流速及介质粒径对As(Ⅲ)迁移影响的实验研究

为了解潜流带中地下水流速和介质颗粒对As（Ⅲ）迁移的影响,选用天然河砂为介质,配制地下水含As（Ⅲ）模拟液,开展室内批实验和动态柱实验并进行表征分析,探讨流速和介质粒径对As（Ⅲ）迁移的影响及机制.结果发现：（1）粒径越小的河砂与As（Ⅲ）相互作用平衡时间越长,As（Ⅲ）的单位吸附量（Qe）随着河砂粒径的增大而减小（0.15～0.18 mm的粒径河砂除外）,单层最大吸附量（Qm）随着粒径的增大呈减小趋势;（2）As（Ⅲ）在河砂上的迁移行为表现出明显的粒径和流速效应;一方面,河砂粒径越小,比表面积越大,增加了水-砂相互作用时间和限制了地下水冲洗速度,不利于As（Ⅲ）在河砂中的迁移;另一方面,流速越大导致空隙通道内的水力剪切力增强,紊流强度的提高减小了滞留边界层厚度,利于As（Ⅲ）在河砂中的迁移.     

江汉平原浅层含水层中土著硫酸盐还原菌对砷迁移释放的影响

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.      

微生物对砷的地球化学行为的影响--暨地下水砷污染机制的最新研究进展

砷在自然界中广泛存在,近年来砷污染对人类健康造成的危害越来越引人关注。微生物在自然界中长期与砷共存,进化出不同的生物转化机制,在自然水体中微生物主要参与砷的不同氧化价态之间的转化过程,即As(V)和As(III)之间的氧化还原作用。砷酸盐异化还原菌（Dissimilatory Arsenate Respiring Prokaryote, DARP）可以将As(V)还原为As(III),化能自养亚砷酸盐氧化菌（Chemoautotrophic Arsenite Oxidizer, CAO）和异养亚砷酸盐氧化菌（Heterotrophic Arsenite Oxidizer, HAO）可以将As(III)氧化为As(V)。这些砷代谢微生物在分类和代谢能力上都具有很大的多样性,它们广泛参与了砷的生物地球化学循环的关键步骤,对特定环境条件下砷的地球化学行为产生重要影响,进而参与了砷的全球循环。在盐碱湖莫诺（Mono）湖中砷的不同价态分层存在,CAO与DARP的紧密偶联共同参与了莫诺湖中的砷的地球化学循环。在孟加拉三角洲的地下含水层中,微生物参与了将砷从固相迁移到水相的关键步骤,最终导致了地下水中的砷污染。     

地下水流动对砷迁移的影响: 大同盆地试验场的观测与模拟

地下水流动特征对水文地球化学特征具有重要控制作用, 研究分析了大同盆地地下水流动特征对高砷水迁移的影响.以山阴县桑干河南岸地下水试验场(SYFS)的监测数据为基础, 建立了河岸带三维非稳定地下水流模型.结果表明, 灌溉在很大程度上影响着地下水位动态变化.灌溉活动减慢了地下水埋深和水平地下水流速, 加速了不同岩性地层之间的垂向水量交换.粉土(L1、L2、L3和L4)、粘土1(L5)和砂1(L6)之间始终存在由上至下的垂向水量交换, 粘土2(L7)、砂2(L8)、粘土3(L9)和砂3(L10)以水平水量交换为主.灌溉水和大气降水从地表向下垂直入渗至含水层的过程中, 推动了地表和包气带沉积物中的砷逐渐向下迁移; 到达含水层后, 水平交换量占主导, 地下水在水平方向上频繁的水量交换促使As在含水层中发生水平迁移.      

土著微生物参与下河套平原地下水中砷的还原作用

为查明土著微生物活动对高砷地下水形成的影响,利用河套平原高砷地下水中分离出的土著微生物(YH002)进行了微宇宙实验研究.实验结果表明: 高砷地下水中加入的葡萄糖提供了微生物生长所需要的碳源,微生物大量繁殖,分泌的有机酸使溶液的pH值降低.在缺氧条件下,溶液中的OD值最高达到了0.189,pH值最低为6.22;在有氧条件下,OD值最高达到了0.286,pH值最低为6.04.溶液中As(III)的初始质量浓度为74 μg/L,占总砷质量浓度的11.2%,在加入微生物和葡萄糖后,在缺氧和有氧条件下,As(III)的质量浓度分别为278 μg/L和310 μg/L,占总砷质量浓度的42%和47%.微宇宙实验说明地下水中的土著微生物能将As(V)还原成As(III).      

