Published online 27 June 2007
Published in J Environ Qual 36:1187-1193 (2007)
DOI: 10.2134/jeq2006.0427
© 2007 American Society of Agronomy, Crop Science Society of America, and Soil Science Society of America
677 S. Segoe Rd., Madison, WI 53711 USA
TECHNICAL REPORTS
Heavy Metals in the Environment
Hydrophobicity of Soil Colloids and Heavy Metal Mobilization
Effects of Drying
Sondra Klitzke* and
Friederike Lang
Berlin Univ. of Technology, Dep. of Soil Science, Salzufer 11-12, D-10587 Berlin, Germany
* Corresponding author (sondra.klitzke{at}tu-berlin.de)
Received for publication October 4, 2006.
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ABSTRACT
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Drying of soil may increase the hydrophobicity of soil and affect the mobilization of colloids after re-wetting. Results of previous research suggest that colloid hydrophobicity is an important parameter in controlling the retention of colloids and colloid-associated substances in soils. We tested the hypothesis that air-drying of soil samples increases the hydrophobicity of water-dispersible colloids and whether air-drying affects the mobilization of colloid-associated heavy metals. We performed batch experiments with field-moist and air-dried (25°C) soils from a former sewage farm (sandy loam), a municipal park (loamy sand), and a shooting range site (loamy sand with 25% Corg). The filtered suspensions (<1.2 µm) were analyzed for concentrations of dissolved and colloidal organic C and heavy metals (Cu, Cd, Pb, Zn), average colloid size, zeta potential, and turbidity. The hydrophobicity of colloids was determined by their partitioning between a hydrophobic solid and a hydrophilic aqueous phase. Drying increased hydrophobicity of the solid phase but did not affect the hydrophobicity of the dispersed colloids. Drying decreased the amount of mobilized mineral and (organo-)mineral colloids in the sewage farm soils but increased the mobilization of organic colloids in the C-rich shooting range soil. Dried samples released less colloid-bound Cd and Zn than field-moist samples. Drying-induced mobilization of dissolved organic C caused a redistribution of Cu from the colloidal to the dissolved phase. We conclude that drying-induced colloid mobilization is not caused by a change in the physicochemical properties of the colloids. Therefore, it is likely that the mobilization of colloids in the field is caused by increasing shear forces or the disintegration of aggregates.
Abbreviations: COC, colloidal organic carbon DOC, dissolved organic carbon DOM, dissolved organic matter TOC, total organic carbon
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INTRODUCTION
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THE INFLUENCE of drying on the physicochemical properties of the soil solution and the solid phase has been well researched. Dried soil samples showed a drastic increase in the concentration of dissolved organic matter (DOM) after rewetting (Bartlett and James, 1980; Baskaran et al., 1994; Courchesne et al., 1995; Münch et al., 2002; Kjærgaard et al., 2004b), leading to a decrease in the pH of the soil solution (Courchesne et al., 1995). The observed increase in dissolved organic carbon (DOC) concentration may be attributed to the disruption of microbial biomass (Christ and David, 1996) and the breakdown of aggregate bonds (Raveh and Avnimelech, 1978). Because DOC contributes to an enhanced mobilization of dissolved heavy metal species by forming soluble metal complexes (Brümmer et al., 1986), drying and rewetting may be conducive to enhancing metal leaching. Drying was found to increase water repellency of the solid phase (Dekker et al., 2001) due to increasing hydrophobicity.
Numerous recent studies have shown that colloid-bound heavy metal transport plays a crucial role in soils (Keller and Domergue, 1996; Jensen et al., 1999; Denaix et al., 2001) and is found to be of greater importance than transport as dissolved ions (Egli et al., 1999; Jensen et al., 1999). Several authors describe the influence of drying and rewetting as important factors controlling colloid release. El-Farhan et al. (2000) observed the highest peak of particle mass recovery after the infiltration on an initially dry field soil. Similarly, field studies of Jann et al. (2002) revealed increasing mobilization of colloids after dry periods. The authors attributed this phenomenon to microerosion and abrasion induced by shear forces. Likewise, Denaix et al. (2001) found markedly increased concentrations of mobilizable Pb-containing colloids in the soil water after dry periods. However, the drying-induced mobilization of colloids seems to be limited to the initial phase of re-wetting: In the frame of column studies using dried soil (soil-water potential: 15 500 hPa), Kjærgaard et al. (2004b) observed an initial increase in colloid release followed by a constant decrease as the pore volume increases. This initial increase may be explained by slaking of aggregates due to the compression by trapped air during the wetting phase (Le Bissonnais, 1996). In the same study, Kjærgaard et al. (2004b) investigated the effect of initial soil matrix potential on water-dispersible colloids, revealing that as a result of enhanced interparticle bonding or cementation of colloids drying leads to a decrease of dispersible colloids in the soil suspension.
