer process was the rate-controlling step.  相似文献   

8.
The effects of four conditioning approaches:Acid,Acid-zero-valent iron(ZVI)/peroxydisulfate(PMS),Fe(Ⅱ)/PMS and ZVI/PMS,on wastewater activated sludge(WAS) dewatering and organics distribution in supernatant and extracellular polymeric substances(EPS) layers were investigated.The highest reduction in bound water and the most WAS destruction was achieved by Acid-ZVI/PMS,and the optimum conditions were pH 3,ZVI dosage 0.15 g/g dry solid(DS),oxone dosage 0.07 g/g DS and reaction time 10.6 min with the reductions in capillary suction time(CST) and water content(Wc) as 19.67% and 8.49%,respectively.Four conditioning approaches could result in TOC increase in EPS layers and supernatant,and protein(PN) content in tightly bound EPS(TB-EPS).After conditioning,organics in EPS layers could migrate to supernatant.Polysaccharide(PS) was easier to migrate to supernatant than PN.In addition,Acid,Acid-ZVI/PMS or Fe(Ⅱ)/PMS conditioning promoted the release of some polysaccharides containing ring vibrations v P=O,v C-O-C,v C-O-P functional groups from TB-EPS.ESR spectra proved that both radicals of SO_4~-· and·OH contributed to dewatering and organics transformation and migration.CST value of WAS positively correlated with the ratios of PN/PS in LB-EPS and total EPS,while it negatively correlated with TOC,PN content and PS content in TB-EPS,as well as PS content in supernatant and LB-EPS.BWC negatively correlated to zeta potential and TOC value,PN content,and HA content in supernatant.  相似文献   

9.
The effects of amphiphilic O/W emulsions,stabilized by the alkyl polyglycoside(APG)or cholesterol-grafted sodium alginate(CSAD)/APG systems,on lambda-cyhalothrin adsorption/desorption mechanisms on natural soil minerals(i.e.,illite and kaolinite)were investigated.Sorption and desorption of lambda-cyhalothrin onto soil minerals was studied via batch equilibration to give insight into the adsorption equilibrium,kinetics,and thermodynamics of lambda-cyhalothrin adsorption onto minerals.The results indicate the following:(i)The adsorption processes for the APG system and CSAD/APG system include:rapid adsorption,slow adsorption,and adsorption equilibrium.The adsorption kinetics of pesticide on illite and kaolinite are in accordance with the Ho and McKay model,and the adsorption isotherm conforms to the Freundlich model.In addition,the adsorption processes of pesticide for the two systems on minerals were spontaneous and feasible(ΔG~00),endothermic(ΔH~00),and mainly involved chemical bonding(ΔH~060).(ii)The equilibrium adsorption percentages of the pesticide on illite for the APG system and CSAD/APG system were 42.4%and 64.8%,and the corresponding equilibrium adsorption percentages on kaolinite were 40.8%and 61.8%,respectively.Moreover,the pesticide adsorption rate K_(2-CSAD/APG)was faster than K_(2-APG),and its adsorption capacity K_(f-CSAD/APG )was greater than K_(f-APG).Meanwhile,the pesticide desorption K_(fd)in the CSAD/APG system was smaller than that in the APG system.As a result,this eco-friendly O/W emulsion based on amphiphilic sodium alginate derivatives might provide a green pesticide formulation,since it could reduce the amount of lambda-cyhalothrin entering aquatic systems to threaten non-target fish and invertebrate species.  相似文献   

10.
A novel adsorbent based on iron oxide dispersed over activated carbon(AC) were prepared, and used for phosphate removal from aqueous solutions. The influence of pre-oxidation treatment on the physical, chemical and phosphate adsorption properties of iron-containing AC were determined. Two series of ACs, non-oxidized and oxidized carbon modified by iron(denoted as AC-Fe and AC/OFe), resulted in a maximum impregnated iron of 4.03% and 7.56%, respectively. AC/O-Fe showed 34.0%–46.6% higher phosphate removal efficiency than the AC-Fe did. This was first attributed to the moderate pre-oxidation of raw AC by nitric acid, achieved by dosing Fe(II) after a pre-oxidation, to obtain higher iron loading, which is favorable for phosphate adsorption. Additionally, the in-situ formed active site on the surface of carbon, which was derived from the oxidation of Fe(II) by nitric acid dominated the remarkably high efficiency with respect to the removal of phosphate. The activation energy for adsorption was calculated to be 10.53 and 18.88 kJ/mol for AC-Fe and AC/OFe, respectively. The results showed that the surface mass transfer and intra-particle diffusion were simultaneously occurring during the process and contribute to the adsorption mechanism.  相似文献   

