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1.
Batch experiments were performed to derive the rate laws for the proton-promoted dissolution of the main vanadium (III, IV and V) oxides at pH 3.1–10.0. The release rates of vanadium are closely related to the aqueous pH, and several obvious differences were observed in the release behavior of vanadium from the dissolution of V2O5 and vanadium(III, IV) oxides. In the first 2 hr, the release rates of vanadium from V2O3 were r = 1.14·([H+])0.269 at pH 3.0–6.0 and r = 0.016·([H+])? 0.048 at pH 6.0–10.0; the release rates from VO2 were r = 0.362·([H+])0.129 at pH 3.0–6.0 and r = 0.017·([H+])? 0.097 at pH 6.0–10.0; and the release rates from V2O5 were r = 0.131·([H+])? 0.104 at pH 3.1–10.0. The release rates of vanadium from the three oxides increased with increasing temperature, and the effect of temperature was different at pH 3.8, pH 6.0 and pH 7.7. The activation energies of vanadium (III, IV and V) oxides (33.4–87.5 kJ/mol) were determined at pH 3.8, pH 6.0 and pH 7.7, showing that the release of vanadium from dissolution of vanadium oxides follows a surface-controlled reaction mechanism. The release rates of vanadium increased with increasing vanadium oxides dose, albeit not proportionally. This study, as part of a broader study of the release behavior of vanadium, can help to elucidate the pollution problem of vanadium and to clarify the fate of vanadium in the environment.  相似文献   

2.
The oxidation of antimony (III) in soils was studied using X-ray absorption fine structure (XAFS) spectra. An andosol soil sample and artificial soil samples (SiO2 blended with iron (III) hydroxide and manganese (IV) oxide) were used herein. After adding antimony (III) oxide to all soil samples, the oxidation process was observed by recording the XAFS spectra of Sb K-edge, Fe K-edge, and Mn K-edge. The results indicated that manganese (IV) oxide played an important role in the oxidation of Sb(III); however iron (III) hydroxide was not directly related to the reaction. During a 2-hr continuous Sb K-edge X-ray absorption near edge structure (XANES) measurement with an interval of 1 min of one of the artificial soil samples (SiO2 + MnO2 + Sb2O3), a pseudo-first-order reaction was determined with an average estimated rate of 0.52 ± 0.04 hr? 1. Compared to the lower oxidation rate of andosol, it is suggested that because of the low concentration of Mn(IV) in natural soils, the oxidation process of Sb(III) might be relatively slow and require more time to convert Sb(III) to Sb(V).  相似文献   

3.
The arsenic removal efficiency of iron-modified activated carbons depends greatly on the number of available iron oxide surface sites, which are given by the surface area of the anchored particles. In this sense, aiming the generation of an adsorbent with superior arsenic adsorption capacity, we developed a protocol to anchor interconnected fibrils of iron oxyhydroxides, using Mn2 + as a morphology regulator. The protocol was based on a microwave-assisted hydrothermal method, using bituminous based activated carbon and both Fe2 + and Mn2 + ions in the hydrolysis solution. The elemental analysis of modified carbons revealed that Mn does not anchor to the carbon. However, when Mn is included in the hydrolysis solution, the iron content in the activated carbon increased up to 3.5?wt%, without considerable decreasing the adsorbent surface area. Under specific hydrothermal conditions, the Mn2 + promoted the formation of iron oxide nanoparticles shaped as interconnected fibrils. This material showed a superior arsenic adsorption capacity in comparison to similar iron modified activated carbons (5?mg As/g carbon, at 2?mg As/L), attributed to the increase in quantity and availability of active sites located on the novel interconnected fibrils of iron oxyhydroxides nanostructures.  相似文献   

