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297 MIGRATION OF SOME POLLUTANTS THROUGH CLAYEY AND SANDY SOILS: CENTRIFUGE MODELLING M. S. S. Almeida Departamento de Engenharia Civil - COPPE S. B. Gurung Depart. of Civil Engineering & Environmmental Engineering Hiroshima University Japan ABSTRACT: This paper presents the migration of benzyl amine and salicylic acid through bentonite soil layer and migration of zinc through dredged sediments carried out in the Mini-Drum centrifuges of Hiroshima University Federal University of Rio de Janeiro. Two types of dredged sediments; one with only sand content and the other with 5% of silt and 28% of clay content were used for the purpose of studying the migration behavior of heavy metals through these soils. The Mini-Drum centrifuge was chosen for carrying out these studies because of its potential to accelerate the flow N (scale factor) times faster than in the corresponding prototype and at the same time maintaining approximate field stress condition in the models. Therefore, both type of models i.e. bentonite models and dredged sediment models were carried out in accelerated gravity field of 105-g and 50-g respectively for making it possible to migrate the chosen pollutants through clayey and fine grain soils. From the test results, bentonite shows the good potential of attenuating benzyl amine and salicylic acid and therefore may be a good material in sealing or containing organic chemicals wastes. Whereas, heavy metal like zinc is attenuated well by dredged sediments when the dredged sediments contain finer grain fractions in the sediments. 1.INTRODUCTION Domestic, industrial or chemical wastes generated put a challenge to Civil Engineers for making the proper disposable site or remediating the contaminated sites in years to come. At present, in civil engineering practice, low permeability clay soils are used as a liner material or cut-off wall material, for containing or sealing-off the underground flow of various fluids, such as leachates from a sanitary landfill, oils from a storage reservoir, chemicals from a chemically contaminated site. In order to assess the potential of the centrifuge modeling of geoenvironmental problems, two different studies have been carried out and these are outlined in the next section. 2.CENTRIFUGE MODELING STUDIES The first study was related with the capability of low permeability clay soils in containing some organic compounds. For this purpose, benzyl amine and salicylic acid, which are organic base and acid respectively were chosen as representative of organic chemicals to study the attenuation potential of bentonite against these chemicals. Test results were fitted to 1-D advection dispersion equation to obtain the migration parameters. The second study was related with problems that may be faced by the civil engineers when dredging lagoon sediments. Some of these sediments may have some degree of contamination with heavy metals such as zinc, cooper, chromium and cadmium (Almeida, et al. 1998, 1999; Borma et al, 1998). In the next 3. THEORY Assuming that advection, dispersion and sorption are the only transport processes involved, the equation used to describe the movement of a solute in saturated, homogeneous porous media during one- dimensional steady flow is (Bear, 1979; Freeze and Cherry, 1979): t Q x C u x C D t C oo ¶ ¶ - ¶ ¶ - ¶ ¶ = ¶ ¶ 2 2 (1) where, C is the concentration of the solute in the aqueous phase; Q is the sorbed mass of the solute per unit mass of solid phase; is the porosity; is the bulk density; D is the longitudinal dispersion coefficient, v is the mean pore-water velocity in the x direction; x is the distance and t is time. The solution of equation (1) requires a relationship between Q and the aqueous phase concentration C, which is most commonly given by CKQ d= (2) the constant Kd is being referred to as the distribution or partition coefficient. Combining equation (2) with (1) leads to: x C u x C D t C R ood -= 2 2 (3) where Rd, the retardation factor, is R K d d= +1 (4) Equation 3 implies that the porosity q and the volumetric flux remain constant in time and space (steady-state flow) and it is applied for modelling one-dimensional transient transport with linear, reversible, instantaneous sorption. Following the analytical approach as suggested by Yamaguchi et al. (1989), the solution of Eq. (3) is given by : [ ] [ ] [ ] Dt utx D ux Dt utx erfcerfctxC 42 1 