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1.
Over the past 30 years the literature has burgeoned with in situ approaches for groundwater remediation. Of the methods currently available, the use of metallic iron (Fe0) in permeable reactive barrier (PRB) systems is one of the most commonly applied. Despite such interest, an increasing amount of experimental and field observations have reported inconsistent Fe0 barrier operation compared to contemporary theory. In the current work, a critical review of the physical chemistry of aqueous Fe0 corrosion in porous media is presented. Subsequent implications for the design of Fe0 filtration systems are modeled. The results suggest that: (i) for the pH range of natural waters (>4.5), the high volumetric expansion of Fe0 during oxidation and precipitation dictates that Fe0 should be mixed with a non‐expansive material; (ii) naturally occurring solute precipitates have a negligible impact on permeability loss compared to Fe0 expansive corrosion; and (iii) the proliferation of H2 metabolizing bacteria may contribute to alleviate permeability loss. As a consequence, it is suggested that more emphasis must be placed on future work with regard to considering the Fe0 PRB system as a physical (size‐exclusion) water filter device.  相似文献   

2.
Lin L  Benson CH  Lawson EM 《Ground water》2005,43(4):582-596
This paper describes reactive transport simulations conducted to assess the impact of mineral fouling on the hydraulic behavior of continuous-wall permeable reactive barriers (PRBs) employing granular zero-valent iron (ZVI) in carbonate-rich alluvial aquifers. The reactive transport model included a geochemical algorithm for simulating corrosion and mineral precipitation reactions that have been observed in ZVI PRBs. Results of simulations show that porosity and hydraulic conductivity of the ZVI decrease over time and that flows are redistributed throughout the PRB in response to fouling of the pore space. Under typical conditions, only subtle changes occur within the first 10 years (i.e., duration of the current field experience record with PRBs), and the most significant changes do not occur until the PRB has operated for at least 30 years. However, changes can occur sooner (or later) if the rate at which mineral-forming ions are delivered to the PRB is higher (or lower) than that expected under typical conditions (i.e., due to higher/lower flow rate or inflowing ground water that has higher/lower ionic strength). When the PRB is more permeable than the aquifer, the median Darcy flux in the PRB does not change appreciably over time because the aquifer controls the rate of flow through the PRB. However, seepage velocities in the PRB increase, and residence times decrease, due to porosity reductions caused by accumulation of minerals in the pore space. When fouling becomes extensive, bypassing and reductions in flow rate in the PRB occur.  相似文献   

3.
A method is presented to evaluate ground water residence time in a zero‐valent iron (ZVI) permeable reactive barrier (PRB) using radon‐222 (222Rn) as a radioactive tracer. Residence time is a useful indicator of PRB hydraulic performance, with application to estimating the volumetric rate of ground water flow through a PRB, identifying flow heterogeneity, and characterizing flow conditions over time as a PRB matures. The tracer method relies on monitoring the decay of naturally occurring aqueous 222Rn as ground water flows through a PRB. Application of the method at a PRB site near Monticello, Utah, shows that after 8 years of operation, residence times in the ZVI range from 80 to 486 h and correlate well with chemical parameters (pH, Ca, SO4, and Fe) that indicate the relative residence time. Residence times in this case study are determined directly from the first‐order decay equation because we show no significant emanation of 222Rn within the PRB and no measurable loss of 222Rn other than by radioactive decay.  相似文献   