4.
Mercury (Hg) is among the most concerned contaminants in the world. It has three major chemical forms in the environment, including Hg0, Hg2 +, and methylmercury (MeHg). Due to their differences in toxicity, mobility, and bioavailability, speciation analysis is critical for understanding Hg cycling and fate in the environment. SnCl2 reduction-atomic fluorescence spectrometry detection is the most commonly used method for analyzing inorganic Hg. However, it should be noted that MeHg may also be reduced by SnCl2, which would result in the overestimation of inorganic Hg. In this study, the reduction of MeHg by SnCl2 in both de-ionized (DI) water and four natural waters was investigated. The results showed that MeHg could be reduced by SnCl2 in DI water whereas this reaction was hard to occur in tested natural waters. By investigating the effects of water chemical characteristics (dissolved organic matter, pH and common anions and cations) on this reaction, SO42 ? was identified to be the dominant factor prohibiting SnCl2 induced MeHg reduction in natural waters. SO42 ? in natural waters was evidenced to be reduced to S2 ? by SnCl2 and the generated S2 ? can complex with MeHg to form MeHgS? which is hard to be reduced by SnCl2. Findings of this study indicate that the effect of MeHg reduction by SnCl2 on inorganic Hg analysis is negligible in natural waters; however, at simulated experimental systems without SO42 ?, SO42 ? should be added as protecting agents to prevent MeHg reduction when analyzing inorganic Hg if it would not cause any other unwanted effects.  相似文献   

5.
The inter-conversion of nitrogen and sulfur species between the gas and particulate phases and their interaction with alkaline species influences the acidity of the aerosols and surface snow. To better understand these processes, a short field campaign was undertaken in Ny-Ålesund, Svalbard, during 13th April 2012 to 24th April 2012. Air measurements were carried out through a particulate sampler equipped with denuders and filter packs for simultaneous collection of trace gases (HNO3, NO2, SO2 and reactive nitrogen compounds) and aerosols, with daily collection of snow samples. Ionic composition of the samples was analyzed using ion chromatography technique. The results suggested that nitrate-rich aerosols are formed when PAN (peroxy acetyl nitrate) disassociates to form NO2 and HNO3 which further hydrolyzes to form pNO3? (particulate nitrate). This resulted in a high contribution of pNO3? (62%) to the total nitrogen budget over the study area. The acidity of the aerosols and snow evaluated through cation/anion ratio (C/A) indicated alkaline conditions with C/A > 2. The bicarbonates/carbonates of Mg2 + played an important role in neutralization processes of surface snow while the role of NH3 was dominant in aerosol neutralization processes. Such neutralization processes can increase the aerosol hygroscopicity causing warming. Chloride depletion in the snow was significant as compared to the aerosols, indicating two important processes, scavenging of coarse sea salt by the snow and gaseous adsorption of SO2 on the snow surface. However, a more systematic and long term study is required for a better understanding of the neutralization processes and chemical inter-conversions.  相似文献   

6.
A method was developed for preparing high purity Al30O8(OH)56(H2O)2418 + (Al30) through elimination of impurities by complexation. Polyaluminum chloride II (PAC30) with Alc content of 75% was adopted as the source of Al30. The PAC30 was prepared under conditions of total aluminum concentration 0.1?mol/L and OH?/Al ratio 2.2 to obtain the highest content of Al30. A precipitation/metathesis method, organic solvent precipitation method and organic complexation method were examined to separate and purify Al30. It was found that only by the organic complexation method could high purity Al30 products be obtained in large yield economically. In the experiments, benzoic acid was used as the coordinating reagent to decompose the main impurity AlO4Al12(OH)24(H2O)127 + (Al13), and the Al30 product could be obtained by precipitation and metathesis operations. It was noteworthy that the decomposition of impurities by benzoic acid could be completed in 2?hr. The Al30 product was characterized by Ferron assay, 27Al-NMR, SEM, XRD and TGA. The results showed that the purity of the Al30 product could exceed 92%.  相似文献   