氧化还原动态变化对沉积物砷和氟释放的影响:以河北白洋淀平原为例

季风性波动引起的降雨、径流和排泄过程会引发浅层地下水系统周期性氧化还原动态变化,从而对地下水系统中有害组分的迁移转化产生影响。为探讨氧化还原动态过程对沉积物中砷(As)和氟(F)释放的影响,本研究选择河北白洋淀地区沉积物样品,利用发酵罐作为反应器,建立氧化还原动态实验体系,并监测动态变化过程中实验体系各组分含量的变化。结果表明,碱性和还原环境均有利于地下水中As、F的富集。还原阶段较高的pH条件有利于溶液中F^-的解吸,且体系中有机物降解会产生大量HC0₃^-和C0₃^2-,与F^-发生竞争吸附而有利于F^-的富集。对于溶液中As的富集,一方面是由于还原条件下体系中的As以As(III)为主,受沉积物的吸附作用较弱,从而有利于As被释放到溶液中;另一方面是因为还原阶段较高的pH也会使反应体系中As和沉积物间的吸附作用被减弱,造成As的解吸附。由于实验所用沉积物砷含量较低,不同S0₄^2-浓度条件对氧化还原动态过程中As、F迁移的影响不明显。总之,氧化还原动态变化过程会强烈影响地下水系统中砷、氟的富集。     

地下水氮循环与砷迁移转化耦合的研究现状和趋势

地下水中铵根、砷、溶解铁的共存是一个普遍现象。它们之间发生强烈的相互作用,并影响地下水系统的氮循环和砷迁移转化。文章在系统总结地下水氮循环过程及影响因素、地下水氮循环功能微生物及特征、地下水砷富集的水文地球化学过程等国内外研究现状的基础上,深入分析了地下水系统中的氮循环过程（硝化、反硝化、铁铵氧化、厌氧铵氧化、硝酸根异化还原产铵等）对地下水砷迁移转化的影响,总结出含水层中铁氧化物和溶解态Fe(II)的动态转化是氮循环影响地下水中砷迁移转化的重要桥梁。据此提出不同氧化还原环境的含水层中氮循环过程、地下水氮循环与砷迁移转化耦合机理、Fe(III)-Fe(II)的循环-地下水氮循环-砷迁移转化之间的相互作用过程、地表水-地下水相互作用带氮-铁-砷的循环过程及其对人类活动的响应等是今后该领域需要关注的重要科学问题和主要发展趋势。这些科学问题的解决不仅有利于识别地下水中氮的来源和迁移转化,而且有利于提高对高砷地下水富集机理的整体认识。     

江汉平原高砷地下水中DOM三维荧光特征及其指示意义

水体中溶解性有机质(dissolved organic matter, DOM)是含水层中砷释放的主控因素之一.江汉平原河湖众多、沟渠广布,地表水体与浅层地下水的交互作用使得DOM的组分特征及其强度有显著差异.为查明江汉平原地下水中溶解性有机质在砷迁移转化过程中的作用,对江汉平原地表水和浅层地下水进行三维荧光光谱分析,使用平行因子分析法提取水体中有机质的分子组成、功能特点和荧光特征,并分析各组分相对含量与地下水中砷与铁的关联.江汉平原水体中DOM包括3种主要组分,组分C1、C2为类腐殖质,C2是生物降解过程中产生的小分子,C3为类蛋白物质.地下水DOM以类腐殖质组分C1、C2为主,地表水以类蛋白类物质C3和小分子腐殖质C2为主.高砷地下水中DOM以陆源为主,主要通过两种途径促进As的迁移转化:(1) DOM的腐殖质组分充当微生物群落的电子运输工具,促进微生物作用下的有机质氧化和铁氧化物的还原,并伴随As的释放及大量溶解性有机碳(dissolved organic carbon, DOC)和HCO₃-的产生;(2) As以铁等金属阳离子为桥接物与腐殖质结合,通过形成As-Fe-DOM络合物,导致地下水中砷的迁移.      