4.
There are many fundamental problems with the injection of nano‐zero‐valent iron (NZVI) particles to create permeable reactive barrier (PRB) treatment zone. Among them the loss of medium porosity or pore blocking over time can be considered which leads to reduction of permeability and bypass of the flow and contaminant plume up‐gradient of the PRB. Present study provides a solution for such problems by confining the target zone for injection to the gate in a funnel‐and‐gate configuration. A laboratory‐scale experimental setup is used in this work. In the designed PRB gate, no additional material from porous media exists. NZVI (d50 = 52 ± 5 nm) particles are synthesized in water mixed with ethanol solvent system. A steady‐state condition is considered for the design of PRB size based on the concept of required contact time to obtain optimum width of PRB gate. Batch experiment is carried out and the results are used in the design of PRB gate width (~50 mm). Effect of high initial NO3–‐N concentration, NZVI concentration, and pore velocity of water in the range of laminar groundwater flow through porous media are evaluated on nitrate‐N reduction in PRB system. Results of PRB indicate that increasing the initial NO3–‐N concentration and pore velocity has inhibitor effect—against the effect of NZVI concentration—on the process of NO3–‐N removal. Settlement velocity (S.V.) of injected NZVI with different concentrations in the PRB is also investigated. Results indicate that the proposed PRB can solve the low permeability of medium in down‐gradient but increasing of the S.V. especially at higher concentration is one of the problems with this system that needs further investigations.  相似文献   

5.
Core samples taken from a zero-valent iron permeable reactive barrier (ZVI PRB) at Cornhusker Army Ammunition Plant, Nebraska, were analyzed for physical and chemical characteristics. Precipitates containing iron and sulfide were present at much higher concentrations in native aquifer materials just upgradient of the PRB than in the PRB itself. Sulfur mass balance on core solids coupled with trends in ground water sulfate concentrations indicates that the average ground water flow after 20 months of PRB operation was approximately twenty fold less than the regional ground water velocity. Transport and reaction modeling of the aquifer PRB interface suggests that, at the calculated velocity, both iron and hydrogen could diffuse upgradient against ground water flow and thereby contribute to precipitation in the native aquifer materials. The initial hydraulic conductivity ( K ) of the native materials is less than that of the PRB and, given the observed precipitation in the upgradient native materials, it is likely that K reduction occurred upgradient to rather than within the PRB. Although not directly implicated, guar gum used during installation of the PRB is believed to have played a role in the precipitation and flow reduction processes by enhancing microbial activity.  相似文献   

6.
An injectable permeable reactive barrier (PRB) technology was developed to sequester 90Sr in groundwater through the in situ formation of calcium‐phosphate mineral phases, specifically apatite that incorporates 90Sr into the chemical structure. This injectable barrier technology extends the PRB concept to sites where groundwater contaminants are too deep or where site conditions otherwise preclude the application of more traditional trench‐emplaced barriers. An integrated, multiscale development and testing approach was used that included laboratory bench‐scale experiments, an initial pilot‐scale field test, and the emplacement and evaluation of a 300‐feet‐long treatability‐test‐scale PRB. The apatite amendment formulation uses two separate precursor solutions, one containing a Ca‐citrate complex and the other a Na‐phosphate solution, to form apatite precipitate in situ. Citrate is needed to keep calcium in solution long enough to achieve a more uniform and areally extensive distribution of precipitate formation. In the summer of 2008, the apatite PRB technology was applied as a 91‐m‐long (300 feet) PRB on the downgradient edge of a 90Sr plume beneath the Hanford Site in Washington State. The technology was deployed to reduce 90Sr flux discharging to the Columbia River. Performance assessment monitoring data collected to date indicate that the barrier is meeting treatment objectives (i.e., 90% reduction in 90Sr concentration). The average reduction in 90Sr concentrations at four downgradient compliance monitoring locations was 95% relative to the high end of the baseline range approximately 1 year after treatment, and continues to meet remedial objectives more than 4 years after treatment.  相似文献   

7.
Various analytical expressions describing the hydraulic behavior of a continuous permeable reactive barrier (PRB) are developed based upon a two-dimensional approximation of the local groundwater flow system. The fully penetrating PRB is represented as an arbitrarily oriented elliptical “analytic element” with a hydraulic conductivity different from that of the aquifer. The validity of this elliptical geometry approximation as a surrogate for rectangular PRB performance is evaluated and put into context. Closed-form expressions for solute travel time distributions along the extent of the barrier and PRB capture zone geometry are evaluated for general barrier dimension (length and width), hydraulic conductivity, and orientation with respect to regional flow. These expressions are used as the foundation of a simple PRB design process, and provide some interesting insights into the hydraulic behavior of continuous permeable reactive barriers.  相似文献   

