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1.
Effect of environmental factors on the complexation of iron and humic acid   总被引:1,自引:0,他引:1  
A method of size exclusion chromatography coupled with ultraviolet spectrophotometry and off-line graphite furnace atomic absorption spectrometry was developed to assess the complexation properties of iron(Fe) and humic acid(HA) in a water environment. The factors affecting the complexation of Fe and HA, such as ionic strength, p H, temperature and UV radiation, were investigated. The Fe–HA complex residence time was also studied. Experimental results showed that p H could influence the deprotonation of HA and hydrolysis of Fe, and thus affected the complexation of Fe and HA. The complexation was greatly disrupted by the presence of Na Cl. Temperature had some influence on the complexation. The yield of Fe–HA complexes showed a small decrease at high levels of UV radiation, but the effect of UV radiation on Fe–HA complex formation at natural levels could be neglected. It took about 10 hr for the complexation to reach equilibrium, and the Fe–HA complex residence time was about 20 hr.Complexation of Fe and HA reached a maximum level under the conditions of p H 6, very low ionic strength, in the dark and at a water temperature of about 25°C, for 10 hr. It was suggested that the Fe–HA complex could form mainly in freshwater bodies and reach high levels in the warm season with mild sunlight radiation. With changing environmental parameters, such as at lower temperature in winter or higher p H and ionic strength in an estuary, the concentration of the Fe–HA complex would decrease.  相似文献   

2.
Chitosan–metal complexes have been widely studied in wastewater treatment, but there are still various factors in complex preparation which are collectively responsible for improving the adsorption capacity need to be further studied. Thus, this study investigates the factors affecting the adsorption ability of chitosan–metal complex adsorbents, including various kinds of metal centers, different metal salts and crosslinking degree. The results show that the chitosan–Fe( Ⅲ) complex prepared by sulfate salts exhibited the best adsorption efficiency(100%) for various dyes in very short time duration(10 min), and its maximum adsorption capacity achieved 349.22 mg/g. The anion of the metal salt which was used in preparation played an important role to enhance the adsorption ability of chitosan–metal complex. SO_4~(2-) ions not only had the effect of crosslinking through electrostatic interaction with amine group of chitosan polymer, but also could facilitate the chelation of metal ions with chitosan polymer during the synthesis process.Additionally, the p H sensitivity and the sensitivity of ionic environment for chitosan–metal complex were analyzed. We hope that these factors affecting the adsorption of the chitosan–metal complex can help not only in optimizing its use but also in designing new chitosan–metal based complexes.  相似文献   

3.
The adsorption of six kinds of chlorophenols on pristine, hydroxylated and carboxylated single-walled carbon nanotubes(SWCNTs) has been investigated. Pseudo-first order and pseudo-second order models were used to describe the kinetic data. All adsorption isotherms were well fitted with Langmuir, Freundlich and Polanyi–Manes models, due to surface adsorption dominating the adsorption process. The close linear relationship between log Kowand log Kdsuggested that hydrophobicity played an important role in the adsorption. The SWCNTs' adsorption capacity for chlorophenols was weakened by addition of oxygen-containing functional groups on the surface, due to the loss of specific surface area, the increase of hydrophilicity and the reduction of π–π interaction. The best adsorption capacity of pristine SWCNTs, SWCNT-OH and SWCNT-COOH for six chlorophenols varied from 19 to 84 mg/g, from 19 to 65 mg/g and from 17 to 65 mg/g,respectively. The effect of pH on the adsorption of 2,6-dichlorophenol(2,6-DCP), was also studied. When p H is over the pK aof 2,6-dichlorophenol(2,6-DCP), its removal dropped sharply. When ionic strength increased(Na Cl or KCl concentration from 0 to 0.02 mmol/L),the adsorption capacity of 2,6-DCP on pristine SWCNTs decreased slightly. The comparison of chlorophenols adsorption by SWCNTs, MWCNTs and PAC was made, indicating that the adsorption rate of CNTs was much faster than that of PAC. The results provide useful information about the feasibility of SWCNTs as an adsorbent to remove chlorophenols from aqueous solutions.  相似文献   