Because drying of soil may induce changes in the solid phase (e.g., increasing hydrophobicity), it is postulated that this may affect colloid dispersibility. Few studies provide first hints on colloid hydrophobicity as an important parameter influencing colloid retention in soils. Wan and Wilson (1994a) demonstrated an increased retention of colloidal latex particles and bacteria with increasing particle hydrophobicity in an unsaturated sand column experiment. Similarly, under saturated conditions, hydrophobic colloids showed a lower recovery than hydrophilic colloids. Thus, the authors concluded that hydrophilic colloids are more mobile than hydrophobic ones (Wan and Wilson, 1994a,b) because they sorb less strongly to the gaswater and solidwater interfaces. These findings, together with the observation that drying can increase the hydrophobicity of the bulk soil, are in conflict with the concept of colloid mobilization after soil drying. In addition to having an impact on colloid mobilization, colloid hydrophobicity plays a key role in metal bioavailability. Carvalho et al. (1999) reported that the relative hydrophobicity of metalcolloid complexes may affect their bioavailability by enhancing their transport across membrane lipid bilayers.
In addition to directly affecting colloid properties, drying and rewetting of soils may affect the dispersibility of colloids by altering the physicochemical properties of the soil solution; for example, increasing DOC concentration of the soil solution enhances colloid stability (Kretzschmar et al., 1999). Moreover, air-dried soils are commonly used for various soil analyses. Although it is well documented that heavy metal and organic C concentrations in the extracts of air-dried and moist soils differ from each other (Wang et al., 2002; Tom-Petersen et al., 2004), studies of the effect on the colloid-bound fractions are absent. Thus, the results of this study may provide important information for the design of analytical procedures.
The effect of drying-induced hydrophobization on the amount and properties of dispersible colloids has not been investigated, and the underlying mechanisms of colloid release after drying are unknown. Therefore, the aim of this study was to investigate whether (i) drying of soil samples increases not only the hydrophobicity of the solid phase but also the hydrophobicity of dispersible colloids and (ii) drying of soil samples increases the colloid-bound and dissolved metal fractions.
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MATERIALS AND METHODS
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Soil Samples
The experiments were conducted with soil samples taken from the Ah horizons of the Berlin sewage farm (Buch soil) classified as Regosol (FAO, 1998) with sandy clay loam texture and the Berlin municipal park Tiergarten (TG) classified as Cambisol with sandy loam. They are both developed on quartenary fluvial sands; however, the sediment structure of the Tiergarten park was changed at the beginning of the last century by adding building rubble and dredged lake sediment. The sites were chosen because they were contaminated by heavy metals due to the impact of sewage water (Buch soil) and building rubble (TG soil). The experimental site on the sewage farm has been divided into three subplots of similar texture (labeled B1, B2, and B3). The entire site is characterized by a high small-scale heterogeneity. Additionally, we investigated the top soil (010 cm) of a former shooting range site near Gütersloh (GS), Lower Saxony, Germany, where oak trees have been growing for the past 30 yr. The soil is a podzolic Cambisol with a texture of loamy sand. It developed on fluvial sandy stream deposits of the Pleistocene. This soil was included in the study due to its high contamination by Pb, which is known to have a high affinity to colloids (Egli et al., 1999; Jensen et al., 1999; Denaix et al., 2001) and because of its high content of organic matter. We sampled the Aeh horizon, which was interrupted by the forest floor Oh horizon. For the analyses we mixed both horizons.
The samples were homogenized and sieved (2 mm) after the removal of roots and stones. The soils did not contain any significant amounts of aggregates before homogenization and sieving. The field-moist soil samples were put in plastic bags and stored in a refrigerator. An aliquot of the samples was dried at 25°C until constant weight and kept in air-tight plastic containers at room temperature until use.