7.
Processes based on non-thermal plasma (NTP) for indoor air treatment inevitably lead to the formation of toxic by-products such as ozone (O3) and nitrogen oxides (NOx). Adding a step of heterogeneous catalysis in series with NTP could allow for the decomposition of the by-products. Therefore, different catalysts were developed based on transition metal oxides, such as NiOx, CoOx and MnOx with different weight percentage 1, 5 and 10 wt.%, deposited on a γ-Al2O3 support. The O3 removal efficiency (ORE) and the NOx removal efficiency (NRE) were very encouraging in dry air: about 65% and 80%, respectively, by using 2 g 5 wt.% MnOx/Al2O3 catalyst under the experimental conditions. However, strongly negative effects of relative humidity (RH) on the catalytic decomposition performance were observed. To overcome this limitation, the catalyst surface was modified to make it hydrophobic using a cost-effective chemical grafting method. This treatment consisted in impregnating the 5 wt.% MnOx/Al2O3 catalyst with different trichloro(alkyl)silanes (TCAS). The effects of different linker lengths and amounts of TCAS for the hydrophobicity and the decomposition performance of surface-modified catalysts under humid conditions were investigated. Our results show that the surface-modified catalyst with the shortest linker and 0.25 mmol/gcat of modifying agent represents the best catalytic decomposition performance for O3. Its ORE is 41% at 60% RH, which is twice that of the non-modified catalyst.  相似文献   

8.
Precipitation represents an important phenomenon for carbon and nitrogen deposition. Here, the concentrations and fluxes of dissolved organic carbon (DOC) and total dissolved nitrogen (TDN) with their potential sources were analyzed in wet precipitation during summer monsoon from the Northern Indo-Gangetic Plain (IGP), important but neglected area. The volume-weighted mean (VWM) concentration of DOC and TDN were 687.04 and 1210.23 µg/L, respectively. Similarly, the VWM concentration of major ions were in a sequence of NH4+ > Ca2+ > SO42- > Na+ > K+ > NO3? > Cl? > Mg2+ > F? > NO2?, suggesting NH4+ and Ca2+ from agricultural activities and crustal dust played a vital role in precipitation chemistry. Moreover, the wet deposition flux of DOC and TDN were 9.95 and 17.06 kg/(ha?year), respectively. The wet deposition flux of inorganic nitrogen species such as NH4+-N and NO3?-N were 14.31 and 0.47 kg/(ha?year), respectively, demonstrating the strong influence of emission sources and precipitation volume. Source attribution from different analysis suggested the influence of biomass burning on DOC and anthropogenic activities (agriculture, animal husbandry) on nitrogenous species. The air-mass back trajectory analysis indicated the influence of air masses originating from the Bay of Bengal, which possibly carried marine and anthropogenic pollutants along with the biomass burning emissions to the sampling site. This study bridges the data gap in the less studied part of the northern IGP region and provides new information for policy makers to deal with pollution control.  相似文献   

9.
Niobium oxide nanowire-deposited carbon fiber (CF) samples were prepared using a hydrothermal method with amorphous Nb2O5·nH2O as precursor. The physical properties of the samples were characterized by means of numerous techniques, including X-ray diffraction (XRD), energy-dispersive spectroscopy (EDS), scanning electron microscopy (SEM), transmission electron microscopy (TEM), selected-area electron diffraction (SAED), UV–visible spectroscopy (UV–vis), N2 adsorption–desorption, Fourier transform infrared spectroscopy (FT-IR), and X-ray photoelectron spectroscopy. The efficiency for the removal of Cr(VI) was determined. Parameters such as pH value and initial Cr(VI) concentration could influence the Cr(VI) removal efficiency or adsorption capacity of the Nb2O5/carbon fiber sample obtained after hydrothermal treatment at 160°C for 14 hr. The maximal Cr(VI) adsorption capacity of the Nb2O5 nanowire/CF sample was 115 mg/g. This Nb2O5/CF sample also showed excellent photocatalytic activity and stability for the reduction of Cr(VI) under UV-light irradiation: the Cr(VI) removal efficiency reached 99.9% after UV-light irradiation for 1 hr and there was no significant decrease in photocatalytic performance after the use of the sample for 10 repeated cycles. Such excellent Cr(VI) adsorption capacity and photocatalytic performance was related to its high surface area, abundant surface hydroxyl groups, and good UV-light absorption ability.  相似文献   