4.
Soil and sediment play a crucial role in the fate and transport of perfluorooctane sulfonate (PFOS) in the environment. However, the molecular mechanisms of major soil/sediment components on PFOS adsorption remain unclear. This study experimentally isolated three major components in soil/sediment: humin/kerogen, humic/fulvic acid (HA/FA), and inorganic component after removing organics, and explored their contributions to PFOS adsorption using batch adsorption experiments and molecular dynamic simulations. The results suggest that the humin/kerogen component dominated the PFOS adsorption due to its aliphatic featureswhere hydrophobic effect and phase transfer are the primary adsorptionmechanism. Compared with the humin/kerogen, the HA/FA component contributed less to the PFOS adsorption because of its hydrophilic and polar characteristics. The electrostatic repulsion between the polar groups of HA/FA and PFOS anions was attributable to the reduced PFOS adsorption.When the soil organicmatterwas extracted, the inorganic component also plays a non-negligible role because PFOS molecules might form surface complexes on SiO2 surface. The findings obtained in this study illustrate the contribution of organic matters in soils and sediments to PFOS adsorption and provided newperspective to understanding the adsorption process of PFOS on micro-interface in the environment.  相似文献   

5.
The study was to investigate the adsorption behavior of arsenite (As(Ⅲ)) and arsenate (As(Ⅴ)) on two variable charge soils, i.e., Haplic Acrisol and Rhodic Ferralsol at different ionic strengths and pH with batch methods. Results indicated that the amount of As(Ⅲ) adsorbed by these two soils increased with increasing solution pH, whereas it decreased with increasing ionic strength under the acidic condition. This suggested that As(Ⅲ) was mainly adsorbed on soil positive charge sites through electrostatic attraction under the acidic condition. Moreover, intersects of As(Ⅴ) adsorption-pH curves at different ionic strengths (a characteristic pH) are obtained for both soils. It was noted that above this pH, the adsorption of As(Ⅴ) was increased with increasing ionic strength, whereas below it the reverse trend was true. Precisely the intersect pH was 3.6 for Haplic Acrisol and 4.5 for Rhodic Ferralsol, which was near the values of PZSE (soil point of zero salt effect) of these soils. The effects of ionic strength and pH on arsenate adsorption by these soils were interpreted by the adsorption model. The results of zeta potential suggested that the potential in adsorption plane becomes less negative with increasing ionic strength above soil PZSE and decreases with increasing ionic strength below soil PZSE. These results further supported the hypothesis of the adsorption model that the potential in the adsorption plane changes with ionic strength with an opposite trend to surface charge of the soils. Therefore, the change of the potential in the adsorption plane was mainly responsible for the change of arsenate adsorption induced by ionic strength on variable charge soils.  相似文献   

6.
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   

7.
A method of size exclusion chromatography coupled with ultraviolet spectrophotometry and off-line graphite furnace atomic absorption spectrometry was developed to assess the complexation properties of iron (Fe) and humic acid (HA) in a water environment. The factors affecting the complexation of Fe and HA, such as ionic strength, pH, temperature and UV radiation, were investigated. The Fe-HA complex residence time was also studied. Experimental results showed that pH could influence the deprotonation of HA and hydrolysis of Fe, and thus affected the complexation of Fe and HA. The complexation was greatly disrupted by the presence of NaCl. Temperature had some influence on the complexation. The yield of Fe-HA complexes showed a small decrease at high levels of UV radiation, but the effect of UV radiation on Fe-HA complex formation at natural levels could be neglected. It took about 10 hr for the complexation to reach equilibrium, and the Fe-HA complex residence time was about 20 hr. Complexation of Fe and HA reached a maximum level under the conditions of pH 6, very low ionic strength, in the dark and at a water temperature of about 25°C, for 10 hr. It was suggested that the Fe-HA complex could form mainly in freshwater bodies and reach high levels in the warm season with mild sunlight radiation. With changing environmental parameters, such as at lower temperature in winter or higher pH and ionic strength in an estuary, the concentration of the Fe-HA complex would decrease.  相似文献   