42 1* exp),( +- += (5) where, C*(x,t) is relative concentration at any depth x, at time t, u is average interstitial velocity = uo/Rd, D is advection-dispersion coefficient = Do/Rd. Using first-term approximation method, Equation (5) reduces to: 1 2 4 (6) where, Ci * is relative concentration, L is depth of soil, i = 1,2, ..... ,n. and 1 2 1 1 2 2 1 2 2 1 ; 2 4 1 2 2 1 1 2 2 1 2 (7) is argument of complementary error function. No literature regarding the modelling of adsorption process using the geotechnical centrifuge was available, rather to avoid this problem researchers seem to have used conservative tracers. Therefore, for the sake of working assumption, amount of chemicals as well as zinc adsorbed on the soil surface have been calculated by using the equation of mass conservation which can be written as: S mc V C M == -- ´´ (8) where, S is the content of chemicals adsorbed (g/kg), mc is total mass of chemical in the solution (g), V is volume of liquid in the system (L), and C is concentration of the liquid draining out from the centrifuge (g/L). The total stress (s ) acting on the soil model in the increasing direction of the centrifuge radius is given by the relation: (( ))== ++òò . /2 0 2 z tR z (9) where, w is rad/sec of centrifuge, Rt, is radius to the top of the model and z, the depth in the soil model. 3.1 - 3. Reduction of Centrifuge Test Data The principle of physical modelling of pollution migration, through the soil mass using geotechnical centrifuge, is governed by the fact that if identical fluids in model and prototype are used, and the average Darcy’s velocity is maintained. Then the permeability of the soil model can be calculated from the rate of discharge (Qm), flowing across the cross-sectional area (Am) under the hydraulic gradient (im). The prototype permeability coefficient (kp) is related to model permeability coefficient (km) by the relation mm mm AiN Q N k pk ´´== (10) Furthermore, scaling laws for the transport of solute through a layer of soil are as follows: (Hensley, 1989) t N tp m= 2 (11) V V Np m= (12) mp DD = ifPe <1 (13) N D D mp = if Pe >1 (14) where, t is time; V is interstitial velocity; D is hydrodynamic dispersion; N is the scale factor; Pe is the Peclect number and the indices p and m refer to prototype and model values respectively. The dependence of hydrodynamic dispersion on the Peclect number is discussed for example, by Bear (1979). The dispersion is velocity dependent for higher Peclect number (Pe>1). 4. MINI-DRUM CENTRIFUGE Model tests were carried out in geotechnical centrifuge. Migration of organic chemicals through the bentonite sand layer was performed in the Mini-Drum centrifuge of Hiroshima University whereas migration of zinc through dredged materials were conducted in the Mini-Drum centrifuge of Federal University of Rio de Janeiro. Brief descriptions on both centrifuges have been given below. A typical diagram of a mini-drum centrifuge isshown in Figure 1. Figure 1 Schematic diagram of Mini-drum centrifuge 4.1. Mini-Drum Centrifuge of Hiroshima University Mini-Drum centrifuge of Hiroshima University has 80-cm. diameter. It houses a ring channel that holds the soil model. The ring channel has the internal dimension of 18.5 cm. as width, 11.5 cm. as depth and an outermost radius of 37.2 cm. The drum can be rotated from axis horizontal mode to axis vertical mode while it is running at or below 260 rpm and facilitate the pouring of bentonite-sand slurry. At axis vertical mode, the drum can be rotated up to 1000 rpm. At a linear modelling scale of N=105, the inside dimensions of the ring channel can model a prototype soil of length = 210 m. width = 18.9 m. and depth = 11.5 m.. Data from the models are routed through slip rings to the externally installed data acquisition system. 300 4.2. Mini-Drum centrifuge of Federal University of Rio de Janeiro This centrifuge has a ring channel of internal diameter = 1.0 m, a height = 0.25 m and a depth = 0.17 m. The face plate, where the instrumentation is housed, is 0.7 m. in diameter. The centrifuge is provided with a tilt mechanism similar to Hiroshima University to facilitate model preparation. With the main drive axis in the vertical direction, the centrifuge can be run at 900 rpm (450-g), carrying a payload of 200 kg. The on board data acquisition system consists of a flight PC with 16 channel unity for signal conditioning of the instrumentation, with the capacity to up grade to 32 channels, if necessary. It is possible to control the fluid levels in the ring channel via digitally controlled standpipe motors with position feedback. In-flight instrumentation includes pore pressure transducers, resistivity probes, temperature probes and displacement transducers. 