10.
To better understand the characteristics and sources of water soluble ions (WSI) in North China Plain (NCP), fine particles (PM2.5) were simultaneously sampled at the summit (SM) and foot (FT) of Mount Tai during May 12th to June 24th, 2017. Ion chromatography analysis showed that concentration of WSI was lower at SM (22.26 ± 16.53 μg/m3) than that at FT (31.02 ± 21.92 μg/m3). The concentration and proportion of SO42? in total WSI were both lower than the values reported in previous studies. Daytime WSI concentrations were higher than that at nighttime at SM, while the opposite results were obtained at FT, possibly associated with more anthropogenic activities and higher boundary layer height (BLH) during daytimes. A severe pollution event occurred during June 14th – June 16th was documented at both FT and SM. Regional transport and topography-forced vertical transport along the slope of the mountain could explain the higher concentrations of pollutants at SM. The analyses also indicated that NH4+ existed mainly in the form of NH4HSO4 and NH4NO3, but (NH4)2SO4 could also exist, especially when emissions of NH4+ and NH3 were increased during daytime at FT. The results of principal component analysis (PCA) illustrated that secondary aerosols, coal/biomass burnings, sea-salts and crustal/soil dusts were the main sources at SM, and secondary aerosols and crustal/soil dusts contributed most at FT. Backward air-mass trajectories were classified into four clusters, of which air masses with the highest frequency and WSI concentrations were originated from the southwest with secondary ions (SO42-, NO3- and NH4+) as major pollutants.  相似文献   

11.
阳离子改型蛭石的铵离子交换平衡特性   总被引:1,自引:0,他引:1  
对经Na^+,Ca^2+、Mg^2+等不同离子处理的改型蛭石在不同pH和温度条件下进行了铵离子交换性能的研究。结果表明,交换反应均在前60min速率最快,约120min就趋向于平衡:铵离子交换总量均随pH变化而波动,在pH=7点上取最大值,且全交换容量按镁型蛭石、钙型蛭石,钠型蛭石顺序依次增大,每100g蛭石分别为59.32,71.89、92.85mmol;改型蛭石对NH^+4等温交换吸附与Langmuir方程相符。表明改型蛭石对NH^+4的吸附主要是单分子层的化学吸附。  相似文献   

12.
采用球磨混合方法,将催化剂以m(Cu/SAPO-34):m(VW/TiO2)为1:1的比例制得干混样品SAPO-Ti。利用固定床实验台架研究了混合催化剂的NH3-SCR脱硝性能及其抗硫性能。采用 XRD、BET、SEM、H2-TPR、NH3-TPD和in-situ DRIFT对材料进行表征,结果显示,球磨混合样品SAPO-Ti同时具有2种催化剂的晶体结构,且酸量增加,中温活性提高。表面形貌研究表明,VW/TiO2催化剂覆盖在Cu/SAPO-34催化剂表面,对Cu/SAPO-34催化剂起到保护作用;原位红外结果显示,Cu/SAPO-34催化剂硫中毒失活主要是在Cu活性位上形成硫酸盐物种,导致活性位减少,脱硝效率下降,而SAPO-Ti表面形成硫酸盐的数量减少,抗硫性能提高,主要是由于表面VW/TiO2催化剂具有良好的抗硫性,保护内部Cu2+活性位,以保持高效中温脱硝性能。  相似文献   

13.
Biological nitrogen removal process could be affected due to the presence of heavy metals owing to their toxicity and accumulation in the sludge.In this study,the impact of Cu~(2+)shock on a long-term nitritation operation was investigated in an air-lift reactor with selfrecirculation.Both the dynamics of microbial community and inhibition kinetics under Cu~(2+) stress were ascertained.The results showed that Cu~(2+) exerted severe inhibition on nitritation performance of an air-lift reactor(ALR) at 25 mg/L.The corresponding NH_4~+-N removal efficiency decreased to below 50%,which was mainly due to the variation of microbial community structure,especially the inhibition of nitrifiers like Nitrosomonas(the relative abundance decreased from 30% to 1% after Cu~(2+)inhibition).Kinetic parameters were obtained and compared after fitting the Haldane model.The long-term Cu~(2+) stress on the ALR aggravated the ammonium affinity and the resistance to substrate self-inhibition of the nitritation sludge,but reduced the resistance to Cu~(2+) inhibition.Furthermore,Cu~(2+)acted as uncompetitive inhibitor on nitritation process.Our results provide new insights into the nitritation characteristics under long-term Cu~(2+) stress.  相似文献   

