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1.
《地学前缘(英文版)》2023,14(2):101494
Permeable reactive barriers (PRBs) are used for groundwater remediation at contaminated sites worldwide. This technology has been efficient at appropriate sites for treating organic and inorganic contaminants using zero-valent iron (ZVI) as a reductant and as a reactive material. Continued development of the technology over the years suggests that a robust understanding of PRB performance and the mechanisms involved is still lacking. Conflicting information in the scientific literature downplays the critical role of ZVI corrosion in the remediation of various organic and inorganic pollutants. Additionally, there is a lack of information on how different mechanisms act in tandem to affect ZVI-groundwater systems through time. In this review paper, we describe the underlying mechanisms of PRB performance and remove isolated misconceptions. We discuss the primary mechanisms of ZVI transformation and aging in PRBs and the role of iron corrosion products. We review numerous sites to reinforce our understanding of the interactions between groundwater contaminants and ZVI and the authigenic minerals that form within PRBs. Our findings show that ZVI corrosion products and mineral precipitates play critical roles in the long-term performance of PRBs by influencing the reactivity of ZVI. Pore occlusion by mineral precipitates occurs at the influent side of PRBs and is enhanced by dissolved oxygen and groundwater rich in dissolved solids and high alkalinity, which negatively impacts hydraulic conductivity, allowing contaminants to potentially bypass the treatment zone. Further development of site characterization tools and models is needed to support effective PRB designs for groundwater remediation. 相似文献
2.
The objectives of this study are to design an optimal electro-enhanced permeable reactive barrier (E2PRB) system for the remediation
of trichloroethylene (TCE)-contaminated water using zero valent iron (ZVI) and direct current (DC) and to investigate the
mechanisms responsible for TCE degradation in different ZVI-DC configurations. A series of column experiments was conducted
to evaluate the effect of different arrangements of electrodes and ZVI barriers in the column on the TCE removal capacity
(RC). In twelve different combinations of ZVI and/or DC application in the test columns, the rate of reductive dechlorination
of TCE was improved up to six times with simultaneous application of ZVI and DC compared to that using ZVI only. The most
effective arrangement of electrode and ZVI for TCE removal was the column set with ZVI and a cathode installed at the down
gradient. Based on the electrokinetic study for the column systems with only DC input, single acid front movement could explain
different RCs. An enhanced dechlorination rate of TCE using E2PRB systems, compared to a conventional PRB system, was observed,
and is considered to be attributed to more electron sources: (1) external DC, (2) electrolysis of water, (3) oxidation of
ZVI, (4) oxidation of dissolved Fe2+, (5) oxidation of molecular hydrogen at the cathode, and (6) oxidation of Fe2+ in mineral precipitates. Each of these electron sources was evaluated for their potential influencing the TCE RC through
the electron competition model and energy consumption. A strong correlation between the quantity of electrons generated, RC,
and the energy-effectiveness was found. 相似文献
3.
A laboratory experiment with two sequenced columns was performed as a preliminary study for the installation of a permeable
reactive barrier (PRB) at a site where a mixed ground water contamination exists. The first column contained granular zero
valent iron (ZVI), the second column was filled with granular activated carbon (GAC). Trichloromethane (TCM, 930 μg/l) and
chlorobenzene (MCB, 260 μg/l) were added to the ground water from the site as the main contaminants. Smaller amounts (<60 μg/l)
of benzene, 1,2-dichloroethane, 1,1,2-trichloroethane (1,1,2-TCA), 1,1-dichloroethene (1,1-DCE), trichloroethene (TCE), tetrachloroethene
(PCE), 1,2-dichloropropane (1,2-DCP), bromodichloromethane (BDCM), dibromochloromethane (DBCM), tribromomethane (TBM), vinyl
chloride and chromate were also added to the water to simulate the complex contamination pattern at the site of interest.
PCE, TCE, 1,1-DCE, DBCM, BDCM, TBM, MCB and chromate were remediated in contact with ZVI, while the remaining contaminants
showed incomplete degradation. A fraction of 8–16.5% TCM was converted to dichloromethane (DCM). Remaining contaminant concentrations
were efficiently sorbed by the GAC until breakthrough of DCM was observed after 1,230 exchanged pore volumes in the GAC. The
results show that the complex mixture of contaminants can be remediated by a sequenced PRB consisting of ZVI and GAC and that
DCM sorption capacity is the critical parameter for the dimensions of the GAC reactor. 相似文献
4.
