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1.
含水层沉积物中含铁矿物的特征与活性会影响砷的迁移转化行为。通过内蒙古含水层沉积物含铁矿物的溶解、还原动力学实验,研究了沉积物含铁矿物特征和活性及其与砷运移的关系。结果表明,沉积物中具还原活性的铁氧化物总量(m0)与岩性有关,细砂为52 μmol/g,黏土为45 μmol/g。初始还原速率k′均在10-5 s-1的数量级。表征活性均匀度的参数γ值介于合成铁氧化物矿物和表层沉积物之间。沉积物中Fe(Ⅲ)氧化物的还原活性主要介于人造纤铁矿与针铁矿的活性水平范围内。沉积物中可能存在两类活性水平不同的Fe(Ⅲ)氧化物。As更倾向于吸附在活性较强的Fe(Ⅲ)氧化物上。还原环境中,活性较强的Fe(Ⅲ)氧化物的还原性溶解,促进了沉积物中砷的释放。  相似文献   

2.
硫酸盐还原菌是厌氧环境中参与砷形态转化的重要微生物种群,其介导的生物地球化学循环过程对铁氧化物表面吸附态砷迁移转化的影响亟待深入研究.选取江汉平原典型高砷含水层原位沉积物分离纯化出一株严格厌氧硫酸盐还原菌Desulfovibrio JH-S1,对其进行砷和铁还原能力鉴定,并通过模拟培养实验探究硫酸盐还原菌参与下的铁矿物相转化对吸附态砷迁移的影响.Desulfovibrio JH-S1具有Fe(III)还原能力,无硫和有硫体系中Fe(III)均能被还原,但在硫酸盐充足条件下铁还原量显著增加;该菌株不具备As(V)还原能力,但添加硫酸盐的培养体系中As(V)去除率可达96%以上.Desulfovibrio JH-S1能够还原硫酸盐从而促进载砷的水铁矿还原转化为纤铁矿,并导致吸附的砷释放.江汉平原高砷含水层土著硫酸盐还原菌兼具硫酸盐/铁还原功能,参与了高砷含水层系统中砷-铁-硫耦合循环,对高砷地下水的形成具有重要作用.   相似文献   

3.
微生物参与铁氧化物矿物的还原性溶解是高砷地下水形成的关键过程,其中具有砷还原功能的微生物如何参与含水层砷释放的生物地球化学过程亟待研究.利用从江汉平原典型高砷含水层中厌氧条件下分离出的四株细菌(Citrobacter sp.JH-1、Clostridium sp.JH-6、Exiguobacterium sp.JH-13、Paenibacillus sp.JH-33),通过室内厌氧模拟培养实验,查明其砷、铁还原能力,并通过分别与铁氧化物矿物及原位沉积物共同培养,探究原位含水层微生物参与的砷释放机理.结果表明:四株细菌均具有厌氧条件下砷、铁还原功能,Citrobacter sp.JH-1砷还原能力最强,96 h内还原的As(Ⅴ)浓度为2.22 μmol/L.其中Citrobacter sp.JH-1不仅可在厌氧和有氧条件下还原溶液中的As(Ⅴ),还可在厌氧条件下还原溶液中的Fe(Ⅲ)和无定型的水铁矿,在与含水层沉积物共培养12 d后,沉积物中铁与砷的释放量分别为510 mg/kg及1 150 μg/kg.江汉平原含水层中的原位微生物兼具砷/铁还原功能,在厌氧条件下可还原沉积物中的铁氧化物矿物并促进砷的释放,为深入揭示高砷地下水成因机理与地下水砷污染的防控提供重要科学依据.   相似文献   

4.
高铁高砷地下水严重威胁饮水质量,曝气-砂滤法因处理效果好且成本低在农村地区得到广泛应用。砂滤过程石英砂表面富集铁和砷后需定期更换,然而废弃石英砂堆置具有砷释放风险。本文以江汉平原某水厂砂滤池废弃石英砂为研究对象,采用激光剥蚀-等离子体质谱(LA-ICP-MS)、拉曼光谱(Raman)、X射线衍射(XRD)和分步化学提取等手段,研究了砂样中的Fe和As含量及形态分布。结果表明,砂粒表面形成了一层厚度为20100 μm的高铁砷薄层,薄层内部Fe和As含量显著高于两侧,Fe和As分布高度相关(R2=0.985)。砂样表面铁矿物以无定型/弱结晶型为主,同时检出赤铁矿和臭葱石等矿物。砂样中Fe和As总含量分别为20.1 mg/g和53.4 μg/g。砂样表面铁主要以易溶解态、碳酸盐结合态和易还原态为主,As主要吸附在铁矿物上。研究区降雨充沛,当废弃石英砂遭遇雨水冲刷或淹没时,可能导致铁砷薄层中As解吸或随Fe矿物还原溶解而释放。  相似文献   