5. MATERIAL USED 5.1 Bentonite The bentonite used in this research was purchased from Katayama Chemicals, Osaka, which has the pH value around 10 and is a Ca- montmorillonite. Griffin et al. (1976) suggest that the Ca-montmorillonite does not produce shrinkage cracks (synersis) as it’s counterpart Na-montmorillonite and therefore, it is believed that the uniform bed of bentonite layer is formed in the soil model. Enagi sand was used for making the incompressible bed under the bentonite layer in order to smooth the flow of chemicals. The Enagi sand has d10 and d60 as 0.14 mm. and 0.4 mm. giving coefficient of uniformity (Cu) and coefficient of curvature (Cc) as 2.86, and 1.12, respectively. The average grain size (d50) was 0.35 mm. and according to JSF classification (JSSMFE, 1990) this sand was classified as poorly graded sand (SP). Therefore, it should provide pervious and incompressible base for the overlain bentonite layer at 105-g in Mini- Drum centrifuge. The circular hole through the soil model is the space of a soil sample taken for the vane shear test. Test result on vane shear test have been described elsewhere (Gurung et al., 1996). 5.2 Chemicals The chemicals benzyl amine and salicylic were selected on the ground of safety in handling. Properties of these chemicals are presented in Table 1. To maintain the compatibility of testing equipment with the chemicals used and for the sake of easy detection of the chemicals during the chemical analysis, initial concentration of the benzyl amine and salicylic acid were prepared as 4.88 g/L and 0.96 g/L respectively. From the initial concentration of the solution it is obvious that the amount of chemical compared to volume of water is negligible, therefore during the calculation, density of the chemical solution is taken as density of water. The soil models where solution of benzyl amine and salicylic acid was permeated have been named as BNmin and SALIcid, respectively in this paper. Table 1. Properties of organic chemicals Chemicals Benzyl amine Salicylic acid Molecular wt. 107.16 138.13 Physical state Liquid Acicular crystal pH 11 2.54 Solubility in water Infinity 2.2 g/L 5.3 Dredged materials Grain size distributions of the dredged material i.e. Sao Francisco sand and Bento Rivbeiro sand are shown in Figure 2. Note that Bento Rebeiro sand has more clay content than Sao Francisco sand. According to the Unified Soil Classification System São Francisco soil (SF) can be classified as a poorly graded sand (SP) and the Bento Ribeiro soil (BR) as a clayey sand (SC). Index properties of these soils are given in Table 2. 5.4 Zinc In the present study, zinc was selected as the heavy metal pollutant for migrating 301 through the soil model of dredged sedimentary deposits. Zinc solutions were prepared from Zinc nitrate [Zn(NO3)26H20] powder at an initial concentration of about 200-ppm. Zinc solution fractions that had migrated through the soil models were collected regularly and sent for titration immediately. The reagent used for detecting the concentration of zinc was ethylenediaminetetra acetic acid disodium salt [C10H14N2O8Na2.2H2O] prepared at a concentration of 0.001M. Table 2. Properties of Sao Francisco and Bento Ribeiro sand Models Properties Sao Francisco Bento Ribeiro Sand (%) 100 67 Silt (%) - 5 Clay (%) - 28 wL (%) - 41 wP (%) - 17 Organic matter (%)0.148 1.53 CEC (cmole/kg) 1.6 4.5 pH value 6.6 6.2 Specific Gravity, Gs 2.59 2.67 maxdg (gf/cm 3) 1.57 1.88 w opt (%) 4.6 13.4 Pore volume (cm3) 1257 948 5.4 Zinc In the present study, zinc was selected as the heavy metal pollutant for migrating through the soil model of dredged sedimentary deposits. Zinc solutions were prepared from Zinc nitrate [Zn(NO3)26H20] powder at an initial concentration of about 200-ppm. Zinc solution fractions that had migrated through the soil models were collected regularly and sent for titration immediately. The reagent used for detecting the concentration of zinc was ethylenediaminetetra acetic acid disodium salt [C10H14N2O8Na2.2H2O] prepared at a concentration of 0.001M. 6. TESTING PROCEDURE Testing procedures have been divided into two headings namely bentonite models and dredged sediment models. 