11.
A series of Pt–V/Ce–Zr–O diesel oxidation catalysts was prepared using the impregnation method. The catalytic activity and sulfur resistance of Pt–V/Ce–Zr–O were investigated in the presence of simulated diesel exhaust. The effect of vanadium on the structure and redox properties of the catalysts was also investigated using the Brunauer–Emmett–Teller method,X-ray diffraction, H2temperature-programmed reduction, CO temperature-programmed desorption, X-ray photoelectron spectroscopy, and Energy Dispersive Spectroscopy. Results showed that the Pt particles were well dispersed on the Ce–Zr–O carrier through the vanadium isolation effect, which significantly improved the oxidation activity toward CO and hydrocarbons. An electron-withdrawing phenomenon occurred from V to Pt, resulting in an increase in the metallic nature of platinum, which was beneficial to hydrocarbon molecular activation.  相似文献   

12.
Hexabromocyclododecanes(HBCDs),a new type of persistent organic pollutants widely used as brominated flame retardants,have attracted wide attention due to their increasing level and toxicity. A method based on high-performance liquid chromatography mass spectrometry(HPLC–MS–MS)in electrospray ionization mode has been developed by optimization of various parameters,which effectively improved the separation degree and responsive intensity of α-,β-and γ-HBCD isomers. The concentrations and distribution profiles of three HBCD isomers were investigated in sediments from the Haihe River in China.It was observed that the concentrations of HBCDs varied in the range of 0.4–58.82 ng/g,showing a decreasing trend along the flow direction,possibly due to attenuation and biodegradation along the flow direction of the Haihe River. The distribution profile of α-,β-,γ-HBCD was 7.91%–88.6%,0–91.47%,and 0.62%–42.83%,respectively. Interestingly,α-HBCD dominated in most sample sites. This was different from the distribution profile in commercial industrial products,which might be attributed to the inter-transformation and different degradation rates of the three HBCD isomers. The potential ecological risk of HBCDs in sediment was characterized under the two-tiered procedure of the European Medicines Evaluation Agency for environmental risk assessment. Although the HBCDs in the selected section of the Haihe River presented "no risk" in the sediment compartment,its risk in sediment cannot be neglected since sediment is one of the important sinks and reservoirs of pollutants.  相似文献   

13.
Cu–Mn, Cu–Mn–Ce, and Cu–Ce mixed-oxide catalysts were prepared by a citric acid sol–gel method and then characterized by XRD, BET, H2-TPR and XPS analyses. Their catalytic properties were investigated in the toluene combustion reaction. Results showed that the Cu–Mn–Ce ternary mixed-oxide catalyst with 1:2:4 mole ratios had the highest catalytic activity, and 99% toluene conversion was achieved at temperatures below 220°C. In the Cu–Mn–Ce catalyst, a portion of Cu and Mn species entered into the CeO2 fluorite lattice, which led to the formation of a ceria-based solid solution. Excess Cu and Mn oxides existed on the surface of the ceria-based solid solution. The coexistence of Cu–Mn mixed oxides and the ceria-based solid solution resulted in a better synergetic interaction than the Cu–Mn and Cu–Ce catalysts, which promoted catalyst reducibility, increased oxygen mobility, and enhanced the formation of abundant active oxygen species.  相似文献   