To characterize the soil samples, the pH was determined in deionized water and 0.01 M CaCl2 solution using 10 g of air-dried soil and 25 mL of the respective solution. The suspension was left to stand overnight before the pH was measured using a WTW inoLab pH meter. Concentrations of organic C, N, and S (Corg, Norg, and Sorg) were measured by a C/N/S-analyzer (vario EL III; Elementar, Hanau, Germany) with soil dried at 105°C. From these parameters, the C/N-ratio was derived. For the determination of the water content, field-moist samples were dried at 25°C and 105°C until constant weight. Table 1 shows the analyzed properties of the sampled soil horizons. Total metal concentrations of the soil were determined by nitric acid-assisted digestion in closed vessels (180°C, 6 h). After cooling, the digested samples were filtered (Ø 150 mm, type 0790 1/2, ref. no. 10301645; Schleicher & Schuell, Dassel, Germany), transferred into 25-mL volumetric flasks, and filled to the mark with deionized water. The solutions were analyzed for Pb, Cu, Cd, and Zn concentrations. For measurement details, refer to the Analyses section.
The mobilization of colloidal and dissolved C, Cd, Cu, Pb, and Zn was studied using triplicate field-moist and air-dried (25°C) samples (<2 mm).
Experimental Setup
Based on the procedure of Curtin et al. (1994), who used a soil to water ratio of 1:10 to determine clay dispersibility, we chose a soil to water ratio of 15 g field-moist soil to 150 mL total solution volume in combination with turbidity measurements (see below). The weight of the dried soil samples was corrected for the loss of water. Samples were shaken for 16 h using an end-over-end-shaker at 18 rpm (GFL 3040, Burgwedel, Germany).
At the end of the experiment, pH and conductivity were measured in the suspensions before filtration (1.2-µm cellulose-nitrate filter, Type 11303-047N; Sartorius, Göttingen, Germany). We determined total organic carbon (TOC) concentrations and total concentrations of Cd, Cu, Pb, and Zn. We determined the turbidity, hydrophobicity, particle size, and zeta potential of the filtrate. An aliquot of the suspension was ultracentrifuged at 300 000 g for 1 h at 10°C (Beckman Optima TL, Krefeld, Germany) to separate colloids larger than 14 nm and with a density >1.2 g cm3 (based on Stoke's law) from the solution. The supernatant was transferred into plastic vessels, acidified with nitric acid, and analyzed for Cd, Cu, Pb, Zn, and DOC concentrations (considered as truly dissolved). The difference between concentrations in ultracentrifuged and not ultracentrifuged samples accounts for colloidal fractions (operationally defined) of the above-mentioned elements.
Analyses
Cadmium, Cu, Pb, and Zn concentrations of the colloidal suspensions were determined after microwave-assisted nitric acid digestion (CEM, MARS Xpress) according to the procedure described in USEPA Method 3015 (USEPA, 1994). The Zn measurement was performed using a flame atomic absorption spectrophotometer (1100; PerkinElmer, Milano, Italy) at a wavelength of 213.7 nm. Copper, Pb, and Cd analyses were determined using a graphite furnance atomic absorption spectrophotometer (Spectra AA 880Z; Varian, Darmstadt, Germany) (wavelength: 327.4, 283.3, and 228.8 nm, respectively). The organic C concentration of the suspensions and solutions was measured by a total organic carbon analyzer (TOC-5050 A; Shimadzu, Duisburg, Germany). The turbidity was determined by a turbidimeter (2100P ISO; Hach, Düsseldorf, Germany). Hydrophobicity of the colloids was measured as a partitioning coefficient between the aqueous suspension and a solid hydrophobic phase (C18 Prep LC Packing, diameter: 40 µm; Bakerbond Type 7025-00; JT Baker, Phillipsburg, NJ). Ten milliliters of filtered suspension were added to 30-mg C18 spheres and shaken for 2 h at 100 rpm (KS501 digital; IKA Labortechnik, Staufen, Germany) to allow for hydrophobic colloids to sorb onto the solids. Afterward, the suspensions were filtered over a 15 µm nylon gauze to remove the C18 spheres. The turbidity (T2) of the filtrate obtained was remeasured. Hydrophobicity (H) was calculated according to the following formula:
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where T1 is the turbidity of the suspension before C18 treatment. Further details about the method are described in Klitzke and Lang (2007).
The contact angle of the bulk soil samples as a measure for hydrophobicity of the solid phase was determined by indirect measurements. The field-moist samples were measured by the capillary rise method as described by Adamson (1990), and air-dried samples were measured by the Wilhelmy plate method (Bachmann et al., 2003). The use of two methods was considered essential due to the different wettabilities of the samples caused by the drying process. Figure 1 depicts the relation of the following parameters: (i) contact angle, (ii) hydrophobicity as determined by C18 spheres, and (iii) wettability.