8.
The problem of permeable reactive barrier (PRB) capture and release behavior is investigated by means of an approximate analytical approach exploring the invariance of steady-state solutions of the advection–dispersion equation to conformal mapping. PRB configurations considered are doubly-symmetric funnel-and-gate as well as less frequent drain-and-gate systems. The effect of aquifer heterogeneity on contaminant plume spreading is hereby incorporated through an effective transverse macro-dispersion coefficient, which has to be known. Results are normalized and graphically represented in terms of a relative capture efficiency M of contaminant mass or groundwater passing a control plane (transect) at a sufficient distance up-stream of a PRB as to comply with underlying assumptions. Factors of safety FS are given as the ratios of required capture width under advective–dispersive and purely advective transport for achieving equal capture efficiency M. It is found that M also applies to the release behavior down-stream of a PRB, i.e., it describes the spreading and dilution of PRB treated groundwater possibly containing incompletely remediated contamination and/or remediation reaction products. Hypothetical examples are given to demonstrate results.  相似文献   

9.
Reactive barriers: hydraulic performance and design enhancements   总被引：2，自引：0，他引：2  
Painter BD 《Ground water》2004,42(4):609-617
The remediation of contaminated ground water is a multibillion-dollar global industry. Permeable reactive barriers (PRBs) are one of the leading technologies being developed in the search for alternatives to the pump-and-treat method. Improving the hydraulic performance of these PRBs is an important part of maximizing their potential to the industry. Optimization of the hydraulic performance of a PRB can be defined in terms of finding the balance between capture, residence time, and PRB longevity that produces a minimum-cost acceptable design. Three-dimensional particle tracking was used to estimate capture zone and residence time distributions. Volumetric flow analysis was used for estimation of flow distribution across a PRB and in the identification of flow regimes that may affect the permeability or reactivity of portions of the PRB over time. Capture zone measurements extended below the base of partially penetrating PRBs and were measured upgradient from the portion of aquifer influenced by PRB emplacement. Hydraulic performance analysis of standard PRB designs confirmed previously presented research that identified the potential for significant variation in residence time and capture zone. These variations can result in the need to oversize the PRB to ensure that downgradient contaminant concentrations do not exceed imposed standards. The most useful PRB design enhancements for controlling residence time and capture variation were found to be customized downgradient gate faces, velocity equalization walls, deeper emplacement of the funnel than the gate, and careful manipulation of the hydraulic conductivity ratio between the gate and the aquifer.  相似文献   

10.
The combination of detailed multilevel ground water geochemistry samples, a natural-gradient tracer test, minislug tests, and a numerical flow and transport model was used to examine flow through a zero-valent iron permeable reactive barrier (PRB) installed to remove explosives from ground water. After 20 months of operation, the PRB continued to completely remove explosives from the ground water flowing through it. However, the data indicate that a portion of ground water flow was being diverted beneath the PRB. Ground water geochemistry was significantly altered by the PRB, and concentrations of some ions, including sulfate, carbonate, and calcium, were substantially reduced due to precipitation. Field data and numerical model results indicate that, after 20 months of operation, flow through the PRB was reduced to approximately one-third of its expected value.  相似文献   

11.
Permeable reactive barriers (PRBs) have gained popularity in recent years as a low-cost method for ground water remediation. However, their cost advantage usually requires that these barriers remain maintenance free for a number of years after installation. In this study, sediment cores were retrieved from a pilot-scale PRB consisting of a sand and wood particle (sawdust) mixture that has been in continuous operation for 15 years treating nitrate from a septic system plume in southern Ontario (Long Point site). Reaction rates for the 15-year-old media were measured in dynamic flow column tests and were compared to rates measured in year 1 using the same reactive mixture. Nitrate removal rates in the 15-year-old media varied, as expected, with temperature in the range of 0.22 to 1.1 mg N/L/d at 6 °C to 10 °C to 3.5 to 6.0 mg N/L/d at 20 °C to 22 °C. The latter rates remained within about 50% of the year 1 rates (10.2 ± 2.7 mg N/L/d at 22 °C). Near the end of the year 15 column test, media particles >0.5 mm in diameter, containing most of the wood particles, were removed from the reactive media by sieving. Nitrate removal subsequently declined by about 80%, indicating that the wood particles were the principal energy source for denitrification. This example shows that some denitrifying PRBs can remain maintenance free and be adequately reactive for decades.  相似文献   

