首页 | 本学科首页   官方微博 | 高级检索  
相似文献
 共查询到20条相似文献,搜索用时 609 毫秒
1.
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   

2.
Nitrate (NO3?) is known to be actively involved in the processes of mineralization and heavy metal transformation; however, it is unclear whether and how it affects the bioavailability of antimony (Sb) in paddy soils and subsequent Sb accumulation in rice. Here, the effects of NO3? on Sb transformation in soil-rice system were investigated with pot experiments over the entire growth period. Results demonstrated that NO3? reduced Sb accumulation in brown rice by 15.6% compared to that in the control. After amendment with NO3?, the Sb content in rice plants increased initially and then gradually decreased (in roots by 46.1%). During the first 15 days, the soil pH increased, the oxidation of Sb(III) and sulfides was promoted, but the reduction of iron oxide minerals was inhibited, resulting in the release of adsorbed and organic-bound Sb from soil. The microbial arsenite-oxidizing marker gene aoxB played an important role in Sb(III) oxidation. From days 15 to 45, after NO3? was partially consumed, the soil pH decreased, and the reductive dissolution of Fe(III)-bearing minerals was enhanced; consequently, iron oxide-bound Sb was transformed into adsorbed and dissolved Sb species. After day 45, NO3? was completely reduced, Sb(V) was evidently reduced to Sb(III), and green rust was generated gradually. Thus, the available Sb decreased due to its enhanced affinity for iron oxides. Moreover, NO3? inhibited the reductive dissolution of iron minerals, which ultimately caused low Sb availability. Therefore, NO3? can chemically and biologically reduce the Sb availability in paddy soils and alleviate Sb accumulation in rice. This study provides a potential strategy for decreasing Sb accumulation in rice in the Sb-contaminated sites.  相似文献   

3.
The soil moisture regime can affect the release of heavy metals in soil. In the previous studies, slightly polluted soils or artificially contaminated soil samples were considered to investigate the effect of soil moisture. We used highly smelter-contaminated and aged soils to study the release of typical heavy metals(Cu, Zn, Cd and Pb) induced by water incubation in batch experiments with characterization via speciation and X-ray diffraction analyses(XRD). The results show that the leachable concentrations of the heavy metals increased slightly in the first 30 days, decreased drastically between 30 and 90 days, and immobilized relatively constant thereafter. The fluctuation was ascribed to the changes of soil Eh and pH, the reductive dissolution of crystalline iron oxides, the formation of new amorphous iron oxides, the absorption of dissolved organic matter and the precipitation of metal sulfide. Speciation analysis indicated that a proportion of the soil heavy metals was transformed from an exchangeable fraction to a less labile fraction after water incubation. And the presence of a lead iron oxide phase and the peak increasing of zinc sulfide were observed via XRD analyses. Finally, water incubation restrained the release of heavy metals after 180 days of incubation, and reduced the leachability of Cu, Zn, Cd and Pb by as much as 1.61%–7.21% for soil A and 0.43%–3.36% for soil B, respectively. The study findings have implications for the formulation of risk control and management strategies for heavy metals in smelter-contaminated soils.  相似文献   

4.
Sediments from an arsenic(As) contaminated groundwater vent site were used to investigate As( Ⅲ) binding, transformation and redistribution in native and iron oxide amended lake sediments using aging spiked batch reactions and a sequential extraction procedure that maintains As(V) and As( Ⅲ) speciation. In the native sediments, fractionation analysis revealed that 10% of the spiked As( Ⅲ) remained intact after a 32-day aging experiment and was predominantly adsorbed to the strongly sorbed(NH_4H_2PO_4 extractable) and amorphous Fe oxide bound(H_3PO_4 extractable) fractions. Kinetic modelling of the experimental results allowed identifying the dominant reaction path for depletion of dissolved As( Ⅲ) to As( Ⅲ)absorbed on to the solid phase, followed by oxidation in the solid phase. Arsenite was initially adsorbed primarily to the easily exchangeable fraction((NH_4)_2SO_4 extractable), then rapidly transformed into As(V) and redistributed to the strongly sorbed and amorphous Fe oxide bound fractions. Oxidation of As( Ⅲ) in recalcitrant fractions was less efficient. The iron oxide amendments illustrated the controls that iron oxides can have on As( Ⅲ) binding and transformation rates. In goethite amended samples As( Ⅲ) oxidation was faster and primarily occurred in the strongly sorbed and amorphous Fe oxide bound fractions. In these samples,19.3 μg Mn was redistributed(compared to the native sediment) from the easily exchangeable and crystalline Fe oxide bound fractions to the strongly sorbed and amorphous Fe oxide bound fractions, indicating that goethite may act as a catalyst for Mn(Ⅱ) oxidation, thereby producing sorbed Mn( Ⅲ/Ⅳ ), which then appears to be involved in rapidly oxidizing As( Ⅲ).  相似文献   