反硝化菌的耐砷驯化及其对水铁矿吸附态砷迁移转化的影响

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。     

纳米锌去除水体中As(Ⅲ)吸附动力学和影响因素

As(Ⅲ)毒性高,易迁移,且是厌氧条件下地下水中主要存在形式。纳米铁颗粒在含砷水体处理中受到广泛关注,而锌具有比铁更低的氧化还原电位且更易保存,被认为是用于氯代有机化合物还原的最佳金属,但有关纳米锌用于水体中砷的研究很少。本文研究了纳米锌吸附As(Ⅲ)的反应动力学性质和吸附As(Ⅲ)的主要影响因素。通过应用准一级动力学、准二级动力学和粒内扩散三种模型对吸附过程进行模拟,结果显示纳米锌吸附As(Ⅲ)的过程更符合二级反应动力学模型,速率常数k₂为0.18 g/(mg·min),吸附量为0.47 mg/g,且去除机理以化学吸附为主。批实验结果表明,纳米锌对As(Ⅲ)吸附最佳条件为:振荡时间120 min,纳米锌投加量2.5 g/L,pH值2~7。在最佳实验条件下,纳米锌对起始浓度为0.565 mg/L As(Ⅲ)和0.568 mg/L As(Ⅴ)进行吸附试验,As(Ⅲ)和As(Ⅴ)的去除率均能达到99.5%以上,表明纳米锌对As(Ⅲ)和As(Ⅴ)都有很好的去除效果,可作为处理水体中砷的吸附材料之一。以纳米锌作为吸附材料与传统方法相比,并不需要将As(Ⅲ)预氧化成As(Ⅴ),在实际应用中可简化水处理程序,节约处理成本。     

Arsenic repartitioning during biogenic sulfidization and transformation of ferrihydrite

Iron (hydr)oxides are strong sorbents of arsenic (As) that undergo reductive dissolution and transformation upon reaction with dissolved sulfide. Here we examine the transformation and dissolution of As-bearing ferrihydrite and subsequent As repartitioning amongst secondary phases during biotic sulfate reduction. Columns initially containing As(V)-ferrihydrite coated sand, inoculated with the sulfate reducing bacteria Desulfovibrio vulgaris (Hildenborough), were eluted with artificial groundwater containing sulfate and lactate. Rapid and consistent sulfate reduction coupled with lactate oxidation is observed at low As(V) loading (10% of the adsorption maximum). The dominant Fe solid phase transformation products at low As loading include amorphous FeS within the zone of sulfate reduction (near the inlet of the column) and magnetite downstream where Fe(II)_(aq) concentrations increase; As is displaced from the zone of sulfidogenesis and Fe(III)_(s) depletion. At high As(V) loading (50% of the adsorption maximum), sulfate reduction and lactate oxidation are initially slow but gradually increase over time, and all As(V) is reduced to As(III) by the end of experimentation. With the higher As loading, green rust(s), as opposed to magnetite, is a dominant Fe solid phase product. Independent of loading, As is strongly associated with magnetite and residual ferrihydrite, while being excluded from green rust and iron sulfide. Our observations illustrate that sulfidogenesis occurring in proximity with Fe (hydr)oxides induce Fe solid phase transformation and changes in As partitioning; formation of As sulfide minerals, in particular, is inhibited by reactive Fe(III) or Fe(II) either through sulfide oxidation or complexation.     

Stabilization of Fe/Cu nanoparticles by starch and efficiency of arsenic adsorption from aqueous solutions