14.
Me/SAPO-34 (Me = Mn, Ni, Co) series of catalysts were prepared by a wetness impregnation method and investigated for the selective catalytic reduction of nitrogen oxides with ammonia (NH3-SCR). Among them, Mn/SAPO-34 catalyst was found as the most promising candidate based on its superior low-temperature activity. The catalysts were characterized by X-ray diffraction (XRD), transmission electron microscopy images (TEM), nuclear magnetic resonance (NMR), X-ray photoelectron spectroscopy (XPS), temperature programmed reduction and desorption (TPR and TPD), and diffuse reflectance infrared Fourier transformed spectroscopy (DRIFTS) of NH3/NOx adsorption. Mn/SAPO-34 is obviously different from Ni/SAPO-34 and Co/SAPO-34 in the active species state and distribution. Surface MnOx species which play an essential role in NO oxidation and NO2 adsorption, act as better active sites than nickel and cobalt mostly in the form of the aluminates and silicates.  相似文献   

15.
十二烷基磺酸钠(SDS)改性蒙脱石对Cu~(2+)、Cd~(2+)的吸附研究   总被引:10,自引:3,他引:7  
以阴离子表面活性剂(十二烷基磺酸钠,SDS)为改性剂制备了有机蒙脱石,研究其对Cu2+、Cd2+的吸附行为,并用XRD、FTIR、SEM、XPS对有机蒙脱石进行表征.实验结果表明,有机蒙脱石对Cu2+、Cd2+的吸附基本上在20min内达到平衡,并随pH增大(1.0~7.0),吸附量增加,最佳pH约为6.0.有机蒙脱石对Cu2+、Cd2+的吸附等温线更符合Langmuir等温吸附方程,SDS改性蒙脱石对Cu2+、Cd2+的最大吸附量较纯蒙脱石分别增加15.7%、15.5%.XRD、FTIR、SEM、XPS及碳含量分析结果显示,SDS主要分布在蒙脱石表面且相对稳定,少量嵌入层间,有机蒙脱石对Cu2+、Cd2+的吸附机制为配位吸附和离子交换.  相似文献   

16.
观察了不同浓度(10、20、40和80 μg/L)重金属离子Cu~(2+)和Zn~(2+)对日本新糠虾存活、蜕皮、蛋白含量和体内磷酸酶(碱性磷酸酶和酸性磷酸酶)活性的慢性(30 d)影响.结果显示:(1)Cu~(2+)和Zn~(2+)能明显降低糠虾存活率,金属离子浓度增高,存活率降低,其中Cu~(2+)引起的存活率降低更为明显,在最高浓度(80 μg/ L)Cu~(2+)组中糠虾的存活率仅为同浓度Zn~(2+)组的1/3,两组均明显低于对照组(P<0.05);Cu~(2+)和Zn~(2+)能明显降低糠虾蜕皮次数,最高浓度(80 μg/ L)Cu~(2+)和Zn~(2+)中糠虾的蜕皮数分别为11.00±1.73(次)和11.33±0.58(次),分别约为对照组的55.92%和57.6%.(2)Cu~(2+)和Zn~(2+)均能明显影响糠虾蛋白含量,其中Cu~(2+)的影响力更强,最高浓度(80 μg/ L)Cu~(2+)组糠虾体内蛋白白含量占湿重比为9.78%,仅约为对照组的1/2.(3)Cu~(2+)和Zn~(2+)能明显抑制糠虾体内两种磷酸酶的活力,碱性磷酸酶和酸性磷酸酶活力能作为糠虾监测环境重金属污染(Cu~(2+)和Zn~(2+))的检测指标.  相似文献   