12.
This study evaluates the efficiency of a full‐scale, 81 m‐wide permeable reactive barrier (PRB) configured by injection of dairy whey in the downgradient region of a contaminant source zone to enhance the in situ biodegradation of high concentrations (102 to 103μg/L) of chlorinated ethenes (CEs). Ten biannual whey injections were completed in a 3.5‐year pilot phase and 1.5‐year operational phase. Improved and sustained dechlorination was observed at extraction/injection and downgradient wells in the fully‐operational phase, when dried whey masses were increased from 13.6 kg to 230–360 kg, whey slurry volumes were increased from 2300 L to 307,000–480,000 L, and extraction/injection well loops were employed for the application of whey. At extraction/injection wells, CEs decreased to low (≤10 μg/L) or undetectable levels. At downgradient wells, average trichloroethene concentrations decreased, by as much as 100% (from ≤384.2 during the pilot phase to ≤102.6 μg/L during the operational phase), while average cis‐dichloroethene concentrations decreased by as much as 57.5% (from ≤6466.1 to ≤4912.2 μg/L). Downgradient vinyl chloride averages either increased by as much as 63.8% (from ≤859.6 to ≤1407.9 μg/L) or decreased by 64.0% (from 1375.4 to 880 μg/L). Downgradient ethene + ethane averages increased by as much as 73.2% (from ≤1145.3 to ≤1347.1 μg/L). On the basis of the 2008 average market price, the estimated material cost of whey is $1.96/kg organic carbon or, for the configuration of an 81 m PRB by biannual application of 300 kg whey, $325/year. Carbon substrate cost comparisons and implications for efficient in situ treatment design are discussed.  相似文献   

13.
The Powder River Basin (PRB) of Wyoming and Montana contains significant coal and coal bed natural gas (CBNG) resources. CBNG extraction requires the production of large volumes of water, much of which is discharged into existing drainages. Compared to surface waters, the CBNG produced water is high in sodium relative to calcium and magnesium, elevating the sodium adsorption ratio (SAR). To mitigate the possible impact this produced water may have on the quality of surface water used for irrigation, the State of Montana passed water anti‐degradation legislation, which could affect CBNG production in Wyoming. In this study, we sought to determine the proportion of CBNG produced water discharged to tributaries that reaches the Powder River by implementing a four end‐member mixing model within a Bayesian statistical framework. The model accounts for the 87Sr/86Sr, δ13CDIC, [Sr] and [DIC] of CBNG produced water and surface water interacting with the three primary lithologies exposed in the PRB. The model estimates the relative contribution of the end members to the river water, while incorporating uncertainty associated with measurement and process error. Model results confirm that both of the tributaries associated with high CBNG activity are mostly composed of CBNG produced water (70–100%). The model indicates that up to 50% of the Powder River is composed of CBNG produced water downstream from the CBNG tributaries, decreasing with distance by dilution from non‐CBNG impacted tributaries from the point sources to ~10–20% at the Montana border. This amount of CBNG produced water does not significantly affect the SAR or electrical conductivity of the Powder River in Montana. Copyright © 2013 John Wiley & Sons, Ltd.  相似文献   

14.
Filtration systems containing metallic iron as reactive medium (Fe0 beds) have been intensively used for water treatment during the last two decades. The sustainability of Fe0 beds is severely confined by two major factors: (i) reactivity loss as result of the formation of an oxide scale on Fe0 and (ii) permeability loss due to pore filling by generated iron corrosion products. Both factors are inherent to iron corrosion at pH > 4.5 and are common during the lifespan of a Fe0 bed. It is of great practical significance to improve the performance of Fe0 beds by properly addressing these key factors. Recent studies have shown that both reactivity loss and permeability loss could be addressed by mixing Fe0 and inert materials. For a non‐porous additive like quartz, the threshold value for the Fe0 volumetric proportion is 51%. Using the Fe0/quartz system as reference, this study theoretically discusses the possibility of (i) replacing Fe0 by bimetallic systems (e.g., Fe0/Cu0), or (ii) partially replacing quartz by a reactive metal oxide (MnO2 or TiO2) to improve the efficiency of Fe0 beds. Results confirmed the suitability of both tools for sustaining Fe0 bed performance. It is shown that using a Fe0:MnO2 system with the volumetric proportion 51:49 will yield a filter with 40% residual porosity at Fe0 depletion (MnO2 porosity 62%). This study improves Fe0 bed design and can be considered as a basis for further refinement and detailed research for efficient Fe0 filters.  相似文献   