Due to the severity of arsenic contamination of soil and water resources around the world, finding new adsorbents for arsenic removal from the water is of high importance. The present study investigates the possible use and effectiveness of starch-stabilized Fe/Cu nanoparticles for adsorption of arsenic from aqueous solutions. First, Fe/Cu nanoparticles at various starch concentrations of 0, 0.02, 0.04 and 0.06 wt% were synthesized and characterized by X-ray diffraction, transmission electron microscopy and zeta potential/particle size analyzer. Then 0.04 wt% stabilized Fe/Cu nanoparticles were tested for the sorption of As(III) and As(V) from synthetic arsenic-contaminated water. To have an understanding about the arsenic adsorption mechanism of nanoparticles, X-ray photoelectron spectroscopy (XPS) was performed before and after adsorption. The results showed that starch provides nanoparticles with a neutral surface and stabilization of nanoparticles is possible with 0.04 wt% or higher concentrations of starch. For 0.04 wt% starch-stabilized Fe/Cu nanoparticles, the adsorption isotherms fit well within the Langmuir equation, with maximum sorption capacities of 90.1 mg/g for As(III) and 126.58 mg/g for As(V) at a pH of 7.0 from the aqueous arsenic solutions. Examining the XPS spectra of nanoparticles before and after adsorption showed that arsenic adsorption by this nanoparticle can be due to the formation of inner-sphere arsenic complexes on the particle surface, and the surface oxygen-containing functional groups involved in adsorption. The high sorption capacity suggests the potential for applying starch-stabilized Fe/Cu nanoparticles to the contaminated waters for removal of arsenic.     

Adsorption kinetic control of As(III &; V) mobilization and sequestration by Mangrove sediment

Elevated concentrations of arsenic in the sediment and pore water in the Sundarban wetlands pose an environmental risk. Adsorption and desorption are hypothesized to be the major processes controlling arsenic retention in surface sediment under oxic/suboxic condition. This study aims to investigate sorption kinetics of As(III & V) and its feedback to arsenic mobilization in the mangrove sediment. It ranges from sand to silty clay loam and shows the adsorption of As(III & V) following the Langmuir relation. Estimates of the maximum adsorption capacity are 59.11 ± 13.26 μg g⁻¹ for As(III) and 58.45 ± 8.75 μg g⁻¹ at 30°C for As(V) in the pH range 4 to 8 and salinity 15–30 psu. Extent of adsorption decreases with increasing pH from 4 to 8 and desorption is the rate-limiting step in the reaction of arsenic with sediment. Arsenic in the sediment could be from a Himalayan supply and co-deposited organic matter drives its release from the sediment. Arsenic concentration in the sediment is well below its maximum absorption capacity, suggesting the release of sorbed arsenic in pore water by the microbial oxidation of organic matter in the sediment with less feedback of adsorption.     

Adsorption, desorption and oxidation of arsenic affected by clay minerals and aging process

 Adsorption/desorption and oxidation/reduction of arsenic at clay surfaces are very important to the natural attenuation of arsenic in the subsurface environment. Although numerous studies have concluded that iron oxides have high affinities for the adsorption of As(V), very little experimental work has addressed the arsenic attenuation capacities of different clay minerals and aging process affecting the transformation of arsenic. The abundance of clay minerals in a variety of geochemical environments and their influence on adsorption of contaminants suggests a need for more experimental work to characterize the adsorption desorption, and oxidation of arsenic on clay minerals. In this investigation three types of clay mineral were studied: the 1 : 1 layer clays [halloysite (IN), sedimentary M-kaolinite, and weathered EPK-kaolinite]; the 2 : 1 layer clays [illite (MT) and illite/montmorillonite (MT)]; the 2 :>: 1 layer clay [chlorite (CA)]. The halloysite and the chlorite had much greater As(V) adsorption (25–35 folds) than the other clay minerals. The clay minerals had lower As(III) adsorption than As(V) adsorption, and the adsorption was affected by pH. Desorption of arsenic from the clay minerals was significantly influenced by the aging process. The quantities of extractable As(III) and As(V) decreased with increasing aging time. The results demonstrated that oxidation of As(III) to As(V) occurred on the clay surfaces, whereas reduction of As(V) to As(III) was not found in any of the clay minerals studied. The oxidation of As(III) was affected by the types of clay and aging time. Received: 22 March 1999 · Accepted: 15 April 1999     

Speciation and natural attenuation of arsenic and iron in a tidally influenced shallow aquifer