6.1 For bentonite models 30 kg. of Enagi sand and 3 kg. of bentonite inter-bedding each other were mixed with 18 kg. of distilled water in an AICO mixer, under de-aired condition of -76 cm. Hg for 9 hours. The reason for mixing under de-aired condition was to avoid entrapping of air bubbles, which have detrimental effect of forming the pockmarks during the consolidation of clay slurry (Gronow et al. 1988). Total amount of 0.001 0.01 0.1 1 10 100 DIAMETER (mm) 0 20 40 60 80 100 FINE MEDIUM COARSE CLAY SILT GRAVELSAND BR Soil SF Sand P E R C E N T P A S S IN G ( % ) Figure 2 Grain size distributions of Sao Francisco and Bento Ribeiro sands 302 slurry poured into the Mini-Drum was kept the same in both the model tests. The acceleration of drum was increased in stages to avoid tensile cracking of bentonite layer. Due to the centrifugation, bentonite and sand were separated in uniform layers. After primary consolidation, solutions of chemical were poured over the bentonite layer through the ring channel. Migration test were carried out at 105-g. Effective stress at the bottom of the bentonite in both cases was calculated as 6.1 kPa (Table 3). One hour after pouring the solution, a drainage valve was opened. Discharged solutions were collected at regular intervals and analyzed by high performance liquid chromatography for determining the relative concentration of discharged solution. Model tests were terminated once the discharge was no longer monitored due to the decrease in hydraulic head. High Performance Liquid Chromatograph (HPLC) was used for the chemical analysis of solution discharged from the Mini-Drum to obtain the breakthrough curve for each chemical.HPLC consists of solvent delivery unit, UV detector and chromatopac. Solvent delivery unit supplies the mobile phase under pressure to the HPLC column, which is designed to retain the different chemicals for different periods. The chemicals from HPLC column then flow to UV detector, which uses deuterium lamp as a light source, and perform the ultraviolet analysis and relay the test data to chromatopac for printing the test results. The linear adsorption coefficients (k) for both the chemicals on bentonite were determined from the classical batch experiments. In each batch, 1 g of bentonite was mixed with 12 mL. of freshly prepared chemical solution (same concentration as in centrifuge model) and shaken for 24 hours giving adequate time for adsorption. Table 3. Model test conditions Models g-levels sv’ (kPa) Bmin 105 6.10 SALIcid 105 6.10 SF 50 22.7 BR 50 25.4 6.2 For dredged sediment models Two centrifuge model containers with dimensions of 21 cm. (width) x 25.8 cm. (length) x 17cm. (height) were mounted in opposite sides of the ring channel, which allowed the drum centrifuge to be used as beam type centrifuge. However, the whole area of the ring channel can be used for modelling geotechnical events as in the case of Hiroshima University one. In the present study, this beam type of facility was used to reduce the volume of the soil models, so that about 20 pore volumes of solution could flow through the soil models during the observation time. A piece of geotextile, having the same plan area as that of the model container, was placed at the bottom of the model container to allow adequate drainage. Above this geotextile, a 5- cm deep soil model was compacted in five layers. In each layer 60 blows of a 2.54-kg hammer, falling from a height of 30.5 cm was used for the compaction of model. Models were compacted at their respective optimum water contents to produce maximum densities, as shown in Table 2. After compaction of a soil model, the centrifuge was tilted from the axis- horizontal mode to the axis-vertical mode with the help of an electrically driven motor. Centrifuge acceleration was then applied in increments of 10-g steps up to 50-g. Following this; tap water was supplied to the soil model from the overhead water tank through an inlet pipe, to saturate the model. Three pore volumes of water were allowed to flow through the soil models in an attempt to ensure complete saturation. It is believed that the accelerated flow flushed out all of the air bubbles. After three pore volumes of water flowed through the soil, the zinc solution was supplied to the soil model. 