The size distribution of the colloids was analyzed by dynamic light scattering (high performance particle size; Malvern Instruments, Herrenberg, Germany) and from the calculated particle size distribution curve (based on the volume) an average diameter was read off. The zeta potential was determined by a Zetasizer 2000 photon correlation spectrometer (Malvern Instruments) on the basis of electrophoretic mobility measurement of the colloids.
For each parameter of the complete sample set, a paired t test was conducted to determine significant differences between results from field-moist and air-dried samples. Because the properties of the Gütersloh soil differ greatly from the other soils included in the study, a second t test was performed based on the Buch and Tiergarten soils only. Statistically significant differences between the triplicates of field-moist and air-dried samples of individual soils were determined by an unpaired t test. We used a level of significance of 95% (P < 0.05) for both tests.
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RESULTS AND DISCUSSION
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Statistically significant differences for each parameter of the complete sample set between field-moist and air-dried samples are displayed in Table 2. The results of the t test are helpful only if there are no inverse effects and if all soils show the same tendency (i.e., increasing or decreasing concentrations of a parameter after drying). If this condition is not met, opposing effects cancel each other out, and the result of the t test is distorted. The significance of effects for individual soils can be indirectly determined by the error bars displayed in the graphs, representing twice the SD at a confidence level of 95%.
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Table 2. Significance of the effects of soil drying on the given soil characteristics. (+) indicates statistically significant differences between field-moist and air-dried samples (P < 0.05). They relate to assessed parameters across all examined soils.
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Influence of Drying on the Composition of the Dissolved Phase
For most of the soil samples, drying did not lead to a major and significant change in pH and conductivity (Tables 2 and 3). In the case of the Gütersloh soil, the observed increase in conductivity after drying may be attributed to the drastic increase in TOC of the suspensions.
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Table 3. pH and electrical conductivity in suspensions (s/w ratio 1:10) of field-moist and air-dried soil samples (±1 SD).
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The DOC concentrations in the air-dried samples were significantly higher than concentrations in the field-moist samples (Table 2), the change being especially pronounced for the Gütersloh soil (Fig. 2). These findings are in accordance with observations reported by Baskaran et al. (1994), Courchesne et al. (1995), and Kaiser et al. (2001).

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Fig. 2. Dissolved and colloidal Corg concentrations in suspensions of field-moist and air-dried samples (error bars depict 1 SD).
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In most samples, drying did not lead to a significant increase in dissolved concentrations of Cd and Zn (Fig. 3a and 3b). Because both metals have a very low affinity to organic C (McBride, 1994), their mobilization is not controlled by the increasing concentration in DOC.

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Fig. 3. (a) Dissolved and colloidal Cd concentrations in suspensions of field-moist and air-dried samples (error bars depict 1 SD). (b) Dissolved and colloidal Zn concentrations in suspensions of field-moist and air-dried samples (values of Gütersloh soil are below quantification limit; error bars depict 1 SD). (c) Dissolved and colloidal Cu concentrations in suspensions of field-moist and air-dried samples (error bars depict 1 SD; air-dried colloidal concentrations of the B1 sample not determined). (d) Dissolved and colloidal Pb concentrations in suspensions of field-moist and air-dried samples (error bars depict 1 SD).
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Dissolved Cu concentrations increased drastically after drying (Fig. 3c) and are statistically significant for all soils except for the Gütersloh soil. These findings are consistent with results reported by Tom-Petersen et al. (2004). The authors attribute this phenomenon to increased concentrations of DOC, which leads to the formation of dissolved organic Cu complexes. The exception of the Gütersloh soil may be explained by the extremely high Pb concentrations exceeding dissolved Cu concentrations by more than two orders of magnitude and therefore displacing Cu from being complexed by DOC.
In contrast to Cu, the effect of drying on the mobilization of dissolved Pb varied for the different samples. The Buch samples were constant, and the Tiergarten and the Gütersloh soils (according to the t test) significantly increased dissolved Pb concentrations after drying (Fig. 3d). In the Gütersloh soil, the increase can be ascribed to the extremely high concentration of DOC, leading to the mobilization of dissolved organic Pb complexes (McBride, 1994). In the Buch soils, we did not observe any increase in dissolved Pb concentrations despite increasing DOC concentrations. The higher affinity of Cu to soil organic matter (McBride, 1994) and the higher stability constants of Cu for humic acids (Lubal et al., 1998) and Cu-EDTA complexes (Lindsay, 1979) could explain why the drying-induced release of organic C does not lead to a mobilization of Pb in the Buch soils but to a preferred complexation of Cu. In the Gütersloh soil, however, the extremely high Pb concentrations exceed the Cu concentrations; therefore, despite the higher affinity of Cu for organic matter, it is displaced by Pb from the organic complex.