The mobility of subsurface arsenic is controlled by sorption, precipitation, and dissolution processes that are tied directly to coupled redox reactions with more abundant, but spatially and temporally variable, iron and sulfur species. Adjacent to the site of a former pesticide manufacturing facility near San Francisco Bay (California, USA), soil and groundwater arsenic concentrations are elevated in sediments near the prior source, but decrease to background levels downgradient where shallow groundwater mixes with infiltrating tidal waters at the plume periphery, which has not migrated appreciably in over two decades of monitoring. We used synchrotron X-ray absorption spectroscopy, together with supporting characterizations and sequential chemical extractions, to directly determine the oxidation state of arsenic and iron as a function of depth in sediments from cores recovered from the unsaturated and saturated zones of a shallow aquifer (to 3.5 m below the surface). Arsenic oxidation state and local bonding in sediments, as As-sulfide, As(III)-oxide, or As(V)-oxide, were related to lithologic redox horizons and depth to groundwater. Based on arsenic and iron speciation, three subsurface zones were identified: (i) a shallow reduced zone in which sulfide phases were found in either the arsenic spectra (realgar-like or orpiment-like local structure), the iron spectra (presence of pyrite), or both, with and without As(III) or As(V) coordinated by oxygen; (ii) a middle transitional zone with mixed arsenic oxidation states (As(III)–O and As(V)–O) but no evidence for sulfide phases in either the arsenic or iron spectra; and (iii) a lower oxidized zone in the saturated freshwater aquifer in which sediments contained only oxidized As(V) and Fe(III) in labile (non-detrital) phases. The zone of transition between the presence and absence of sulfide phases corresponded to the approximate seasonal fluctuation in water level associated with shallow groundwater in the sand-dominated, lower oxic zone. Total sediment arsenic concentrations showed a minimum in the transition zone and an increase in the oxic zone, particularly in core samples nearest the former source. Equilibrium and reaction progress modeling of aqueous-sediment reactions in response to decreasing oxidation potential were used to illustrate the dynamics of arsenic uptake and release in the shallow subsurface. Arsenic attenuation was controlled by two mechanisms, precipitation as sulfide phases under sulfate-reducing conditions in the unsaturated zone, and adsorption of oxidized arsenic to iron hydroxide phases under oxidizing conditions in saturated groundwaters. This study demonstrates that both realgar-type and orpiment-type phases can form in sulfate-reducing sediments at ambient temperatures, with realgar predicted as the thermodynamically stable phase in the presence of pyrite and As(III) under more reduced conditions than orpiment. Field and modeling results indicate that the potential for release of arsenite to solution is maximized in the transition between sulfate-reduced and iron-oxidized conditions when concentrations of labile iron are low relative to arsenic, pH-controlled arsenic sorption is the primary attenuation mechanism, and mixed Fe(II,III)-oxide phases do not form and generate new sorption sites.     

平均粒径对砂土剪切特性的影响及细观机理

针对平均粒径对砂土剪切特性的影响作用,结合室内试验和离散元模拟方法对不同平均粒径砂土进行了细观研究。基于3种不同平均粒径砂土的直剪试验结果,通过建立反映砂土剪切试验特征的PFC（particle flow code）颗粒流模型,详细研究了不同粒径砂土在剪切过程中土样体积变化、力链网络、孔隙率和配位数等细观结构参数的变化特征和规律,并从细观角度分析了颗粒粒径对土样宏观剪切特性的影响机制。结果表明：具有不同平均粒径砂土的细观结构参数在剪切过程中存在显著差异,并且其细观参数差异主要集中体现在剪切带处;剪切力学特性的影响主要体现在抗剪强度和剪胀效应方面,砂土平均粒径越大,抗剪强度越高,剪胀效应越明显;具有不同平均粒径的砂土在剪切过程中土颗粒运动规律及剪切带形态变化特征存在一定的差异,平均粒径越大,剪切带内上跨式颗粒占比越大,剪切带厚度越大。     

The influence of groundwater chemistry on arsenic concentrations and speciation in a quartz sand and gravel aquifera)