5.
Hausmannite is a common low valence Mn oxide mineral, with a distorted spinel structure, in surficial sediments. Although natural Mn oxides often contain various impurities of transitional metals (TMs), few studies have addressed the effect and related mechanism of TM doping on the reactivity of hausmannite with metal pollutants. Here, the reactivity of cobalt (Co) doped hausmannite with aqueous As(III) and As(V) was studied. Co doping decreased the point of zero charge of hausmannite and its adsorption capacity for As(V). Despite a reduction of the initial As(III) oxidation rate, Co-doped hausmannite could effectively oxidize As(III) to As(V), followed by the adsorption and fixation of a large amount of As(V) on the mineral surface. Arsenic K-edge EXAFS analysis of the samples after As(V) adsorption and As(III) oxidation revealed that only As(V) was adsorbed on the mineral surface, with an average As-Mn distance of 3.25–3.30 Å, indicating the formation of bidentate binuclear complexes. These results provide new insights into the interaction mechanism between TMs and low valence Mn oxides and their effect on the geochemical behaviors of metal pollutants.  相似文献   

6.
Arbuscular mycorrhizal fungi (AMF) have great potential for assisting heavy metal hyperaccumulators in the remediation of contaminated soils. However, little information is available about the community composition of AMF under natural conditions in soils contaminated by antimony (Sb). The objective of this study was to investigate the characteristics of AMF molecular diversity, and to explore the effects of Sb content and soil properties on the AMF community structure in an Sb mining area. Four Sb mine spoils and one adjacent reference area were selected from around the Xikuangshan mine in southern China. The association of AMF molecular diversity and community composition with the rhizosphere soils of the dominant plant species was studied by Polymerase Chain Reaction-Denaturing Gradient Gel Electrophoresis (PCR-DGGE). Results from all five studied sites showed that the diversity of AMF decreased with increasing Sb concentration. Principal component analysis (PCA) indicated that the AMF community structure was markedly different among these groups. Further redundancy analysis (RDA) showed that Sb contaminationwas the dominating factor influencing the AMF community structure in the Sb mine area. However, the multivariate analysis showed that, apart from the soil Sb content, extractable nitrogen content and organic matter content also attributed to AMF sequence distribution type. Some AMF sequences were only found in the highly contaminated area and these might be ideal candidates for improving phytoremediation efficiency in Sb mining regions. Gene sequencing analysis revealed that most species were affiliated with Glomus, suggesting that Glomus was the dominant AMF genus in the studied Sb mining area.  相似文献   