Influence of Drying on the Composition and Properties of Dispersible Colloids
All analyzed soils had substantial amounts of colloids in the suspension, except for the Tiergarten soil, which releases few if any colloids.
Based on turbidity measurements, the statistical analysis of all samples does not show any significant effect of drying on the mobilization of colloids (Table 2). This is because drying shows inverse effects for different soil samples: The Gütersloh soil shows increasing colloid mobilization after drying, whereas the Buch soils show decreased colloid mobilization and the Tiergarten soil shows constant colloid mobilization after drying. Therefore, in the statistical analysis, two opposing effects cancel each other out. The decrease and constancy in colloid mobilization are in contrast to results obtained from field studies reported by Denaix et al. (2001), who conducted their study on soil of similar texture and pH, and by Jann et al. (2002), who conducted their study on calcareous gravel, indicating colloid mobilization after re-wetting of dry soil. However, decreasing colloid concentrations are supportive of findings in sandy soils of different clay content as reported by Kjærgaard et al. (2004a, 2004b).
The decreasing amount of mobilized colloids may be explained by the following three processes:
- Enhanced aggregation during the drying process as described by Thill and Spalla (2003).
- Drying-induced disintegration of organomineral complexes as suggested by Peltovuori and Soinne, 2005. The break-up of weak bonds between organic matter and hydroxides (Haynes and Swift, 1989) may reduce the stability of mineral colloids, resulting in a decrease in colloid mobilization.
- Hydrophobization of colloids (see below).
The difference in changes of turbidity was most pronounced for the samples B1 and Gütersloh. Although soil B1 demonstrated a decrease in turbidity after drying, the Gütersloh soil showed the opposite (Fig. 4). The high content of organic matter of the latter creates the potential for a three-dimensional network forming under field-moist conditions (Schaumann et al., 2000). Such a cross-linked gel structure of organic material could impede the release of colloids into the solution. In previously dried soil, however, any such restrictive network that existed would have likely been destroyed and would take time to redevelop. Thus, on rewetting, colloids would initially be able to move freely into solution, resulting in an enhanced release of colloids. An additional factor that may have contributed to the increased release of colloids from the organic-rich Gütersloh soil is thought to be the disruption of biomass (Christ and David, 1996) and possible release of organic matter associated with microbial death and cell lysing on drying. The higher initial water content of the Gütersloh soil may also have been a factor.

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Fig. 4. Turbidity in the soil suspensions of field-moist and air-dried samples (error bars depict 1 SD).
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With the exception of the Tiergarten samples, our results demonstrate a significantly increasing contact angle of the solid phase after drying (Fig. 5 and Table 2), which is consistent with an increasing water repellency (Goebel et al., 2004). This result implies that drying increases hydrophobicity and agrees with observations reported by Dekker et al. (2001) and Hurraß and Schaumann (2006). The change in hydrophobicity of the dispersible colloids does not follow the change in hydrophobicity of the solid sample. We observed smaller changes in the hydrophobicity of the colloids, but in general they remained hydrophilic (Fig. 6). We postulate that drying renders the colloids of the solid phase hydrophobic, but these hydrophobic colloids are no longer suspended after drying. This assertion is supported by the work of Wan and Wilson (1994a, 1994b), who observed that hydrophobic colloids are less mobile. As a result, only colloids that are not affected by the hydrophobization process, i.e., hydrophilic colloids are found in the analyzed suspensions. Another possible explanation for the occurrence of hydrophilic colloids is the presence of amphiphilic organic molecules because they were found to be an important factor controlling wettability (Hurraß and Schaumann, 2006). Their nonpolar groups are thought to sorb onto the hydrophobic surface, whereas the polar groups would point toward the aqueous phase, rendering the surface hydrophilic and thus allowing better mobilization of colloids of hydrophobic samples.

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Fig. 6. Hydrophobicity of colloidal suspensions of field-moist and air-dried soil (error bars depict 1 SD).