We examined the chemical reactions influencing dissolved concentrations, speciation, and transport of naturally occurring arsenic (As) in a shallow, sand and gravel aquifer with distinct geochemical zones resulting from land disposal of dilute sewage effluent. The principal geochemical zones were: (1) the uncontaminated zone above the sewage plume [350 μM dissolved oxygen (DO), pH 5.9]; (2) the suboxic zone (5 μM DO, pH 6.2, elevated concentrations of sewage-derived phosphate and nitrate); and (3) the anoxic zone [dissolved iron(II) 100–300 μM, pH 6.5–6.9, elevated concentrations of sewage-derived phosphate]. Sediments are comprised of greater than 90% quartz but the surfaces of quartz and other mineral grains are coated with nanometer-size iron (Fe) and aluminum (Al) oxides and/or silicates, which control the adsorption properties of the sediments. Uncontaminated groundwater with added phosphate (620 μM) was pumped into the uncontaminated zone while samples were collected 0.3 m above the injection point. Concentrations of As(V) increased from below detection (0.005 μM) to a maximum of 0.07 μM during breakthrough of phosphate at the sampling port; As(III) concentrations remained below detection. These results are consistent with the hypothesis that naturally occurring As(V) adsorbed to constituents of the coatings on grain surfaces was desorbed by phosphate in the injected groundwater. Also consistent with this hypothesis, vertical profiles of groundwater chemistry measured prior to the tracer test showed that dissolved As(V) concentrations increased along with dissolved phosphate from below detection in the uncontaminated zone to approximately 0.07 and 70 μM, respectively, in the suboxic zone. Concentrations of As(III) were below detection in both zones. The anoxic zone had approximately 0.07 μM As(V) but also had As(III) concentrations of 0.07–0.14 μM, suggesting that release of As bound to sediment grains occurred by desorption by phosphate, reductive dissolution of Fe oxides, and reduction of As(V) to As(III), which adsorbs only weakly to the Fe-oxide-depleted material in the coatings. Results of reductive extractions of the sediments suggest that As associated with the coatings was relatively uniformly distributed at approximately 1 nmol/g of sediment (equivalent to 0.075 ppm As) and comprised 20%-50% of the total As in the sediments, determined from oxidative extractions. Quartz sand aquifers provide high-quality drinking water but can become contaminated when naturally occurring arsenic bound to Fe and Al oxides or silicates on sediment surfaces is released by desorption and dissolution of Fe oxides in response to changing chemical conditions.

     

西南表层岩溶带土壤中砷的迁移规律实验与模拟

岩溶地下河是我国西南地区的重要水源,工业生产过程中产生的砷污染物,除通过落水洞等直接进入并污染地下水外,还会在表层岩溶带溶缝、溶隙内吸附、滞留及富集,并在特定条件下再次迁移,成为"稳定次生污染源".以广西某砷污染事件为例,采用窄缝槽物理模型装置进行砷的动态吸附、解吸实验,并结合地球化学模拟研究砷污染物在表层岩溶带土壤中的迁移规律.实验结果显示表层岩溶带对砷的吸附以物理吸附（扩散过程）为主,相比吸附过程而言解吸速率则显得缓慢,而酸溶液相比去离子水可促进砷的解吸过程.地球化学模拟结果表明土壤矿物中以针铁矿对砷的吸附贡献最大,而酸溶液通过溶蚀针铁矿等矿物削弱对砷的吸附能力.因此在西南岩溶地区,表层岩溶带系统一旦纳入砷污染物,则解吸过程缓慢,易形成砷污染物的滞留、富集;而酸雨作用下砷的解吸、迁移过程加快,则会提高地下水系统的污染风险.      

Characteristics of arsenic adsorption from aqueous solution: Effect of arsenic species and natural adsorbents

Batch and column experiments were conducted on As adsorption from aqueous solution by natural solids to test the feasibility of these materials to act as adsorbents for As removal from groundwater and drinking water. The solids considered are natural hematite and natural siderite. The As species studied are As(V), As(III) and dimethylarsinic acid (DMA). Arsenic(III), As(V) and DMA were removed to different extents by the solids studied from water solutions containing these three As species, with the highest efficiency for As(V). In aqueous solutions with a mixture of As species, adsorption kinetics depend on the species. On both materials, As(V) was preferentially adsorbed in the batches and first reached equilibrium, followed by DMA and As(III). The As adsorption took place more slowly on natural hematite and natural siderite compared with ferrihydrite. The results demonstrate that the amount of As removed from As(III) batches was greater than that from As(V) batches due to a surface alteration of the solids caused by As(III) oxidation. Although the highest efficiency for As retention was observed on hematite HIO1 in the batch experiments, siderite used as column filling was more efficient in removing As from water containing the As species studied in comparison with hematite. The coating of fresh Fe(III)-oxides was much more intensive in the siderite-packed column than in the hematite-packed column. The combination of siderite and hematite would promote the column filling performance in removing As from aqueous solution.