15.
Abiotic degradation of chlorinated solvents by reactive iron minerals such as iron sulfides, magnetite, green rust, and other Fe(II)‐containing minerals has been observed in both laboratory and field studies. These reactive iron minerals form under iron‐ and sulfate‐reducing conditions which are commonly found in permeable reactive barriers (PRBs), enhanced reductive dechlorination (ERD) treatment locations, landfills, and aquifers that are chemically reducing. The objective of this review is to synthesize current understanding of abiotic degradation of chlorinated solvents by reactive iron minerals, with special focus on how abiotic processes relate to groundwater remediation. Degradation of chlorinated solvents by reactive minerals can proceed through reductive elimination, hydrogenolysis, dehydrohalogenation, and hydrolysis reactions. Degradation products of abiotic reactions depend on degradation pathways and parent compounds. Some degradation products (e.g., acetylene) have the potential to serve as a signature product for demonstrating abiotic reactions. Laboratory and field studies show that various minerals have a range of reactivity toward chlorinated solvents. A general trend of mineral reactivity for degradation of chlorinated solvents can be approximated as follows: disordered FeS > FeS > Fe(0) > FeS2 > sorbed Fe2+ > green rust = magnetite > biotite = vermiculite. Reaction kinetics are also influenced by factors such as pH, natural organic matter (NOM), coexisting metal ions, and sulfide concentration in the system. In practice, abiotic reactions can be engineered to stimulate reactive mineral formation for groundwater remediation. Under appropriate site geochemical conditions, abiotic reactions can occur naturally, and can be incorporated into remedial strategies such as monitored natural attenuation.  相似文献   

16.
There are ongoing efforts to render conventional biosand filters (BSF) more efficient for safe drinking water provision. One promising option is to amend BSF with a reactive layer containing metallic iron (Fe0). The present communication presents some conceptual options for efficient Fe0‐amended BSF in its fourth generation. It is shown that a second fine‐sand layer should be placed downwards from the Fe0‐reactive layer to capture dissolved iron. This second fine‐sand layer could advantageously contain adsorbing materials (e.g. activated carbons, wooden charcoals). An approach for sizing the Fe0‐reactive layer is suggested based on 3 kg Fe0 per filter. Working with the same Fe0 load will ease comparison of results with different materials and the scaling up of household BSF to large scale community slow sand filters (SSF).  相似文献   

17.
In order to better understand the nature of deep crustal high electrical conductivity, we studied the electrical properties of a tilted section of a former lower continental crust exposed in the Calabrian arc of the Alpine-Apennine mountain system. Geoelectric field measurements and impedance measurements on rock samples showed that these high-grade metamorphic rocks are generally highly resistive as expected for crystalline, electrolytically conducting rocks of low porosity. This holds for graphite-free metabasites as well as for metapelites which generally contain accessory, up to 3% biogenic graphite in the form of isolated grains. Clearly as an exception, a group of thin stratiform black horizons with thicknesses of 1-15 cm within the metapelitic series was detected by means of self-potential (SP) measurements. Rock samples from these horizons exhibit high, quasi-metallic bulk conductivities of up to 50 S/m (0.02 Ωm) in agreeement with up to 20% syngenetic graphite, forming a network of interconnected streaks or crack fillings. The high amount of carbon most probably originates from organic matter of Corg-rich black shales. Relative enrichment of the low mobility graphitic matter compared to the carbon content of the assumed protoliths may have been due to pressure solution and partial melting during prograde metamorphism, without major contribution of a fluid phase, resulting in isolated graphite flakes. Although enriched, graphite in this form has little effect on electrical conductivity. For the Calabrian black horizons, microscopic analyses make conceivable that, in a further decisive step, isolated graphite grains were mechanically smeared to continuous pathways during uplift by shearing, producing hereby the observed graphitic network which is needed to generate high conductivity. As Corg-rich black shales are common members of sedimentary sequences throughout the earth’s history, good conductors of this type may be expected in the continental crust at any depth depending on tectonic and metamorphic history, with the exception of magmatic protoliths. Regarding the extremely high conductivity of the meta-black shale samples containing syngenetic sheared graphite, a total thickness of a few meters of such rocks is sufficient to explain magnetotelluric high conductivity anomalies in the deep crust.  相似文献   