2 cm depth of zinc solution was maintained constantly over the soil model throughout the zinc migration process. The 2 cm depth of zinc solution above the soil model yielded a hydraulic gradient of 1.4 in an accelerated gravity field of 50-g. The zinc solutions that migrated through the soil models were collected regularly, and titration of the samples were carried out immediately to trace the breakthrough curve. 303 Table 4. Transport parameters for the models Interstitial Velocity u (m/h) Hydrodynamic Dispersion, D (m2/h) Name of model Tests Model Prototype Model Prototype Bmin 0.0032 0.300x10-4 5.90x10-5 5.90x10-5 SALIcid 0.0101 0.900x10-4 17.9x10-5 17.9x10-5 SF 2.2600 452.3x10-4 0.085 0.0017 BR 0.3870 77.40x10-4 0.030 0.0006 After attaining equilibrium of a breakthrough curve, the zinc solution was stopped and tap water was supplied to the soil model to cleanse zinc from the soil model, in order to obtain the desorption part of the breakthrough curve. However, in the present study only the absorption results have been presented, as the numerical simulation was not carried out for the desorption studies. The cleansing process was carried out until the relative concentration of effluent dropped to below 2%. Effective vertical stresses at the bottom of the soil model were calculated to be 22.7 kPa, and 25.48 kPa for SF and BR soil models, respectively. 7. RESULTS AND DISCUSSION 7.1 Bentonite soil models Each soil model was prepared in the same way and therefore is the replicate of each other. As this is the first attempt to model the chemical flow using the Mini-Drum centrifuge, emphasis here is centred at the validation of transport phenomena by comparing the breakthrough curves obtained from the model tests and theoretical advection-dispersion equation. Theoretical breakthrough curve for each of the chemicals was calculated by considering the bentonite layer only without considering the underlain sand layer because it is the bentonite that is effective in attenuating the chemicals. For the theoretical model, relative concentration i.e. effluent concentrations divided by the initial concentration of the chemical solution (C/Co) was calculated by using Eq. (6) and the average interstitial velocity (u) and advection-dispersion coefficient (D) was calculated by using Eq. (7). The prediction of BNmin breakthrough curve by the theoretical model is shown in Figure 3 where good fit between theoretical and centrifuge models can be observed. The u and D for this model were calculated as 3.2x10-3 m/h and 5.9x10-5 m2/h, respectively. Similarly, the prediction of theoretical model for the SALIcid is presented in the Figure 4 and is in good agreement. Toward the end, the theoretical model over-predicts the SALIcid values, which is believed to be due to the reaction between salicylic acid and bentonite, as the discharged solution never showed the initial concentration of 0.96 g/L. The convection-dispersion parameters for this model was calculated as u = 10.1x10-3 m/h and D = 17.9x10-5 m2/h. These values are about 3 times greater than the corresponding values of BNmin. These higher values of u and D are believed to be due to the higher molecular weight of the salicylic acid (Table 1.) which make the flow faster under the accelerated gravity field. The peclet number (Pe) of these two models were calculated to be less than unity hence, the model values of D have been reported as the corresponding prototype values of D in Table 4. However, the values of u and D in both the cases are very low (nominal), which may suggest that bentonite have good potential in attenuating the tested organic chemicals. 7.2 Dredged material models Data from the centrifuge tests on Sao Francisco sand and Bento Ribeiro sand are presented in Figures 5 and 6. The diagrams shown are for relative concentrations versus elapsed time, where relative concentrations are the measured effluent concentrations divided by the initial concentration. The interstitial velocity of the Sao Francisco soil model was found to be nearly six times higher than that of the Bento Ribeiro soil model (Table 4) and is 304 due to the high fines content in Bento Ribeiro soil. Note that Sao Francisco soil has almost zero clay content. 