Alexandra N. Golab Mark A. Peterson Buddhima Indraratna 《Environmental Earth Sciences》2009,59(1):241-254
The Shoalhaven region of NSW experiences environmental acidification due to acid sulphate soils (ASS). In order to trial an
environmental engineering solution to groundwater remediation involving a permeable reactive barrier (PRB), comprehensive
site characterisation and laboratory-based batch and column tests of reactive materials were conducted. The PRB is designed
to perform in situ remediation of the acidic groundwater (pH 3) that is generated in ASS. Twenty-five alkaline reactive materials
have been tested for suitability for the barrier, with an emphasis on waste materials, including waste concrete, limestone,
calcite-bearing zeolitic breccia, blast furnace slag and oyster shells. Following three phases of batch tests, two waste materials
(waste concrete and oyster shells) were chosen for column tests that simulate flow conditions through the barrier and using
acidic water from the field site (pH 3). Both waste materials successfully treated with the acidic water, for example, after
300 pore volumes, the oyster shells still neutralised the water (pH 7). 相似文献
5.
《Applied Geochemistry》2005,20(9):1648-1657
An upflow packed column was operated to evaluate the potential of a mixture of municipal compost and calcite to promote sulphidogenesis in the remediation of a simulated mine water at high flows (>0.1 m d−1). Results showed that the pH was neutralised and metals (Fe, Al, Zn, Cu) were significantly removed. Metal removal was attributed to the combined result of precipitation as metal (oxy)hydroxides and carbonates, co-precipitation with these (oxy)hydroxides and sorption onto the compost surface rather than to precipitation as metal sulphides. The two last mechanisms are especially significant for Zn, whose hydroxide is not expected to precipitate at pH 6–7. Before the saturation of compost sorption sites, 60% of the influent Zn was estimated to have been removed by co-precipitation with Fe- and Al-(oxy)hydroxide and 40% by sorption onto the municipal compost. 相似文献
6.
In this study, the retention of Ca and other metals (Pb, Cu, Fe, Zn and Mn) in the Oostriku peat bog (central Estonia) was modelled. Equilibrium sorption of metals on amorphous ferric oxyhydroxide and solid organic matter was simulated at steady-state. Ferric oxyhydroxide formation and possible precipitation of other metals (Mn, Pb and Cu) in the peat was also assessed. Evolution of metal sorption fronts along a peat profile over time was simulated with a dynamic model to test if metal–metal competition effects could cause Pb and Cu to sorb at higher amounts in the uppermost peat than in the lower peat, as observed in the field. The predicted sorbed amounts of metals were compared with those previously observed in the peat. In general, good agreement between both batch and dynamic model results and the independent observations at the Oostriku peat site was obtained. This suggests that the relatively simple model approach employed here might be generally useful for assessing other peat sites and similar applications. 相似文献
7.
《Applied Geochemistry》2002,17(8):1081-1092
Different types of fine-grained chemical precipitates were characterized in the surroundings of the pyrite-chalcopyrite mine of Libiola (Northern Italy). Both water chemistry and sediment composition were used to investigate metal mobility near the mine area. Local drainage waters were very acidic (with a pH as low as 2.5) and were rich in dissolved metals (Fe, Al, Cu, Zn, Mn, Ni). Sediments associated with low pH water (pH <4.5) were ochreous mixtures of schwertmannite and goethite with traces of jarosite. Their chemistry was dominated by Fe and they had, compared to other sediments investigated, low concentrations of other metals. When the acidity decreased gradually, other precipitates formed. At a pH of approximately 5, a poorly crystalline, whitish, Al-rich precipitate occurred. At a pH between 6 and 7, a poorly crystalline, blue, Cu (Zn) rich phase was present. These “sequential” precipitation events progressively reduced the metal loading typical of the acidic mine water when there was a gradual mixing with normal water. When a sudden mixing between normal waters (pH ∼8, Ca–HCO3, low metal bearing) and acidic waters took place, a rapid flocculation occurred of mixed precipitates containing Fe, Al and trace elements. 相似文献
8.