18.
Previous studies have shown how biogenic silica particles undergo conversion to aluminosilicate phases in large tropical deltaic systems, thus affecting the world ocean budget of major seawater cations. This study tackles the important question of the silica budget in the coastal zone of the Mississippi River Delta, providing evidence for the role of biogenic silica diagenesis in this subtropical system from direct examination of individual diatom particles, sediment leachates and pore-water composition. The estimated reactive silica stored in the study area (5990 km2) is based on operational leaches that account for altered biogenic silica particles and other authigenic aluminosilicate phases in addition to fresh biogenic silica. Early diagenesis of silica in the delta front occurs mainly where more siliceous material is deposited. An inner-shelf area, where hypoxic conditions are found, significantly contributes to the formation of authigenic products of Si alteration. Data suggest that the limiting factor of silica alteration processes is the availability of detrital phases such as Al and Fe. The estimated total reactive silica accumulation in the study area is 1.45×1010 mol Si year−1, representing ∼2.2% of the long-term bulk sediment accumulation. On the basis of a conservative appraisal, the authigenic mineral components account for ∼40% of the long-term reactive silica storage. This study shows that non-tropical deltaic systems are significantly more important sinks of silica than previously thought and that, where conditions are favourable, a consistent portion of reactive silica not leaving the shelf is stored within the delta in the form of authigenic components.  相似文献   

19.
Permeable reactive barriers (PRBs) are a popular technology for passive contaminant remediation in aquifers through installation of reactive materials in the pathway of a plume. Of fundamental importance are the degree of remediation inside the reactor (residence time) and the portion of groundwater intercepted by a PRB (capture width). Based on a two-dimensional conformal mapping approach (previously used in related work), the latter is studied in the present work for drain-and-gate (DG) PRBs, which may possess a collector and a distributor drain (“full” configuration) or a collector drain only (“simple” configuration). Inherent assumptions are a homogeneous unbounded aquifer with a uniform far field, in which highly permeable drains establish constant head boundaries. Solutions for aquifer flow fields in terms of the complex potential are derived, illustrated, and analyzed for doubly symmetric DG configurations and arbitrary reactor hydraulic resistance as well as ambient groundwater flow direction. A series of practitioner-friendly charts for capture width is given to assist in PRB design and optimization without requiring complex mathematics. DG PRBs are identified as more susceptible to flow divergence around the reactor than configurations using impermeable side structures (e.g., funnel-and-gate), and deployment of impermeable walls on drains is seen to mitigate this problem under certain circumstances.  相似文献   

20.
The use of metallic iron filters (Fe0 filters) has been discussed as a promising low‐cost option for safe drinking water production at household level. Filter clogging due to the volumetric expansive nature of iron corrosion has been identified as the major problem of Fe0 filters. Mixing Fe0 and sand (yielding Fe0/sand filters) has been proposed as a tool to extent filter service life. However, no systematic discussion rationalizing Fe0/sand mixtures is yet available. This communication theoretically discussed suitable Fe0/sand proportions for efficient filters. Results suggested that Fe0/sand filters should not contain more that 50 vol% Fe0 (25 wt% when Fe0 is mixed with quartz). The actual Fe0 percentage in a filter will depend on its intrinsic reactivity.  相似文献   

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