14.
Currently, the Chinese central government is considering plans to build a trilateral economic sphere in the Bohai Bay area, including Beijing, Tianjin and Hebei(BTH), where haze pollution frequently occurs. To achieve sustainable development, it is necessary to understand the physical mechanism of the haze pollution there. Therefore, the pollutant transport mechanisms of a haze event over the BTH region from 23 to 24 September 2011 were studied using the Weather Research and Forecasting model and the FLEXible-PARTicle dispersion model to understand the effects of the local atmospheric circulations and atmospheric boundary layer structure. Results suggested that the penetration by sea-breeze could strengthen the vertical dispersion by lifting up the planetary boundary layer height(PBLH) and carry the local pollutants to the downstream areas; in the early night, two elevated pollution layers(EPLs) may be generated over the mountain areas: the pollutants in the upper EPL at the altitude of 2–2.5 km were favored to disperse by long-range transport, while the lower EPL at the altitude of 1 km may serve as a reservoir, and the pollutants there could be transported downward and contribute to the surface air pollution.The intensity of the sea–land and mountain–valley breeze circulations played an important role in the vertical transport and distribution of pollutants. It was also found that the diurnal evolution of the PBLH is important for the vertical dispersion of the pollutants,which is strongly affected by the local atmospheric circulations and the distribution of urban areas.  相似文献   

15.
Fertilizer input for agricultural food production, as well as domestic and industrial surface water pollutants in the North China Plain, increases pressures on locally scarce and vulnerable water resources. In order to: (a) understand pollutant exchange between surface water and groundwater, (b) quantify nutrient loadings, and (c) identify major nutrient removal pathways by using qualitative and quantitative methods, including the geochemical model PHREEQC, a one-year study at a wheat (Triticum aestivum L.) and maize (Zea mays L.) double cropping system in the Baiyang Lake area in Hebei Province, China, was undertaken. The study showed a high influence of low-quality surface water on the shallow aquifer. Major inflowing pollutants into the aquifer were ammonium and nitrate via inflow from the adjacent Fu River (up to 29.8 mg/L NH4-N and 6.8 mg/L NO3-N), as well as nitrate via vertical transport from the field surface (up to 134.8 mg/L NO3-N in soil water). Results from a conceptual model show an excess nitrogen input of about 320 kg/ha/a. Nevertheless, both nitrogen species were only detected at low concentrations in shallow groundwater, averaging at 3.6 mg/L NH4-N and 1.8 mg/L NO3-N. Measurement results supported by PHREEQC-modeling indicated cation exchange, denitrification, and anaerobic ammonium oxidation coupled with partial denitrification as major nitrogen removal pathways. Despite this current removal capacity, the excessive nitrogen fertilization may pose a future threat to groundwater quality. Surface water quality improvements are therefore recommended in conjunction with simultaneous monitoring of nitrate in the aquifer, and reduced agricultural N-inputs should be considered.  相似文献   

16.
In 2013,China issued "Air Pollution Prevention and Control Action Plan(Action Plan)" to improve air quality.To assess the benefits of this program in Beijing-Tianjin-Hebei(BTH)region,where the density of population and emissions vary greatly,we simulated the air quality benefit based on Ben MAP to satisfy the Action Plan.In this study,we estimate PM_(2.5) concentration using Voronoi spatial interpolation method on a grid with a spatial resolution of 1 × 1 km~2.Combined with the exposure-response function between PM_(2.5) concentration and health endpoints,health effects of PM_(2.5) exposure are analyzed.The economic loss is assessed by using the willingness to pay(WTP) method and human capital(HC) method.When the PM_(2.5) concentration falls by 25% in BTH and reached 60 μg/m~3 in Beijing,the avoiding deaths will be in the range of 3175 to 14051 based on different functions each year.Of the estimated mortality attributable to all causes,3117 annual deaths were due to lung cancer,1924 – 6318 annual deaths were due to cardiovascular,and343 – 1697 annual deaths were due to respiratory.Based on WTP,the estimated monetary values for the avoided cases of all cause mortality,cardiovascular mortality,respiratory mortality and lung cancer ranged from 1110 to 29632,673 to 13325,120 to 3579,1091 to 6574 million yuan,respectively.Based on HC,the corresponding values for the avoided cases of these four mortalities were 267 to 1178,161 to 529,29 to 143 and 261 million yuan,respectively.  相似文献   