5.
鹿帅  苏小四  冯晓语  孙超 《地学前缘》2022,29(4):455-467
沈阳黄家水源地是我国北方地区典型的傍河地下水水源地,近岸带地下水中铁(Fe)、锰(Mn)、砷(As)含量严重超标。为查明地下水中As的来源与影响因素,对研究区河水、地下水以及土壤样品进行采集与测试,分析了水样常规指标与碳硫稳定同位素、土样中典型矿物、砷的含量及赋存形态。结果表明,研究区河水中As含量很低,而地下水中As含量普遍超标。河水入渗初期,氧化性河水使部分含As矿物发生氧化而释放As;随着河水入渗,地下水向还原环境转变,含As的Fe/Mn矿物发生还原性溶解,地下水中As含量逐渐升高。研究区典型矿物有黄铁矿、菱铁矿、软锰矿、赤铁矿、针铁矿、菱锰矿等,通过可交换态砷解吸、有机质结合态砷氧化、铁锰氧化物结合态砷还原性溶解等,介质中的As释放至地下水中。地下水中As含量与酸碱度(pH)、氧化还原电位(Eh)呈一定负相关,与溶解有机碳(DOC)、 HCO 3 -、Fe、Mn含量呈正相关。  相似文献   

6.
砷是土壤中重要的(类)重金属污染物,其毒性主要取决于在环境中的形态及氧化还原状态。游离态Fe(Ⅱ)(Fe(Ⅱ)_(aq))驱动铁(氢)氧化物晶相重组过程是土壤铁循环的重要组成,对土壤中重金属的吸附、固定、钝化等环境行为有重要影响。本研究采用~(57)Fe稳定同位素示踪方法研究厌氧条件下Fe(Ⅱ)_(aq)驱动针铁矿晶相重组过程中砷的氧化还原及形态变化过程。结果显示,在只有针铁矿存在的对照处理中,针铁矿本身对As(Ⅲ)没有氧化作用,但83%的As(Ⅲ)被吸附到针铁矿表面。在Fe(Ⅱ)_(aq)和针铁矿共存体系中,Fe(Ⅱ)_(aq)可与针铁矿中结构态Fe(Ⅲ)发生铁原子交换,As(Ⅲ)的存在降低了铁原子交换速率。同时,在Fe(Ⅱ)_(aq)驱动针铁矿晶相转化过程中,77%的As(Ⅲ)被氧化成As(Ⅴ),As活性降低。另外,部分吸附在针铁矿表面的As(Ⅲ)和氧化转化后的As(Ⅴ)通过针铁矿的晶格单元包裹或取代Fe结构位的形式被针铁矿结构化固定,从而进一步降低了As的活性。  相似文献   

7.
高砷含水层沉积物矿物学特征及砷的活化   总被引：2，自引：0，他引：2  
利用X射线衍射和X射线荧光分析、沉积物序列提取试验及矿物饱和度的计算,对采自江汉平原中部沙湖地区典型高砷含水层钻孔沉积物样品矿物学进行了分析,并讨论了控制含水层中砷释放和迁移的地球化学机制.对矿物在沉积物与土壤中的分布及组成的对比分析,在一定程度上指示了矿物赋存环境和/或高砷水形成的环境背景:土壤与沉积物中高岭石以低于其他3种粘土矿物的含量普遍存在,指示了含水层沉积物形成过程江汉平原存在一定的湿热古气候环境;沉积物绿泥石含量低于土壤中绿泥石,恰恰反映了土壤比沉积物略强的碱性环境;沉积物中黄铁矿的存在,显示了含水层局部的强还原性环境,指示地下水中广泛存在的Fe2+容易与二价硫发生沉淀并结合砷.砷主要以无定形铁锰氧化物结合态(平均在31％以上)形式存在,其次以碳酸盐和有机质结合态存在.无定形铁锰氧化物的还原溶解可能是控制砷迁移到地下水中主要的地球化学机制.相对高含量的绿泥石容易在含水层中发生风化,其溶解过程可以将铁释放到地下水中,从而成为影响地下水中砷活化的潜在因素.  相似文献   