7.
The redox-sensitive elements, such as iron, manganese, sulfur, phosphorus, and arsenic, shift their speciation every millimeter (mm) across the soil-water interface in the flooded soil environments. Monitoring of element speciation at this high-resolution (HR) within the SWI is still difficult. The key challenge lies in obtaining sufficient porewater samples at specific locations along the soil gradient for downstream analysis. Here with an optimized inductively coupled plasma mass spectrometry (ICP-MS) method and a HR porewater sampler, we demonstrate mm-scale element profiles mapping across the SWI in paddy soils. High-concentrations of iron and manganese (> 10 mg/L) were measured by ICP-MS in an extended dynamic range mode to avoid signal overflow. The iron profile along the SWI generated by the ICP-MS method showed no significant difference (p < 0.05) compared to that measured independently using a colorimetric method. Furthermore, four arsenic (arsenite, arsenate, monomethylarsonic and dimethylarsinic acid), two phosphorus (phosphite and phosphate) and two sulfur (sulfide and sulfate) species were separated in 10 min by ion chromatography -ICP-MS with the NH4HCO3 mobile phase. We verified the technique using paddy soils collected from the field, and present the mm-scale profiles of iron, manganese, and arsenic, phosphorus, sulfur species (relative standard deviation < 8%). The technique developed in this study will significantly promote the measurement throughput in limited samples (e.g. 100 μL) collected by HR samplers, which would greatly facilitate redox-sensitive elements biogeochemical cycling in saturated soils.  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.
Municipal solid waste(MSW) incineration has become an important anthropogenic source of heavy metals(HMs) to the environment. However, assessing the impact of MSW incineration on HMs in the environment, especially soils, can be a challenging task because of various HM sources. To investigate the effect of MSW incineration on HMs in soils, soil samples collected at different distances from four MSW incinerators in Shanghai, China were analyzed for their contents of eight HMs(antimony, cadmium, chromium, copper,lead, mercury, nickel, and zinc) and lead(Pb) isotope ratios. Source identification and apportionment of HMs were accomplished using principal component analysis and Pb isotope analysis. Results indicated that the relatively high contents of cadmium, lead,antimony, and zinc in the soils at 250 m and 750–1250 m away from the MSW incinerators were related to MSW incineration, while the elevated contents of the other four HMs were associated with other anthropogenic activities. Based on Pb isotope analysis, the contribution ratio of MSW incineration(which had been operated for more than 14 years)to the accumulation of Pb in soil was approximately 10% on average, which was lower than coal combustion only. Incinerator emissions of Pb could have a measurable effect on the soil contamination within a limited area(≤1500 m).  相似文献   

10.
Photolysis of some polycyclic aromatic hydrocarbons (PAHs) on soil surfaces may play an important role in the fate of PAHs in the environment.Photolysis of PAHs on soil surfaces under UV irradiation was investigated.The effects of oxygen,irradiation intensity and soil moisture on the degradation of the three PAHs were observed.The results showed that oxygen,soil moisture and irradiation intensity enhanced the photolysis of the three PAHs on soil surfaces.The degradation of the three PAHs on soil surfaces is related to their absorption spectra and the oxidation-half-wave potential.The photolysis of PAHs on soil surfaces in the presence of oxygen followed pseudo first-order kinetics.The photolysis half-lives ranged from 37.87 days for benzo[a]pyrene to 58.73 days for phenanthrene.The results indicate that photolysis is a successful way to remediate PAHs-contaminated soils.  相似文献   

11.
Heavy metal concentrations in agricultural soils of Zhejiang Province were monitored to indicate the status of heavy metal contamination and assess environmental quality of agricultural soils. A total of 908 soil samples were collected from 38 counties in Zbejiang Province and eight heavy metal (Cd, Cr, Pb, Hg, Cu, Zn, Ni and As) concentrations had been evaluated in agricultural soil. It was found 775 samples were unpolluted and 133 samples were slightly polluted and more respectively, that is approximately 14.65% agricultural soil samples had the heavy metal concentration above the threshold level in this province by means of Nemerow's synthetical pollution index method according to the second grade of Standards for Soil Environmental Quality of China (GB15618- 1995). Contamination of Cd was the highest, followed by Ni, As and Zn were lower correspondingly. Moreover, Inverse Distance Weighted (IDW) interpolation method was used to make an assessment map of soil environmental quality based on the Nemerow's pollution index and the soil environmental quality was categorized into five grades. Moreover, ten indices were calculated as input parameters for principal component analysis (PCA) and the principal components (PCs) were created to compare environmental quality of different soils and regions. The results revealed that environmental quality of tea soils was better than that of paddy soils, vegetable soils and fruit soils. This study indicated that GIS combined with multivariate statistical approaches proved to be effective and powerful tool in the mapping of soil contamination distribution and the assessment of soil environmental quality on provincial scale, which is beneficial to environmental protection and management decision-making by local government.  相似文献   