Randolph A. Koski LeeAnn Munk Andrea L. Foster Wayne C. Shanks III Lisa L. Stillings 《Applied Geochemistry》2008
The oxidation of sulfide-rich rocks, mostly leftover debris from Cu mining in the early 20th century, is contributing to metal contamination of local coastal environments in Prince William Sound, Alaska. Analyses of sulfide, water, sediment, precipitate and biological samples from the Beatson, Ellamar, and Threeman mine sites show that acidic surface waters generated from sulfide weathering are pathways for redistribution of environmentally important elements into and beyond the intertidal zone at each site. Volcanogenic massive sulfide deposits composed of pyrrhotite and (or) pyrite + chalcopyrite + sphalerite with subordinate galena, arsenopyrite, and cobaltite represent potent sources of Cu, Zn, Pb, As, Co, Cd, and Hg. The resistance to oxidation among the major sulfides increases in the order pyrrhotite ? sphalerite < chalcopyrite ? pyrite; thus, pyrrhotite-rich rocks are typically more oxidized than those dominated by pyrite. The pervasive alteration of pyrrhotite begins with rim replacement by marcasite followed by replacement of the core by sulfur, Fe sulfate, and Fe–Al sulfate. The oxi
dation of chalcopyrite and pyrite involves an encroachment by colloform Fe oxyhydroxides at grain margins and along crosscutting cracks that gradually consumes the entire grain. The complete oxidation of sulfide-rich samples results in a porous aggregate of goethite, lepidocrocite and amorphous Fe-oxyhydroxide enclosing hydrothermal and sedimentary silicates. An inverse correlation between pH and metal concentrations is evident in water data from all three sites. Among all waters sampled, pore waters from Ellamar beach gravels have the lowest pH (∼3) and highest concentrations of base metals (to ∼25,000 μg/L), which result from oxidation of abundant sulfide-rich debris in the sediment. High levels of dissolved Hg (to 4100 ng/L) in the pore waters probably result from oxidation of sphalerite-rich rocks. The low-pH and high concentrations of dissolved Fe, Al, and SO4 are conducive to precipitation of interstitial jarosite in the intertidal gravels. Although pore waters from the intertidal zone at the Threeman mine site have circumneutral pH values, small amounts of dissolved Fe2+ in the pore waters are oxidized during mixing with seawater, resulting in precipitation of Fe-oxyhydroxide flocs along the beach–seawater interface. At the Beatson site, surface waters funneled through the underground mine workings and discharged across the waste dumps have near-neutral pH (6.7–7.3) and a relatively small base-metal load; however, these streams probably play a role in the physical transport of metalliferous particulates into intertidal and offshore areas during storm events. Somewhat more acidic fluids, to pH 5.3, occur in stagnant seeps and small streams emerging from the Beatson waste dumps. Amorphous Fe precipitates in stagnant waters at Beatson have high Cu (5.2 wt%) and Zn (2.3 wt%) concentrations that probably reflect adsorption onto the extremely high surface area of colloidal particles. Conversely, crystalline precipitates composed of ferrihydrite and schwertmannite that formed in the active flow of small streams have lower metal contents, which are attributed to their smaller surface area and, therefore, fewer reactive sorption sites. Seeps containing precipitates with high metal contents may contribute contaminants to the marine environment during storm-induced periods of high runoff. Preliminary chemical data for mussels (Mytilus edulis) collected from Beatson, Ellamar, and Threeman indicate that bioaccumulation of base metals is occurring in the marine environment at all three sites. 相似文献
9.