8.
利用X射线吸收精细结构分析(XAFS)和铁的穆斯堡尔谱(Mossbauer)对黔西南高砷煤中砷和铁的存在形式进行了研究.研究发现,高砷煤中的砷主要以高价砷的形式存在,也有少量以As2O3、砷黄铁矿、砷硫化物的形式存在.除1个样品中的铁全部以顺磁性针铁矿或超顺磁性的针铁矿的形式存在外,其它样品中的Fe主要是黄铁矿中的Fe,约占全铁的60%～91%;其次是黄铁钾矾中的Fe,约占全铁的9%～40%.  相似文献   

9.
为了研究厌氧微生物作用下沉积物中砷的形态转化及固液界面的分配过程对砷的环境行为与归趋的影响,通过采集锦州湾清洁沉积物进行负载砷,利用微生物培养与非生物培养实验,对比研究厌氧微生物作用下砷铁硫共还原条件下污染体系中砷的环境行为与归趋。实验结果表明在培养的42 d周期内,液相的总砷量首先砷浓度保持降低趋势,而后再次升高。在培养第3~7 d时液相的As5+迅速被还原,约26%的溶解态砷从液相移除,97%以上的As5+被还原为As3+。同时微生物作用下固相中90%以上铁氧化物矿物逐渐转化为次生的亚铁矿物,固相中结晶态铁氧化物发生明显活化,而硫酸盐还原产物硫离子综合调控体系中游离的亚铁离子和As3+。因此,厌氧微生物还原条件下,砷,铁,硫同步发生还原,硫离子调控体系中砷和铁环境行为,硫化亚铁成为亚铁矿物的主要形态,硫化砷是砷的主要归趋。  相似文献   

10.
采集缺氧活性污泥进行室内微生物驯化,培养耐砷反硝化菌。把耐砷反硝化菌、营养液和吸附As(V)的水铁矿在厌氧条件下培养,研究反硝化菌代谢作用下,系统中Fe、Mn、NO3-和As形态的动态变化。结果表明,缺氧活性污泥中的反硝化菌具有一定的耐砷能力。在砷含量500μg/L以内,其反硝化强度基本不受砷的影响。在吸附有砷的水铁矿体系中,反硝化菌所产生的反硝化作用可导致溶液中NO3-含量的降低、Fe含量的升高、As含量降低,且As(III)所占比例增加。这说明,体系中水铁矿的还原性溶解和As(V)的还原性解吸已经发生。As含量降低的原因是,在培养体系中水铁矿的含量高,Fe的释放量只占很小比例,表层水铁矿被还原后,在次表层形成新的水铁矿吸附位,这种新吸附位不仅可以吸附溶液中已经存在的As,而且能够再吸附由于还原性溶解和解吸所释放出的As。  相似文献   

11.
Fe released into solution is isotopically lighter (enriched in the lighter isotope) than hornblende starting material when dissolution occurs in the presence of the siderophore desferrioxamine mesylate (DFAM). In contrast, Fe released from goethite dissolving in the presence of DFAM is isotopically unchanged. Furthermore, Δ56Fesolution-hornblende for Fe released to solution in the presence of ligands varies with the affinity of the ligand for Fe. The extent of isotopic fractionation of Fe released from hornblende also increases when experiments are agitated continuously. The Fe isotope fractionation observed during hornblende dissolution with organic ligands is attributed predominantly to retention of 56Fe in an altered surface layer, while the lack of isotopic fractionation during goethite dissolution in DFAM is consistent with the lack of an altered layer. When a siderophore-producing soil bacterium is added to the system (without added organic ligands), Fe released to solution from both hornblende and goethite differs isotopically from Fe in the bulk mineral: Δ56Fesolution-starting material = −0.56 ± 0.19 (hornblende) and −1.44 ± 0.16 (goethite). Increased isotopic fractionation is attributed in this case to the fact that as bacterial respiration depletes the system in oxygen and aqueous Fe is reduced, equilibration between aqueous ferrous and ferric iron creates a pool of isotopically heavy ferric iron that is assimilated by bacterial cells. Adsorption of isotopically heavy ferrous iron (Fe(II) enriched in the heavier isotope) or precipitation of isotopically heavy Fe minerals may also contribute to observed fractionations.To test whether these Fe isotope signatures are recorded in natural systems, we also investigated extractions of samples of soils from which the bacteria were isolated. These extractions show variability in the isotopic signatures of exchangeable Fe and Fe oxyhydroxide fractions from one soil sample to another, but exchangeable Fe is observed to be lighter than Fe in soil Fe oxyhydroxides and hornblende. This observation is consistent with isotopically light Fe-organic complexes in soil pore water derived from the Fe-silicate starting materials in the presence of growing microorganisms, as documented in experiments reported here. The contributions from phenomena including organic ligand-promoted nonstoichiometric dissolution of Fe silicates, uptake of ferric iron by organisms, adsorption of isotopically heavy ferrous iron, and precipitation of iron minerals should create complex isotopic signatures in soils. Better understanding of these processes and the timescales over which they contribute to fractionation is needed.  相似文献   