8.
Fe–Mn binary oxide (FMBO) possesses high efficiency for As(III) abatement based on the good adsorption affinity of iron oxide and the oxidizing capacity of Mn(IV), and the composition and structure of FMBO play important roles in this process. To compare the removal performance and determine the optimum formula for FMBO, magnetic graphene oxide (MRGO)–FMBO and MRGO–MnO2 were synthesized with MRGO as a carrier to improve the dispersity of the adsorbents in aquifers and achieve magnetic recycling. Results indicated that MRGO–FMBO had higher As(III) removal than that of MRGO–MnO2, although the ratios of Fe and Mn were similar, because the binary oxide of Fe and Mn facilitated electron transfer from Mn(IV) to As(III), while the separation of Mn and Fe on MRGO–MnO2 restricted the process. The optimal stoichiometry x for MRGO–FMBO (MnxFe3-xO4) was 0.46, and an extraordinary adsorption capacity of 24.38 mg/g for As(III) was achieved. MRGO–FMBO showed stable dispersive properties in aquifers, and exhibited excellent practicability and reusability, with a saturation magnetization of 7.6 emu/g and high conservation of magnetic properties after 5 cycles of regeneration and reuse. In addition, the presence of coexisting ions would not restrict the practical application of MRGO–FMBO in groundwater remediation. The redox reactions of As(III) and Mn(IV) on MRGO–FMBO were also described. The deprotonated aqueous As(III) on the surface of MRGO–FMBO transferred electrons to Mn(IV), and the formed As(V) oxyanions were bound to ferric oxide as inner-sphere complexes by coordinating their “–OH” groups with Mn(IV) oxides at the surface of MRGO–FMBO. This work could provide new insights into high-performance removal of As(III) in aquifers.  相似文献   

9.
A study on the removal of Co(Ⅱ) from aqueous solutions by water treatment residuals(WTR)was conducted in batch conditions. The sorption process of Co(Ⅱ) followed pseudosecondorder kinetics, with 30 hr required to reach equilibrium. Using the Langmuir adsorption isotherm model, a relatively high maximum sorption capacity of 17.31 mg/g Co(Ⅱ) was determined. The adsorption of Co(Ⅱ) was dependent on pH values and was affected by the ionic strength. Results show that Co(Ⅱ) adsorption was a spontaneous endothermic process and was favorable at high temperature. Most of the adsorbed Co(Ⅱ) stayed on the WTR permanently, whereas only small amounts of adsorbed Co(Ⅱ) were desorbed. The shifting of peaks in FT-IR spectra indicated that Co(Ⅱ) interacted with the WTR surface through strong covalent bond formation with Fe(Al)–O functional groups. It was concluded that WTR can be a suitable material from which to develop an efficient adsorbent for the removal of Co(Ⅱ) from wastewater.  相似文献   

10.
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   

11.
Shortage in phosphorus (P) resources and P wastewater pollution is considered as a serious problem worldwide. The application of modified biochar for P recovery from wastewater and reuse of recovered P as agricultural fertilizer is a preferred process. This work aims to develop a calcium and magnesium loaded biochar (Ca–Mg/biochar) application for P recovery from biogas fermentation liquid. The physico-chemical characterization, adsorption efficiency, adsorption selectivity, and postsorption availability of Ca-Mg/biochar were investigated. The synthesized Ca–Mg/biochar was rich in organic functional groups and in CaO and MgO nanoparticles. With the increase in synthesis temperature, the yield decreased, C content increased, H content decreased, N content remained the same basically, and BET surface area increased. The P adsorption of Ca–Mg/biochar could be accelerated by nano-CaO and nano-MgO particles and reached equilibrium after 360 min. The process was endothermic, spontaneous, and showed an increase in the disorder of the solid–liquid interface. Moreover, it could be fitted by the Freundlich model. The maximum P adsorption amounts were 294.22, 315.33, and 326.63 mg/g. The P adsorption selectivity of Ca–Mg/biochar could not be significantly influenced by the typical pH level of biogas fermentation liquid. The nano-CaO and nano-MgO particles of Ca–Mg/biochar could reduce the negative interaction effects of coexisting ions. The P releasing amounts of postsorption Ca–Mg/biochar were in the order of Ca–Mg/B600 > Ca–Mg/B450 > Ca–Mg/B300. Results revealed that postsorption Ca–Mg/biochar can continually release P and is more suitable for an acid environment.  相似文献   