17.
The concentration and speciation of heavy metals in soil solution isolated from long-term contaminated soils were investigated. The soil solution was extracted at 70% maximum water holding capacity (MWHC) after equilibration for 24 h. The free metal concentrations (Cd2+, Cu2+, Pb2+, and Zn2+) in soil solution were determined using the Donnan membrane technique (DMT). Initially the DMT was validated using artificial solutions where the percentage of free metal ions were significantly correlated with the percentages predicted using MINTEQA2. However, there was a significant difference between the absolute free ion concentrations predicted by MINTEQA2 and the values determined by the DMT. This was due to the significant metal adsorption onto the cation exchange membrane used in the DMT with 20%, 28%, 44%, and 8% mass loss of the initial total concentration of Cd, Cu, Pb, and Zn in solution, respectively. This could result in a significant error in the determination of free metal ions when using DMT if no allowance for membrane cation adsorption was made. Relative to the total soluble metal concentrations the amounts of free Cd2+ (3%–52%) and Zn2+ (11%–72%) in soil solutions were generally higher than those of Cu2+ (0.2%–30%) and Pb2+ (0.6%–10%). Among the key soil solution properties, dissolved heavy metal concentrations were the most significant factor governing free metal ion concentrations. Soil solution pH showed only a weak relationship with free metal ion partitioning coefficients (Kp) and dissolved organic carbon did not show any significant influence on Kp.  相似文献   

18.
零价铁(ZVI)去除Cu2+的特性及机制研究   总被引:3,自引:2,他引:1  
陈玉伟  王建龙 《环境科学》2009,30(11):3353-3357
研究了零价铁去除水溶液中铜离子的影响因素及动力学特性,并利用X射线衍射(XRD)分析对反应机制进行了探讨.结果表明,当溶液中Cu2+的浓度为300 mg/L,零价铁的用量为1 g/L时,Cu2+的去除率99%.Cu2+的去除速度很快,且反应前30min零价铁去除Cu2+的过程可以用一级反应动力学方程模拟.零价铁去除Cu2+的机制主要基于氧化还原反应,Cu2+的还原产物主要为Cu和Cu2O.  相似文献   

19.
A series of H-SAPO-34 zeolites were synthesized by a hydrothermal method in fluoride media. The as-synthesized H-SAPO-34 zeolites were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), N2 physisorption, temperature-programmed desorption of NH3 (NH3-TPD) and nuclear magnetic resonance (NMR) measurements. The results showed that a certain concentration of F anions promoted the nucleation and crystallization of H-SAPO-34. The H-SAPO-34 synthesized in the fluoride media showed high crystallinity, uniform particle size distribution, large specific surface area and pore volume, and enhanced acidity. Therefore, Cu/SAPO-34 based on the fluoride-assisted zeolite showed a broadened temperature window for the selective catalytic reduction of NO by NH3 (NH3-SCR) reaction due to the enhanced acidity of the zeolite and the improved dispersion of copper species.  相似文献   

20.
陈海平  周立祥  王世梅  梁剑茹 《环境科学》2009,30(11):3364-3370
城市污泥通常含有大量有机质但也存在数量不等有害金属,在不影响污泥有益成分的基础上,去除和回收污泥中金属,既使污泥无害化又产生经济效益,意义重大.针对苏州某工业园区污泥重金属含量较高,研究利用生物沥浸-溶剂萃取-电积技术回收城市污泥中重金属Cu的工艺,并探讨了采用5-壬基水杨醛肟萃取剂M5640从城市污泥生物沥浸液中萃取分离Cu和Fe的最佳工艺参数.结果表明,经过生物沥浸处理72 h后,城市污泥中重金属Cu溶出率高达90%.当最佳工艺条件为:萃取剂体积分数为2%,相比(有机相与水相体积比,以O/A表示)为1/3,沥浸液pH为2.0时,沥浸液中Cu的一级萃取率达到95%以上,而Fe的共萃率低于10%;反萃取试验结果表明,在反萃取相比为2/1的条件下用1.5 mol/L硫酸溶液进行反萃取,Cu的一级反萃取率达到80.07%;反萃取后的富集Cu溶液作为电解液,在槽电压为2.1 V、电解温度为55℃条件下电积6 h,Cu回收率达到90%以上.在整个工艺中萃余液和反萃液均可循环利用无废液排放,对含Cu高的污泥,利用生物沥浸-溶剂萃取-电积技术回收有良好的应用前景.  相似文献   

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