12.
High As contents in groundwater were found in Rayen area and chosen for a detailed hydrogeochemical study. A total of 121 groundwater samples were collected from existing tube wells in the study areas in January 2012 and analyzed. Hydrogeochemical data of samples suggested that the groundwater is mostly Na–Cl type; also nearly 25.62 % of samples have arsenic concentrations above WHO permissible value (10 μg/l) for drinking waters with maximum concentration of aqueous arsenic up to 25,000 μg/l. The reducing conditions prevailing in the area and high arsenic concentration correlated with high bicarbonate and pH. Results show that arsenic is released into groundwater by two major phenomena: (1) through reduction of arsenic-bearing iron oxides/oxyhydroxides and Fe may be precipitated as iron sulfide when anoxic conditions prevail in the aquifer sediments and (2) transferring of As into the water system during water–acidic volcanic rock interactions.  相似文献   

13.
Cronobacter sakazakii还原作用对针铁矿晶体结构的影响   总被引：1，自引：0，他引：1  
厌氧条件下,Cronobacter sakazakii以乙酸钠作为电子供体,针铁矿中Fe(Ⅲ)作为电子受体进行生命活动,其新陈代谢过程伴随Fe(Ⅲ)的还原。细菌增殖和稳定生长过程中不停还原针铁矿并大量累积Fe(Ⅱ);当细菌衰亡时,Fe(Ⅱ)的产生随之减缓;细菌的活动停止时,Fe(Ⅱ)不再积累并最终保持稳定。同步辐射XRD测试表明,微生物还原作用后针铁矿出现了一系列新衍射峰：4.8、6.03、6.13、6.84、7.7和11.4 峰,可能形成具层状结构的新物相。在XANES图谱中Fe主吸收峰向低能量方向移动1 eV,边前峰峰位中心向低能量方向移动且峰面积减小,表明Cronobacter sakazakii的异化Fe(Ⅲ)还原作用使针铁矿中Fe氧化态降低,矿物晶体结构发生了变化。  相似文献   

14.
Due to the strong reducing capacity of ferrous Fe, the fate of Fe(II) following dissimilatory iron reduction will have a profound bearing on biogeochemical cycles. We have previously observed the rapid and near complete conversion of 2-line ferrihydrite to goethite (minor phase) and magnetite (major phase) under advective flow in an organic carbon-rich artificial groundwater medium. Yet, in many mineralogically mature environments, well-ordered iron (hydr)oxide phases dominate and may therefore control the extent and rate of Fe(III) reduction. Accordingly, here we compare the reducing capacity and Fe(II) sequestration mechanisms of goethite and hematite to 2-line ferrihydrite under advective flow within a medium mimicking that of natural groundwater supplemented with organic carbon. Introduction of dissolved organic carbon upon flow initiation results in the onset of dissimilatory iron reduction of all three Fe phases (2-line ferrihydrite, goethite, and hematite). While the initial surface area normalized rates are similar (∼10−11 mol Fe(II) m−2 g−1), the total amount of Fe(III) reduced over time along with the mechanisms and extent of Fe(II) sequestration differ among the three iron (hydr)oxide substrates. Following 16 d of reaction, the amount of Fe(III) reduced within the ferrihydrite, goethite, and hematite columns is 25, 5, and 1%, respectively. While 83% of the Fe(II) produced in the ferrihydrite system is retained within the solid-phase, merely 17% is retained within both the goethite and hematite columns. Magnetite precipitation is responsible for the majority of Fe(II) sequestration within ferrihydrite, yet magnetite was not detected in either the goethite or hematite systems. Instead, Fe(II) may be sequestered as localized spinel-like (magnetite) domains within surface hydrated layers (ca. 1 nm thick) on goethite and hematite or by electron delocalization within the bulk phase. The decreased solubility of goethite and hematite relative to ferrihydrite, resulting in lower Fe(III)aq and bacterially-generated Fe(II)aq concentrations, may hinder magnetite precipitation beyond mere surface reorganization into nanometer-sized, spinel-like domains. Nevertheless, following an initial, more rapid reduction period, the three Fe (hydr)oxides support similar aqueous ferrous iron concentrations, bacterial populations, and microbial Fe(III) reduction rates. A decline in microbial reduction rates and further Fe(II) retention in the solid-phase correlates with the initial degree of phase disorder (high energy sites). As such, sustained microbial reduction of 2-line ferrihydrite, goethite, and hematite appears to be controlled, in large part, by changes in surface reactivity (energy), which is influenced by microbial reduction and secondary Fe(II) sequestration processes regardless of structural order (crystallinity) and surface area.  相似文献   