12.
Oxidation of Cr(Ⅲ) by manganese oxides may pose a potential threat to environments due to the formation of toxic Cr(Ⅵ) species. At present, it was still unclear whether the extent of Cr(Ⅲ) oxidation and fate of Cr(Ⅵ) would be changed when manganese oxides co-exist with other minerals, the case commonly occurring in soils. This study investigated the influence of goethite and kaolinite on Cr(Ⅲ) oxidation by birnessite under acidic p H condition(p H 3.5)and background electrolyte of 0.01 mol/L Na Cl. Goethite was found not to affect Cr(Ⅲ)oxidation, which was interpreted as the result of overwhelming adsorption of cationic Cr(Ⅲ) onto the negatively-charged birnessite(point of zero charge(PZC) 3.0) rather than the positively-charged goethite(PZC = 8.8). However, more Cr(Ⅵ) would be retained by the surface with the increase in addition of goethite because of its strong ability on adsorption of Cr(Ⅵ) at low p H. Moreover, either Cr(Ⅲ) oxidation or distribution of the generated Cr(Ⅵ)between the solid and solution phases was not affected by kaolinite(PZC 3.0), indicating its low affinity for Cr species. Reactions occurring in the present mixed systems were suggested, which could be partly representative of those in the soils and further indicates that the mobility and risk of Cr(Ⅵ) would be decreased if goethite was present.  相似文献   

13.
While the transformation of antimony(Sb) in paddy soil has been previously investigated, the biogeochemical processes of highly chemical active Sb in the soil remain poorly understood. In addition, there is a lack of quantitative understanding of Sb transformation in soil. Therefore, in this study, the kinetics of exogenous Sb in paddy soils were investigated under anaerobic and aerobic incubation conditions. The dissolved Sb(V) and the Sb(V) extracted by diffusive gradient technique decreased u...  相似文献   

14.
Response of soil catalase activity to chromium contamination   总被引:3,自引:0,他引:3  
The impact of chromium(III) and (VI) forms on soil catalase activity was presented. The Orthic Podzol, Haplic Phaeozem and Mollic Gleysol from di erent depths were used in the experiment. The soil samples were amended with solution of Cr(III) using CrCl3, and with Cr(VI) using K2Cr2O7 in the concentration range from 0 to 20 mg/kg, whereas the samples without the addition of chromium served as control. Catalase activity was assayed by one of the commonly used spectrophotometric methods. As it was demonstrated in the experiment, both Cr(III) and Cr(VI) have an ability to reduce soil catalase activity. A chromium dosage of 20 mg/kg caused the inhibition of catalase activity and the corresponding contamination levels ranged from 75% to 92% for Cr(III) and 68% to 76% for Cr(VI), with relation to the control. Catalase activity reached maximum in the soil material from surface layers (0–25 cm), typically characterized by the highest content of organic matter creating favorable conditions for microorganisms.  相似文献   

15.
The spatial variability in the concentrations of 1,2,3,4,5,6-hexachlorocyclohexane (HCH) and 1,1,1-trichloro-2,2-bis-(p-chlorophenyl) ethane (DDT) in surface soils was studied on the basis of the analysis of 131 soil samples collected from the surface layer (0-20 cm depth) of the alluvial region of Beijing, China. The concentrations of total HCHs (including α-, β-, γ-, and δ-isomers) and total DDTs (i ncluding p,p'-DDT, p,p'-DDD, p,p'-DDE, and o,p'-DDT) in the surface soils tested were in the range from nondetectable to 31.72 μg/kg dry soil, with a mean value of 0.91, and from nondetectable to 5910.83 μg/kg dry soil, with a mean value of 32.13,respectively. It was observed that concentrations of HCHs in all soil samples and concentrations of DDTs in 112 soil samples were much lower than the first grade (50 μg/kg) permitted in "Environment quality standard for soils in China (GB15618-1995)". This suggests that the pollution due to organochlorine pesticides was generally not significant in the farmland soils in the Beijing alluvial region. In this study, the spatial distribution and trend of HCHs and DDTs were analyzed using Geostatistical Analyst and GS (513).Spatial distribution indicated how these pesticides had been applied in the past. Trend analysis showed that the concentrations of HCHs,DDTs, and their related metabolites followed an obvious distribution trend in the surface soils from the alluvial region of Beijing.  相似文献   