Column bioreactors were used for studying mechanisms of metal removal, assessment of long-term stability of spent reactive mixtures, as well as potential metal mobility after treating highly contaminated acid mine drainage (AMD; pH 2.9–5.7). Several physicochemical, microbiological, and mineralogical analyses were performed on spent reactive mixtures collected from 4 bioreactors, which were tested in duplicate for two hydraulic retention times (7.3d and 10d), with downward flow over an 11-month period. Consistent with the high metal concentrations in the AMD feed, and with low metal concentrations measured in the treated effluent, the physicochemical analyses indicated very high concentrations of metals (Fe, Mn, Cd, Ni, and Zn) in the top and bottom layers of the reactive mixtures from all columns. Moreover, the concentrations of Fe (50.8–57.8 g/kg) and Mn (0.53–0.70 g/kg) were up to twice as high in the bottom layers, whereas the concentrations of Cd (6.77–13.3 g/kg), Ni (1.80–5.19 g/kg) and Zn (2.53–13.2 g/kg) were up to 50-times higher in the top layers. Chemical extractions and elemental analysis gave consistent results, which indicated a low fraction of metals removed as sulfides (up to 15% of total metals recovered in spent reactive mixtures). Moreover, Fe and Mn were found in a more stable chemical form (residual fraction was 42–74% for Mn and 30–77% for Fe) relative to Cd, Ni or Zn, which seemed more weakly bound (oxidisable/reducible fractions) and showed higher potential mobility. Besides identifying (oxy)hydroxide and carbonate minerals, the mineralogical analyses identified metal sulfides containing Fe, Cd, Ni and Zn. Metal removal mechanisms were, therefore, mainly adsorption and other binding mechanisms with organic matter (for Cd, Ni and Zn), and the precipitation as (oxy)hydroxide minerals (for Fe and Mn). After 15 months, however, the column bioreactors did not lose their capacity for removing metals from the AMD. Although the metals were immobile during the bioreactor treatment, their mobility could increase from spent reactive mixtures, if stored inappropriately. Metal recovery by acidic leaching of spent substrates at the end of bioreactor operation could be an alternative. 相似文献
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12.
文中研究在粒状铁化学还原三氯乙烯渗透反应格栅和生物降解苯和甲苯渗透反应格栅的联合格栅技术中,下游生物降解格栅中铁还原环境下微生物对苯和甲苯的生物降解。通过模拟粒状铁渗透反应格栅下游铁还原环境,主要研究微生物以苯、甲苯作为碳源时,对碳源的专一性。通过批实验发现,对于分别用苯和甲苯培养驯化的微生物,互换碳源后,微生物对2 000.00μg/L苯和甲苯的生物降解半衰期分别由之前的1.0和1.5 d减少到0.7和1.0 d,互换碳源后苯和甲苯的去除率分别增加38%和32%。在粒状铁渗透反应格栅下游生物降解渗透反应格栅中,微生物在铁还原环境下以苯、甲苯作为碳源时对碳源没有专一性,苯和甲苯可以同时被生物降解去除。 相似文献
13.
渗透反应格栅(permeable reactive barrier,PRB)在国外被广泛应用于场地尺度的地下水污染修复,因其无须外源动力、不占地面空间、运行成本低等优势在国内受到广泛关注。不同场地水文地质条件、污染物类型、污染羽分布具有差异性,前期场地调查、反应材料的筛选、反应墙尺寸结构的设计对于PRB的有效运行至关重要。本文以PRB修复河南某Cr(Ⅵ)污染场地为例,详细阐述场地调查、材料筛选、材料反应参数确定、PRB结构优化等方面的研究过程及成果,可为后续PRB修复技术的应用提供参考。研究结果表明:PRB修复技术适用于该场地,铸铁与活性炭混合材料为最佳修复材料;反应门长40 m(反应材料厚2 m,上下游分别为2 m厚砾石层),东西两侧隔水墙长为60 m的U型漏斗-门系统型PRB,可有效捕获并修复污染羽,工程成本远低于连续反应墙式PRB,为该场地修复最优PRB结构类型。 相似文献
14.