17.
The methylene blue(MB)removal abilities of raw activated carbon and iron/cerium modified raw activated carbon(Fe–Ce-AC)by adsorption were researched and compared.The characteristics of Fe–Ce-AC were examined by N_2adsorption,zeta potential measurement,FTIR,Raman,XRD,XPS,SEM and EDS.After modification,the following phenomena occurred:The BET surface area,average pore diameter and total pore volume decreased;the degree of graphitization also decreased.Moreover,the presence of Fe_3O_4led to Fe–Ce-AC having magnetic properties,which makes it easy to separate from dye wastewater in an external magnetic field and subsequently recycle.In addition,the equilibrium isotherms and kinetics of MB adsorption on raw activated carbon and Fe–Ce-AC were systematically examined.The equilibrium adsorption data indicated that the adsorption behavior followed the Langmuir isotherm,and the pseudo-second-order model matched the kinetic data well.Compared with raw activated carbon,the maximum monolayer adsorption capacity of Fe–Ce-AC increased by27.31%.According to the experimental results,Fe–Ce-AC can be used as an effective adsorbent for the removal of MB from dye wastewater.  相似文献   

18.
We investigated the role of glutathione(GSH) and phytochelatins(PCs) on the detoxification of selenite using Arabidopsis thaliana. The wild-type(WT) of Arabidopsis thaliana and its mutants(glutathione deficient Cad 2–1 and phytochelatins deficient Cad 1–3) were separately exposed to varying concentrations of selenite and arsenate and jointly to both toxicants to determine their sensitivities. The results of the study revealed that, the mutants were about 20-fold more sensitive to arsenate than the WT, an indication that the GSH and PCs affect arsenate detoxification. On the contrary, the WT and both mutants showed a similar level of sensitivity to selenite, an indication that the GSH and PCs do not significantly affect selenite detoxification. However, the WT is about 8 times more sensitive to selenite than to arsenate, and the mutants were more resistant to selenite than arsenate by a factor of 2. This could not be explained by the accumulation of both elements in roots and shoots in exposure experiments. The co-exposure of the WT indicates a synergistic effect with regards to toxicity since selenite did not induce PCs but arsenic and selenium compete in their PC binding as revealed by speciation analysis of the root extracts using HPLC–ICP–MS/ESI–MS. In the absence of PCs an antagonistic effect has been detected which might suggest indirectly that the formation of Se glutathione complex prevent the formation of detrimental selenopeptides. This study, therefore, revealed that PC and GSH have only a subordinate role in the detoxification of selenite.  相似文献   

19.
Organic matters (OMs) and their oxidization products often influence the fate and transport of heavy metals in the subsurface aqueous systems through interaction with the mineral surfaces. This study investigates the ethanol (EtOH)-mediated As(III) adsorption onto Zn-loaded pinecone (PC) biochar through batch experiments conducted under Box–Behnken design. The effect of EtOH on As(III) adsorption mechanism was quantitatively elucidated by fitting the experimental data using artificial neural network and quadratic modeling approaches. The quadratic model could describe the limiting nature of EtOH and pH on As(III) adsorption, whereas neural network revealed the stronger influence of EtOH (64.5%) followed by pH (20.75%) and As(III) concentration (14.75%) on the adsorption phenomena. Besides, the interaction among process variables indicated that EtOH enhances As(III) adsorption over a pH range of 2 to 7, possibly due to facilitation of ligand–metal(Zn) binding complexation mechanism. Eventually, hybrid response surface model–genetic algorithm (RSM–GA) approach predicted a better optimal solution than RSM, i.e., the adsorptive removal of As(III) (10.47 μg/g) is facilitated at 30.22 mg C/L of EtOH with initial As(III) concentration of 196.77 μg/L at pH 5.8. The implication of this investigation might help in understanding the application of biochar for removal of various As(III) species in the presence of OM.  相似文献   

设为首页 | 免责声明 | 关于勤云 | 加入收藏

Copyright©北京勤云科技发展有限公司  京ICP备09084417号