15.
The arsenic accumulation process in intertidal sediments of Iriomote Island, Japan, is analyzed as a naturally balanced arsenic-fixation system. Major and minor element chemistry is analyzed by X-ray fluorescence photometry, mineralogy is investigated by X-ray diffractometry, and four arsenic compounds are characterized by hydrogen-generated atomic absorption photometry. It is found that arsenic is accumulated by iron hydroxides/oxides precipitated following the decomposition of humic acids in the shallower sediment, and is subsequently incorporated into iron sulfide minerals at depth. The arsenic is immobile during incorporation into arsenic-bearing phases, suggesting that arsenic is unlikely to be released into the porewater under natural conditions in early diagenesis. The formation and decomposition of arsenic-bearing organic compounds appear to be associated with the formation and decomposition of arsenic in oxyhydroxides/oxides, suggesting that microbial activity may play an important role in controlling the behavior of arsenic and arsenic-bearing phases in the sediment column.  相似文献   

16.
Iron (hydr)oxides not only serve as potent sorbents and repositories for nutrients and contaminants but also provide a terminal electron acceptor for microbial respiration. The microbial reduction of Fe (hydr)oxides and the subsequent secondary solid-phase transformations will, therefore, have a profound influence on the biogeochemical cycling of Fe as well as associated metals. Here we elucidate the pathways and mechanisms of secondary mineralization during dissimilatory iron reduction by a common iron-reducing bacterium, Shewanella putrefaciens (strain CN32), of 2-line ferrihydrite under advective flow conditions. Secondary mineralization of ferrihydrite occurs via a coupled, biotic-abiotic pathway primarily resulting in the production of magnetite and goethite with minor amounts of green rust. Operating mineralization pathways are driven by competing abiotic reactions of bacterially generated ferrous iron with the ferrihydrite surface. Subsequent to the initial sorption of ferrous iron on ferrihydrite, goethite (via dissolution/reprecipitation) and/or magnetite (via solid-state conversion) precipitation ensues resulting in the spatial coupling of both goethite and magnetite with the ferrihydrite surface. The distribution of goethite and magnetite within the column is dictated, in large part, by flow-induced ferrous Fe profiles. While goethite precipitation occurs over a large Fe(II) concentration range, magnetite accumulation is only observed at concentrations exceeding 0.3 mmol/L (equivalent to 0.5 mmol Fe[II]/g ferrihydrite) following 16 d of reaction. Consequently, transport-regulated ferrous Fe profiles result in a progression of magnetite levels downgradient within the column. Declining microbial reduction over time results in lower Fe(II) concentrations and a subsequent shift in magnetite precipitation mechanisms from nucleation to crystal growth. While the initial precipitation rate of goethite exceeds that of magnetite, continued growth is inhibited by magnetite formation, potentially a result of lower Fe(III) activity. Conversely, the presence of lower initial Fe(II) concentrations followed by higher concentrations promotes goethite accumulation and inhibits magnetite precipitation even when Fe(II) concentrations later increase, thus revealing the importance of both the rate of Fe(II) generation and flow-induced Fe(II) profiles. As such, the operating secondary mineralization pathways following reductive dissolution of ferrihydrite at a given pH are governed principally by flow-regulated Fe(II) concentration, which drives mineral precipitation kinetics and selection of competing mineral pathways.  相似文献   