Acid neutralization mechanisms and metal release in mine tailings: a laboratory column experiment 总被引：1，自引：0，他引：1
Jasna Jurjovec Carol J. Ptacek David W. Blowes 《Geochimica et cosmochimica acta》2002,66(9):1511-1523
Mining and milling of base metal ore deposits can result in the release of metals to the environment. When sulfide minerals contained in mine tailings are exposed to oxygen and water, they oxidize and dissolve. Two principal antagonistic geochemical processes affect the migration of dissolved metals in tailings impoundments: sulfide oxidation and acid neutralization. This study focuses on acid neutralization reactions occurring in the saturated zone of tailings impoundments. To simulate conditions prevailing in many tailings impoundments, 0.1 mol/L sulfuric acid was passed continuously through columns containing fresh, unoxidized tailings, collected at Kidd Creek metallurgical site. The results of this column experiment represent a detailed temporal observation of pH, Eh, and metal concentrations. The results are consistent with previous field observations, which suggest that a series of mineral dissolution-precipitation reactions control pH and metal mobility. Typically, the series consists of carbonate minerals, Al and Fe(III) hydroxides, and aluminosilicates. In the case of Kidd Creek tailings, the dissolution series consists of ankerite-dolomite, siderite, gibbsite, and aluminosilicates. In the column experiment, three distinct pH plateaus were observed: 5.7, 4.0, and 1.3. The releases of trace elements such as Cd, Co, Cr, Cu, Li, Ni, Pb, V, and Zn were observed to be related to the pH buffering zones. High concentrations of Zn, Ni, and Co were observed at the first pH plateau (pH 5.7), whereas Cd, Cr, Pb, As, V, and Al were released as the pH of the pore water decreased to 4.0 or less. 相似文献
15.
Coupled physicochemical and bacterial reduction mechanisms for passive remediation of sulfate- and metal-rich acid mine drainage 总被引：1，自引：0，他引：1
S. N. Muhammad F. M. Kusin Z. Madzin 《International Journal of Environmental Science and Technology》2018,15(11):2325-2336
Treatment of acid mine drainage (AMD) highly rich in sulfate and multiple metal elements has been investigated in a continuous flow column experiment using organic and inorganic reactive media. Treatment substrates that composed of spent mushroom compost (SMC), limestone, activated sludge and woodchips were incorporated into bacterial sulfate reduction (BSR) treatment for AMD. SMC greatly assisted the removals of sulfate and metals and acted as essential carbon source for sulfate-reducing bacteria (SRB). Alkalinity produced by dissolution of limestone and metabolism of SRB has provided acidity neutralization capacity for AMD where pH was maintained at neutral state, thus aiding the removal of sulfate. Fe, Pb, Cu, Zn and Al were effectively removed (87–100%); however, Mn was not successfully removed despite initial Mn reduction during early phase due to interference with Fe. The first half of the treatment was an essential phase for removal of most metals where contaminants were primarily removed by the BSR in addition to carbonate dissolution function. The importance of BSR in the presence of organic materials was also supported by metal fraction analysis that primary metal accumulation occurs mainly through metal adsorption onto the organic matter, e.g., as sulfides and onto Fe/Mn oxides surfaces. 相似文献
16.
Sorption is an important process in the modelling and prediction of the movement of heavy metals in unsaturated clay barriers. This experimental study investigates the effect of pH changes in the acidic range on the sorption characteristics of heavy metals such as: lead, copper and zinc in an unsaturated soil. A series of one-dimensional coupled solute and moisture leaching column tests, using different heavy metal solutions, were conducted on an unsaturated illitic soil at varying pH values. Variations of volumetric water content (VWC) with distance were measured for different time durations, and concentrations of heavy metals in the liquid and solid phases were analysed. Partitioning coefficient profiles of contaminants along the soil column were determined for each individual layer in the soil.
Results from column leaching tests showed that the sorption characteristics of heavy metals are controlled by many factors which should be taken into consideration, i.e. the VWC, time of wetting, soil pH, and the influent heavy metal concentrations. Simplification of Kd as a constant and of the VWC as a linear function cannot be considered a good assumption and may lead to an improper evaluation of the sorption phenomena and also to serious errors in predicting contaminant transport through unsaturated soils. 相似文献
17.