16.
Sulfate, nitrate and ammonium(SNA) are the dominant species in secondary inorganic aerosol, and are considered an important factor in regional haze formation. Size-fractionated aerosol particles for a whole year were collected to study the size distribution of SNA as well as their chemical species in Shanghai. SNA mainly accumulated in fine particles and the highest average ratio of SNA to particulate matter(PM) was observed to be 47% in the fine size fraction(0.49–0.95 μm). Higher sulfur oxidation ratio and nitrogen oxidation ratio values were observed in PM of fine size less than 0.95 μm. Ion balance calculations indicated that more secondary sulfate and nitrate would be generated in PM of fine size(0.49–0.95 μm). Sulfur K-edge X-ray absorption near-edge structure(XANES) spectra of typical samples were analyzed. Results revealed that sulfur mainly existed as sulfate with a proportion(atomic basis) more than 73% in all size of PM and even higher at 90% in fine particles. Sulfate mainly existed as(NH4)2SO4 and gypsum in PM of Shanghai. Compared to non-haze days, a dramatic increase of(NH4)2SO4 content was found in fine particles on haze days only, which suggested the promoting impact of(NH4)2SO4 on haze formation. According to the result of air mass backward trajectory analysis, more(NH4)2SO4 would be generated during the periods of air mass stagnation. Based on XANES, analysis of sulfate species in size-fractionated aerosol particles can be an effective way to evaluate the impact of sulfate aerosols on regional haze formation.  相似文献   

17.
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   

18.
Hexachlorobenzene (HCB), a persistent organic pollutant (POP), has been found in paddy soils. To improve the understanding of HCB contamination in paddy soils, a laboratory simulative study was carried out to investigate the behavior of HCB in a paddy soil and rice plants. This study was divided into three experiments. First, an experiment aimed to examine the evaporation of HCB in paddy soil. In the second experiment, rice was planted in 10 mg/kg HCB contaminated soil and after pot culture at 3, 6, 9, and 27 weeks (at maturity), both soil and plant samplings were scheduled to be sampled. The soil samples comprised rhizosphere soil, nonrhizosphere soil, and unplanted contaminated soil, whereas plant samples included shoots, roots, and rice grains (dehusked). Lastly, in this part, HCB in xylem saps was designed to be examined. The results showed that (1) the HCB translocation from paddy soil to rice by vaporization; (2) the HCB concentration in rice grains was surprisingly high; (3) the observed HCB decrease in rice rhizosphere offers a potential means for in situ HCB degradation; (4) HCB might not be transported along transpiration in rice.  相似文献   

19.
Antibiotic micro-pollution is usually found at the ng/L–level in drinking water sources or discharge water of wastewater treatment plants. In this study, a novel approach mediated by manganese oxidizing bacteria (MnOB) in a biofilter was developed to control the pollution. The results indicated that the biogenic manganese oxide (MnOx) produced during the oxidation of the feeding manganese ions could coat the surface of the filtering sand effecting the simultaneous removal of antibiotics. It was found that the removal of antibiotics is insured as long as the feeding manganese was well removed and was not influenced by the hydraulic loading. The growth rate of the MnOB group revealed that the antibiotic concentration at 50 and 100 ng/L promoted their activity, but it was inhibited at 500 and 1000 ng/L. The structure of the bacterial community was stable in the presence of antibiotics (50 ng/L), but their extracellular processes changed. The removal performance of the feeding manganese seemed to relate to the extracellular processes of the dominant bacterial genus. Moreover, the freshly formed MnOx was a buserite-like material that was rich in Mn(III) and Mn(IV) (94.1%), favoring the degradation. The biofilter did not generate additional antibiotic resistant genes in the presence of antibiotics.  相似文献   

20.
Arsenic(As) and antimony(Sb) are usually coexistent in mine wastes and pose a great threat to human health. The As immobilization by nano zero-valent iron(n ZVI) is promising, however, the stabilization for co-occurring As and Sb is not known. Herein, the immobilization and transformation of As and Sb in n ZVI-treated sediments were evaluated using complementary leaching experiments and characterization techniques. Raw sediment samples from a gold-antimony deposit revealed the co-existence of ul...  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