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Our findings indicate that drying of the soil does not lead to a major change in the physicochemical properties of the suspensions: The zeta potential and the particle size of the suspended colloids remained constant (data not shown). The extremely high conductivity values of the Tiergarten soil (Table 3) account for a high ionic strength of the soil solution and explain the lack of colloids in the suspension.
Concentrations of colloidal organic C (COC) remained constant or showed an increase (Fig. 2) for most soils, with the differences being most pronounced and statistically significant (t test) for the Tiergarten and Gütersloh soils. Our results support the findings of Kjærgaard et al. (2004a, 2004b), who observed an increase in COC after drying. We explain this phenomenon by the disintegration of organomineral complexes (Peltovuori and Soinne, 2005) and the disruption of microbial biomass (Christ and David, 1996) in the C-rich Gütersloh soil.
Our results reveal no increase in the colloid-bound metal fraction (data not shown), as would be expected from suggestions in the literature (Denaix et al., 2001). We observed a clear decline in the concentrations and fractions of colloid-bound Cd and Zn (Table 2). Our data suggest a preferential cementation of inorganic particles of the soil matrix induced by the drying process, leading to a lower degree of colloid dispersibility after rewetting.
Colloid-bound Cu concentrations decreased in two soils after drying despite increasing COC concentrations. This implies that there is no correlation between these two parameters, although Cu has a high affinity to organic matter (McBride, 1994). These findings suggest that (i) colloidal Cu in these soil suspensions may be mainly bound to inorganic particles, which may have an organic surface coating, and (ii) because the suspensions of air-dried samples showed elevated concentrations of DOC, one might hypothesize an equilibrium between colloidal Cu and dissolved organically complexed Cu (i.e., high DOC concentrations could lead to a desorption of Cu from the colloids). This assumption would be in line with increasing concentrations of dissolved Cu in the suspensions of the air-dried samples.
Although the drying process leads to a significant decrease in colloidal Pb concentrations for the Buch and the Tiergarten soils, concentrations remain constant in the Gütersloh sample. If the Gütersloh soil is left out in the t test (Table 2), changes for the Buch and Tiergarten soils are significant. This difference could be ascribed to the lower pHH2O and the high organic C content of the Gütersloh soil, allowing for the formation of Pb-organic precipitates (Lang et al., 2005). However, the fractions of colloidal Pb for all soils (data not shown) remain unchanged by the drying process. For the Buch soils colloidal Pb accounts for between 70 and 96% of total Pb in suspension, whereas in the Gütersloh soil dissolved Pb is predominant. Similarly to Cu, the data set does not reveal any correlation between COC and colloidal Pb. These findings lead to the conclusion that colloidal Pb in the Buch soils is bound predominantly to inorganic colloids.
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CONCLUSION
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Our batch experiments showed that drying of the studied soils does not lead to a uniform increase in the concentration of water-dispersible colloids. We conclude that the influence of drying on the dispersibility of pedogenic colloids is likely to depend on their composition. In a C-rich matrix, mainly organic colloids are mobilized by soil drying, whereas in a more mineral matrix, (organo)-mineral colloids are immobilized, possibly due to enhanced cementation during the drying process. Drying-induced (im)mobilization of colloids does not always go along with the change in concentration of colloid-associated heavy metals. This indicates that drying does not only affect the mobilization of colloids but also the equilibrium between colloidal and dissolved species. Absolute concentrations of the investigated colloid-bound heavy metals were found to decrease in almost all soil samples for Cd and Zn and, in some soils, for Cu and Pb. This decrease may be attributed to the immobilization of colloids (as observed for Zn and Cd and, in some samples, for Pb) or to the mobilization of heavy-metal sorbing DOM leading to a redistribution of the metal between colloidal and dissolved phase (as observed for Cu). Because drying did not influence the physicochemical properties of the colloids, our results suggest that drying-induced colloid mobilization in the field is most likely due to shear forces (as explained by Jann et al., 2002) or the dispersion of macroaggregates (Kjærgaard et al., 2004a) rather than by a major change in physicochemical properties of the colloids. Future studies should assess whether the presented results are applicable to intact cores.
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ACKNOWLEDGMENTS
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We thank Claudia Kuntz for her help with laboratory analyses, Gabriele Schaumann for fruitful discussion, David Meredith for proofreading the manuscript, and the reviewers for helpful and constructive criticism and comments. This work was supported by the German Research Foundation (La 1398/2).
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