An innovative setup of a permeable reactive barrier (PRB) was installed in Willisau, Switzerland to remediate chromate contaminated groundwater. Instead of a conventional continuous barrier, this PRB consists of cylinders installed in rows: a single row for lower expected CrVI-concentrations and an offset double row for higher expected CrVI-concentrations. The cylinders are filled with reactive grey cast-Fe shavings mixed with gravel to prevent extensive precipitation of secondary phases in the pore space. The treatment of the contaminants takes place both within the cylinders and in the dissolved FeII plume generated downstream of the barrier. Monitoring of the contamination situation over a period of 3 a provided evidence of the mobilization, transport and behavior of the contaminants in the aquifer. Groundwater and reactive material were sampled upstream, within and downstream of the barrier by a Multi-Port Sampling System (MPSS) that revealed the geochemical processes as a function of time and space. Comprehensive chemical analyses included sensitive parameters such as CrVI, FeII/FeIII, redox potential, dissolved O2 and pH. Several campaigns using multiple optical tracers revealed a rather complex hydrological regime at different scales, thereby complicating the barrier performance. 相似文献
18.
Immobilization of trace elements in contaminated soils by zero-valent iron (ZVI) is a promising remediation method, but questions about its long-term performance remain unanswered. To quantify immobilization and predict possible contaminant remobilization on long timescales detailed knowledge about immobilization mechanisms is needed. This study aimed at assessing the long-term effect of ZVI amendments on dissolved copper and arsenic in contaminated soils, at exploring the immobilization mechanism(s), and at setting up a geochemical model able to estimate dissolved copper and arsenic under different scenarios. Samples from untreated and ZVI-treated plots in two field experiments where ZVI had been added 6 and 15 years ago were investigated by a combination of batch experiments, geochemical modeling and extended X-ray absorption fine structure (EXAFS) spectroscopy. Dissolved copper and arsenic concentrations were described by a multisurface geochemical model with surface complexation reactions, verified by EXAFS. The ZVI remained “reactive” after 6–15 years, i.e. the dissolved concentrations of copper and arsenic were lower in the ZVI-treated than in the untreated soils. There was a shift in copper speciation from organic matter complexes in the untreated soil to surface complexes with iron (hydr)oxides in the ZVI-treated soil. The pH value was important for copper immobilization and ZVI did not have a stabilizing effect if pH was lower than about 6. Immobilization of arsenic was slightly pH-dependent and sensitive to the competition with phosphate. If phosphate was ignored in the modeling, the dissolution of arsenate was greatly underestimated. 相似文献
19.
Core samples were taken at two sites from a peat deposit buried by a sanitary landfill operated by the city of Vancouver since the 1960s and from a third site where the same peat bed is not covered by landfill. Twenty-nine subsamples from the three cores were analyzed by a variety of techniques to determine the concentration of as many as 34 constituents. The content of heavy metals, the principal object of this investigation, is highest in the lower part of the peat succession, in which there is a significant amount of interbedded inorganic sediment, rather than in the upper clean bog peat. Individual layers as little as 2.5 cm thick can hold concentrations of heavy metals ten times that of the nearby layers. The heavy metal contents show a high positive correlation with those of iron and manganese and a very low correlation with sulfur. Iron from the landfill has been transported by downward percolating groundwater in solution or colloidal suspension into the lower layers of peat deposit where the passing heavy metals were sorbed. A comparison of the amounts of heavy metals stored in the peat alone with the amount leaving the whole landfill annually suggests that some metals, notably lead and arsenic, might be retained in the peat for very long periods, whereas other metals such as zinc and mercury might be quickly lost. 相似文献
20.
Hexavalent chromium is a soluble, mobile, and highly toxic metal ion in groundwater. Adsorption by permeable reactive barriers (PRBs) with special sorbent is a common method to remove hexavalent chromium. A series of experiments have been performed to remove hexavalent chromium in groundwater under PRB with modified chitosan. Therefore, in this paper, the authors first estimated adsorption characteristics of the modified chitosan in a column test, and then calibrated the PRB adsorption parameters in a sandbox test, and finally designed an optimal width, length, and depth of the PRB with the same reactive media in a three-dimensional aquifer. The results showed that the modified chitosan might be a potential adsorption medium. The design schemes can meet the water quality standard of 0.1 mg/L Cr(VI). Heterogeneity of dispersion is a crucial factor when designing the PRB. Therefore, the design of the PRB structures can be appropriate and serve as reference for groundwater remediation. 相似文献