17.
A <2.0-mm fraction of a mineralogically complex subsurface sediment containing goethite and Fe(II)/Fe(III) phyllosilicates was incubated with Shewanella putrefaciens (strain CN32) and lactate at circumneutral pH under anoxic conditions to investigate electron acceptor preference and the nature of the resulting biogenic Fe(II) fraction. Anthraquinone-2,6-disulfonate (AQDS), an electron shuttle, was included in select treatments to enhance bioreduction and subsequent biomineralization. The sediment was highly aggregated and contained two distinct clast populations: (i) a highly weathered one with “sponge-like” internal porosity, large mineral crystallites, and Fe-containing micas, and (ii) a dense, compact one with fine-textured Fe-containing illite and nano-sized goethite, as revealed by various forms of electron microscopic analyses. Approximately 10-15% of the Fe(III)TOT was bioreduced by CN32 over 60 d in media without AQDS, whereas 24% and 35% of the Fe(III)TOT was bioreduced by CN32 after 40 and 95 d in media with AQDS. Little or no Fe2+, Mn, Si, Al, and Mg were evident in aqueous filtrates after reductive incubation. Mössbauer measurements on the bioreduced sediments indicated that both goethite and phyllosilicate Fe(III) were partly reduced without bacterial preference. Goethite was more extensively reduced in the presence of AQDS whereas phyllosilicate Fe(III) reduction was not influenced by AQDS. Biogenic Fe(II) resulting from phyllosilicate Fe(III) reduction remained in a layer-silicate environment that displayed enhanced solubility in weak acid. The mineralogic nature of the goethite biotransformation product was not determined. Chemical and cryogenic Mössbauer measurements, however, indicated that the transformation product was not siderite, green rust, magnetite, Fe(OH)2, or Fe(II) adsorbed on phyllosilicate or bacterial surfaces. Several lines of evidence suggested that biogenic Fe(II) existed as surface associated phase on the residual goethite, and/or as a Fe(II)-Al coprecipitate. Sediment aggregation and mineral physical and/or chemical factors were demonstrated to play a major role on the nature and location of the biotransformation reaction and its products.  相似文献   

18.
灌溉等人为活动会造成外源物质的输入,如硝酸盐、有机质等,从而引起浅层地下水环境发生周期性波动。为研究农业灌溉对沉积含水层中碘迁移富集过程的影响,选取代表性富碘沉积物,通过室内实验模拟了灌溉活动外源物质输入条件下,盆地地下水系统中碘迁移释放的（生物）地球化学过程。实验结果表明：厌氧条件下,外源有机质输入可促使微生物利用有机质作为电子供体,还原固相铁矿物相,进而造成搭载于铁氧化物/氢氧化物表面的碘释放,以碘离子形式在地下水中富集;而在NO3-输入情况下,微生物会优先利用NO3-为电子受体,至硝酸盐被全部消耗后,Fe（Ⅲ）可进一步被还原为Fe（Ⅱ）。研究结果表明,人为活动造成浅表环境外源物质的输入可直接影响浅层地下水中碘的迁移释放过程。伊利石黏土矿物吸附的铁氧化物矿物相可能为浅层环境中碘的主要搭载介质,微生物作用下,铁氧化物/氢氧化物的还原溶解是高碘地下水形成的主控因素。  相似文献   

19.
The behaviour of trace amounts of arsenate coprecipitated with ferrihydrite, lepidocrocite and goethite was studied during reductive dissolution and phase transformation of the iron oxides using [55Fe]- and [73As]-labelled iron oxides. The As/Fe molar ratio ranged from 0 to 0.005 for ferrihydrite and lepidocrocite and from 0 to 0.001 for goethite. For ferrihydrite and lepidocrocite, all the arsenate remained associated with the surface, whereas for goethite only 30% of the arsenate was desorbable. The rate of reductive dissolution in 10 mM ascorbic acid was unaffected by the presence of arsenate for any of the iron oxides and the arsenate was not reduced to arsenite by ascorbic acid. During reductive dissolution of the iron oxides, arsenate was released incongruently with Fe2+ for all the iron oxides. For ferrihydrite and goethite, the arsenate remained adsorbed to the surface and was not released until the surface area became too small to adsorb all the arsenate. In contrast, arsenate preferentially desorbs from the surface of lepidocrocite. During Fe2+ catalysed transformation of ferrihydrite and lepidocrocite, arsenate became bound more strongly to the product phases. X-ray diffractograms showed that ferrihydrite was transformed into lepidocrocite, goethite and magnetite whereas lepidocrocite either remained untransformed or was transformed into magnetite. The rate of recrystallization of ferrihydrite was not affected by the presence of arsenate. The results presented here imply that during reductive dissolution of iron oxides in natural sediments there will be no simple correlation between the release of arsenate and Fe2+. Recrystallization of the more reactive iron oxides into more crystalline phases, induced by the appearance of Fe2+ in anoxic aquifers, may be an important trapping mechanism for arsenic.  相似文献   

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