12.
Batch experiments were conducted to evaluate fluoride removal by Al,Fe,and Ti-based coagulants and adsorbents,as well as the effects of coexisting ions and formation of aluminum–fluoride complexes on fluoride removal by co-precipitation with alum(Al_2(SO_4)_3·18H_2O).Aluminum sulfate was more efficient than the other coagulants for fluoride removal in the pH range between 6 and 8.Nano-crystalline TiO_2 was more effective for fluoride removal than Al and Fe hydroxides in a pH range of 3–5.Coexisting anions in water decreased the removal of fluoride in the order:phosphate(2.5 mg/L) arsenate(0.1 mg/L) bicarbonate(200 mg/L) sulfate(100 mg/L) = nitrate(100 mg/L) silicate(10 mg/L) at a pH of 6.0.The effect of silicate became more significant at pH 7.0.Calcium and magnesium improved the removal of fluoride.Zeta-potential measurements determined that the adsorption of fluoride shifted the PZC of Al(OH)_3 precipitates from 8.9 to 8.4,indicating the chemical adsorption of fluoride at the surface.The presence of fluoride in solution significantly increased the soluble aluminum concentration at pH 6.5.A Visual MINTEQ modeling study indicated that the increased aluminum solubility was caused by the formation of AlF~(2+),AlF~(+2),and AlF_3complexes.The AlF_x complexes decreased the removal of fluoride during co-precipitation with aluminum sulfate.  相似文献   

13.
刘泽珺  周少奇  马福臻 《环境科学》2018,39(3):1233-1240
采用原位聚合热合成法成功制备了聚丙烯酰胺-壳聚糖季铵盐半互穿网络水凝胶(PAAm/HACC semi-IPN)新型吸附剂(s-IPN 1.5)和(s-IPN 3),并用于吸附水体中的腐殖酸.利用扫描电镜(SEM)、红外光谱(FT-IR)、X射线衍射光谱(XRD)等方法对吸附剂的结构进行表征.考察了溶液pH、离子强度、接触时间、腐殖酸初始浓度及温度等对吸附剂吸附腐殖酸的影响.结果表明s-IPN 3的吸附效果要优于s-IPN 1.5.吸附剂对腐殖酸的吸附量随着pH的增大而减小,随温度的升高而增大,且一定的离子强度有助于吸附剂对腐殖酸的吸附.吸附过程能较好地用准二级动力学模型及Sips等温模型进行拟合.吸附剂在pH 7.0,离子强度0.01 mol·L-1,温度为298 K条件下的最大吸附量可高达238.08 mg·g-1,吸附效果显著,能有效去除水体中的腐殖酸.  相似文献   

14.
This study focuses on the effects of pH and fluoride at different molar ratios of fluoride to Al (RF:Al) on the removal of cadmium (Cd2+) and phosphate by Al coagulation. Fluoride at RF:Al ≥ 3:1 inhibits the removal of Cd over wide Al dose ranges from 5 to 10 mg/L as Al. The removal of phosphate decreases significantly at high RF:Al of 10:1 whereas at lowered RF:Al (i.e., ≤ 6:1), an adverse effect is observed only at insufficient Al doses below 2 mg/L. Fluoride shows inhibitive effects towards the removal of Cd at pH 7 and 8 and that of phosphate at pH 6. Fluoride decreases the ζ-potential in both systems, and the decreasing extent is positively correlated to the elevated RF:Al. The Al fluoride interactions include the formation of Al–F complexes and the adsorption of fluoride onto Al(OH)3 precipitates, i.e., the formation of Al(OH)nFm. Al–F complex formation inhibits Al hydrolysis and increases residual Al levels, and a more significant increase was observed at lower pH. Al–F complexes at high RF:Al complicate the coagulation behavior of Al towards both negative and positive ionic species. Moreover, fluoride at low RF:Al shows little effect on Al coagulation behavior towards Cd2 + and phosphate, and the spent defluoridation adsorbent, i.e., aluminum (Al) hydro(oxide) with adsorbed fluoride at RF:Al of below 0.1:1, may be reclaimed as a coagulant after being dissolved.  相似文献   

15.
Herein,palygorskite(PAL)was activated via a simple hydrothermal process in the presence of ammonium sulfide,and the effects of activation on the microstructure,physico-chemical feature and adsorption behaviors of PAL were intensively investigated.The hydrothermal process evidently improved the dispersion of PAL crystal bundles,increased surface negative charges and built more active –Si–O-groups served as the new"adsorption sites".The adsorption property of the activated PAL for Methyl Violet(MV)was systematically investigated by optimizing the adsorption variables,including p H,ionic strength,contact time and initial MV concentration.The activated PAL exhibited a superior adsorption capability to the raw PAL for the removal of MV(from 156.05 to 218.11 mg/g).The kinetics for MV adsorption followed pseudo second-order kinetic models,while the isotherm and thermodynamics results showed that the adsorption pattern well followed the Langmuir model.The structure analysis of PAL before and after adsorption demonstrated that electrostatic interaction and chemical association of –X–O-are the prominent driving forces for the adsorption process.  相似文献   