0,0 0,2 0,4 0,6 0,8 1,0 1,2 0,0 10,0 20,0 30,0 40,0 50,0 Time (Hours) R el at iv e co nc en tr at io n FITTED OBS u = 0.03x10-3 m/hour D = 0.5x10-4 m2/hour Rd = 2.5 Fig. 3 Breakthrough curve for Benzyl amine The centrifuge data were analysed by the computer code CXTFIT, a non-linear least- squares routine designed to provide one or more parameters for a number of transport equation formulations (Parker and van Genuchten, 1984). Two parameters, the dispersion coefficient (D) and the retardation factor (Rd), were simultaneously obtained using CXTFIT. The breakthrough curves from these centrifuge model tests have been well fitted by the CXTFIT code as shown in Figures 6 and 7 for Sao Francisco sand and Bento Ribeiro soil respectively. The regression coefficient r2 obtained for each test shown in Figures 6 and 7 indicates the quality of the fit for the centrifuge data by usingCXTFIT. The equilibrium model describes the shape of the breakthrough curves quite well. In present case N=50 and Pe is 29.1 and 169.7 for the test with Bento Ribeiro and Sao Francisco soil respectively. The interstitial velocity and hydrodynamic dispersion in the test, in term of both model and prototype values, have been presented in Table 4. The ispersion coefficient of Sao Francisco soil is higher than the dispersion coefficient of Bento Ribeiro soil showing the dependence of the dispersion coefficient with interstitial velocities for the high Peclect numbers used. The calculated value of retardation factor (Rd) for Bento Ribeiro clayey sand was found greater than the Rd of Sao Francisco sand. 0,0 0,2 0,4 0,6 0,8 1,0 1,2 0,0 2,0 4,0 6,0 8,0 10,0 12,0 14,0 Time (Hours) R el at iv e co nc en tr at io n FITTED OBS u =0.09x10-3 m/hour D = 0.1x10-4 m2/hour Rd = 8.1 Fig. 4 Breakthrough curve for Salicyclic acid 0,0 0,2 0,4 0,6 0,8 1,0 1,2 0,0 0,2 0,4 0,6 Time (Hours) R el at iv e co nc en tr at io n OBS FITTED u = 4.5 x 10 -3 m/hour D = 85.7 x 10 -3 m 2/hour Fig. 5 Breakthrough curve for zinc (SF sand) 8. CONCLUSION In this study, Mini-Drum centrifuge facility available at Hiroshima University and Federal University of Rio de Janeiro were used to investigate the migration of benzyl amine, salicylic acid and zinc through clayey and sandy soil models respectively. Predictions of 1-D advection-dispersion theoretical model and the computer code CXITFIT are in good agreement with the centrifuge test results and thus validate the migration phenomena through clayey and fine grain soil in the accelerated gravity field. This shows that Mini-Drum centrifuges can be a useful tool in modelling pollution migration problems related to geotechnical engineering. 0,0 0,2 0,4 0,6 0,8 1,0 0,0 1,0 2,0 3,0 Time (Hours) R el at iv e co nc en tr at io n OBS FITTED u = 7.7 x 10 -3 m/hour D = 30.5 x 10 -3 m 2/hour Fig. 6 Breakthrough curve for zinc (B R sand) 305 Benzyl amine treated bentonite shows about three times lower interstitial velocity than salicylic acid treated bentonite. Consequently, dispersion coefficient of benzyl amine is lower than salicylic acid. This difference in behavior may be attributed to higher affinity of benzyl amine to water and lower molecular weight of benzyl amine than salicylic acid. Both the interstitial velocities and dispersion coefficients for benzyl amine and salicylic acid are much smaller than the corresponding values of zinc. Although the organic compounds were migrated at the acceleration level of 105-g compared to 50-g for the zinc migration. This phenomenon suggests the importance of clayey soil in attenuating the migration of pollutants. Furthermore, the interstitial velocity of the São Francisco sand is six times greater than the interstitial velocity of the Bento Ribero soil. Similarly, the dispersion coefficient of the São Francisco sand is also greater than the dispersion coefficient of the Bento Ribero sand. This difference in behavior is due to the higher percentage of clay content i.e. 28 % in Bento Ribero sand than the 0 % of clay content in São Francisco sand. 9. REFERENCES Almeida, M.S.S., Barbosa, M.C., and Casanova, F., and M.C. 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Parker J.C. and van Genuchten M.T., (1984), Determining Transport Parameters from Laboratory and Field Tracer Experiments. Virginia Agricultural Experiment Station, Bulletin 84-3, ISSN 0096-6088, 81 p. JSF M 111-1990 (1990), Method of classification of soils for Engineering purposes. Japanese Society of Soil Mech. and Founds. Engineering. (In Japanese) Yamaguchi, T., Moldrup, P., and Yokosi, S. (1989), Using breakthrough curves for parameter estimation in the advection- dispersion model of solute transport. Soil Sci. Soc. Am. J. Vol. 53, no. 6. pp. 1635- 1641.
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