16.
以硝酸钙、磷酸氢二铵和腐殖酸为原料,制备了腐殖酸负载羟基磷灰石(HA/HAP)复合吸附剂.同时,利用SEM、BET、FT-IR、XRD对复合吸附剂结构和形貌进行表征,研究了HA/HAP对废水中Cd~(2+)的吸附工艺.结果表明,腐殖酸使羟基磷灰石孔容和孔径增大、比表面积减小,从而提高了羟基磷灰石的吸附性能.在pH=6、吸附剂投加量为800 mg、接触时间为180 min时吸附率最佳,为98.3%.HA/HAP对废水中Cd~(2+)的吸附是自发的、吸热的、可持续的化学吸附,反应前120 min适合采用准一级动力学伴随着内扩散模型描述,后120 min适合采用准二级动力学伴随着内扩散模型描述,Dubinin-Radushkevich(D-R)等温线模型拟合的吸附数据在不同温度下效果最好(R~20.98),吸附量分别为259.15、266.05和264.66 mg·g~(-1).研究表明,静电吸附到腐殖酸活性位点后Cd~(2+)主要以络合反应被吸附到羟基磷灰石的表面和两个羟基中间.  相似文献   

17.
In order to study the influences of functionalized groups onto the adsorption of tetracycline (TC), we prepared a series of amino and amino–Fe3 + complex mesoporous silica adsorbents with diverse content of amino and Fe3 + groups (named N,N-SBA15 and Fe-N,N-SBA15). The resulting mesoporous silica adsorbents were fully characterized by X-ray powder diffraction, Fourier transform infrared spectrometer and N2 adsorption/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/Fe3 + groups. The functionalized amino groups decreased the adsorption capacity while the coordinated Fe3 + 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 Fe3 + content increased from 3.93% to 8.26%, the Qmax of the adsorbents increased from 102 to 188 mmol/kg. The solution pH 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   

18.
腐殖酸对针铁矿吸附磷的影响机理   总被引:3,自引:0,他引:3  
通过添加HA(Humic acid,腐殖酸),研究不同环境条件下HA对针铁矿吸附磷的影响.结果显示,加入HA能显著降低磷吸附量,pH为4.5时分别加入100和40 mg/L HA,磷的最大吸附量分别降低了26.6%和25.6%;pH为7.0时分别加入100和40mg/L HA,磷的最大吸附量分别降低了26.8%和23.1%.不同添加顺序试验结果表明:针铁矿对磷的吸附量大小顺序为后添加HA>同时添加HA和磷>先添加HA;无论是否添加HA,针铁矿对磷的吸附量都随着pH的升高而降低,相应的吸附等温线也都符合Langmuir吸附等温方程;总有机碳和红外光谱特征表明,HA和磷在针铁矿表面吸附点位形成竞争吸附,并且针铁矿表面的羟基在吸附磷和HA的过程中起到了一定的作用.  相似文献   

19.
Insights from the adverse effect of humic acid(HA) on arsenate removal with hydrous ferric oxide(HFO) coprecipitation can further our understanding of the fate of As(V) in water treatment process. The motivation of our study is to explore the competitive adsorption mechanisms of humic acid and As(V) on HFO on the molecular scale. Multiple complementary techniques were used including macroscopic adsorption experiments, surface enhanced Raman scattering(SERS), extended X-ray absorption fine structure(EXAFS) spectroscopy, flow-cell attenuated total reflectance Fourier transform infrared(ATR-FTIR) measurement, and charge distribution multisite complexation(CDMUSIC) modeling. The As(V) removal efficiency was reduced from over 95% to about 10% with the increasing HA concentration to 25 times of As(V) mass concentration. The SERS analysis excluded the HA-As(V) complex formation. The EXAFS results indicate that As(V) formed bidentate binuclear surface complexes in the presence of HA as evidenced by an As-Fe distance of 3.26–3.31 ?. The in situ ATR-FTIR measurements show that As(V) replaces surface hydroxyl groups and forms innersphere complex. High concentrations of HA may physically block the surface sites and inhibit the As(V) access. The adsorption of As(V) and HA decreased the point of zero charge of HFO from 7.8 to 5.8 and 6.3, respectively. The CD-MUSIC model described the zeta potential curves and adsorption edges of As(V) and HA reasonably well.  相似文献   

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