TECHNICAL REPORTS: SURFACE WATER QUALITY
Use of Industrial Byproducts to Filter Phosphorus and Pesticides in Golf Green Drainage Water Sheela G. Agrawal,* Kevin W. King, James F. Moore, Phil Levison, and Jon McDonald Golf courses are vulnerable to phosphate (PO43−) and pesticide loss by infiltration of the sandy, porous grass rooting media used and through subsurface tile drainage. In this study, an effort was made to remove PO43−, chlorothalonil, mefenoxam, and propiconazole in a golf green’s drainage water with a filter blend comprised of industrial byproducts, including granulated blast furnace slag, cement kiln dust, silica sand, coconut shell– activated carbon, and zeolite. To test this filter media, two 6-h storm events were simulated by repeat irrigation of the golf green after PO43− and pesticide application. Drainage flows ranged from 0.0034 to 0.6433 L s−1 throughout the course of the simulations. A significant decrease in the chlorothalonil load for the experimental run (with filter media) was observed compared with the control (without filter media) (p < 0.05). In general, percent reductions in chlorothalonil were very high (>80%) near peak flows. In contrast, filter media was not effective in removing PO43−, mefenoxam, or propiconazole (p > 0.05). Instead, it appears that the filter blend added PO43− to the effluent above flow rates of 0.037 L s−1. Overall, flow rate, the amount of filter media used, and contaminant properties may have influenced the filter media’s ability to remove contaminants. More research is needed to determine the optimal blend and configuration for the filter media to remove significant amounts of all contaminants investigated.
Copyright © 2011 by the American Society of Agronomy, Crop Science Society of America, and Soil Science Society of America. All rights reserved. No part of this periodical may be reproduced or transmitted in any form or by any means, electronic or mechanical, including photocopying, recording, or any information storage and retrieval system, without permission in writing from the publisher. J. Environ. Qual. 40:1273–1280 (2011) doi:10.2134/jeq2010.0390 Posted online 7 June 2011. Received 10 Sept. 2010. *Corresponding author (
[email protected]). © ASA, CSSA, SSSA 5585 Guilford Rd., Madison, WI 53711 USA
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here are over million acres of turfgrass (parks, roadsides, private and commercial lawns, golf courses, cemeteries, sod farms, etc.) in the United States, of which golf courses comprise approximately 3.2% (King and Balogh, 2006). Despite their seemingly small land area percentage, golf courses can adversely affect surface water quality because of the frequent applications of fertilizer and pesticides, irrigations, aerations, and mowing required to maintain healthy, playable turfgrass (Turgeon, 1996; Witteveen and Bavier, 1999; King and Balogh, 2006). According to the Golf Course Superintendents Association of America, the average golf course uses approximately 74 kg of phosphorus (P) per hectare of managed turf per year (Pimentel et al., 1991; USGS, 2006; GCSAA, 2009). This amount is more than twice that used in the agricultural sector and contributes to the degradation of surface waters by eutrophication (USGS, 2006; GCSAA, 2009). Although there is no comprehensive data set for annual pesticide use on golf courses, a few case studies have estimated an average usage between 4 and 270 kg a.i. ha−1 yr−1 (Kriner, 1985; Merrigan et al., 1996; Joyce, 1998; Schueler, 2000; Haith and Duffany, 2007; Magri and Haith, 2009). In contrast, the agricultural sector averages between 1 and 3.5 kg a.i. ha−1 yr−1 (Pimentel et al., 1991; USGS 2006; Haith and Duffany, 2007; Magri and Haith, 2009). As with fertilizers, excess pesticides and their residuals degrade surface water quality and can adversely affect aquatic species, birds, and humans (Cohen et al., 1999; Moore et al., 2002, Rohr et al., 2006). Golf courses are particularly vulnerable to P and pesticide loss because of the sandy, porous grass rooting media used and the presence of subsurface tile drainage (Pira, 1997; Marshall et al., 2001; Shuman, 2003; Soldat and Petrovic, 2008). The rooting media and tile lines promote rapid infiltration and removal of excess water from the course (Reddy et al., 1978; Mansell et al., 1985). Tile drainage also helps to maintain necessary water table depths for plant growth and sufficient soil void space to prevent soil compaction and rutting (King et al., 2006). The intended effect is to enhance turf playability, especially under seasonally saturated conditions and after storm events (Sims et al., 1998; Dils and Heathwaite, 1999; King et al., 2006; Algoazany et al., S.G. Agrawal, K.W. King, and P. Levison, USDA–ARS, Soil Drainage Research Unit, 590 Woody Hayes Dr., Columbus, OH 43210; J.F. Moore, U.S. Golf Association, 770 Sam Bass Rd., McGregor, TX 76657; J. McDonald, Kristar Enterprises, Inc., 360 Sutton Pl., Santa Rosa, CA 95407. Assigned to Associate Editor Gary Feyereisen.
Abbreviations: CKD, cement kiln dust; CS AC, coconut shell–activated carbon; DOC, dissolved organic carbon; EC, electrical conductivity; GBFS, granulated blast furnace slag; MDL, method detection limit; TSS, total suspended solids.
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2007; Gentry et al., 2000; Kinley et al., 2007). However, King et al. (2006) showed that dissolved P in golf course subsurface drainage waters exceeded concentrations that promote eutrophication and even P loads in agricultural drainage (Kladivko et al., 1999). Similarly, Petrovic and Larsson-Kovach (1996) observed a 62% infiltration loss of the water-soluble pesticide mecoprop in newly seeded, sandy, highly irrigated turf stands (Magri and Haith, 2009). Moreover, P and pesticides transported in subsurface drainage water bypass natural and managed surface filter processes, like riparian and vegetated buffer strips, and thus compound runoff loads to surface waters (Schwab and Thiel, 1963; Boyd et al., 2003; King et al., 2006; King et al., 2007). Current methods used to limit P and pesticide loss from golf courses to surface waters involve the implementation of agronomic best management practices and include adjusting the timing and rate of application, the type of fertilizer or pesticide used, the volume of irrigation water, and mowing heights, among others (Oguz, 2004). More recently, there has been an interest in capturing and filtering drainage effluent at tile end. For example, King et al. (2010) reported 51.6, 58.2, and 28.8 average percent removals of phosphate (PO43−), chlorothalonil, and metalaxyl, respectively, from simulated drainage water by end-of-tile filters filled with activated alumina and carbon and zeolite. Similarly, McDowell et al. (2008) used slag to remove dissolved reactive phosphorus in a field trial. The investigators observed a 60 to 69% reduction in drainage water–dissolved reactive phosphorus loads after the water was passed through tile drains that were backfilled with slag or fitted with slag-filled filter socks. Generally, materials high in Ca, Fe, Al, and Mg are very effective at removing P through sorption (adsorption and precipitation). Over the past 25 yr, sorption of dissolved P by industrial byproducts and natural materials rich in these constituents (e.g., blast furnace slag, iron oxide mine tailings, fly ash, zeolite, bone char, and limestone) has received considerable attention (Bhargava and Sheldarkar, 1993; Johansson and Gustafsson, 2000; Agyei et al., 2002; Özacar, 2003; Namasivayam and Sangeetha, 2004; Oguz, 2004, 2005; Drizo et al., 2002, 2006; Shilton et al., 2006, Penn et al., 2007, 2009; McDowell et al., 2008). Similarly, biomass-derived byproducts, such as biochar and activated carbons, can sorb dissolved P and, more importantly, pesticides. Not only is use of these materials very effective and inexpensive, but it also has the potential to significantly reduce the waste streams of several industrial byproducts. Furthermore, many of these byproducts
could potentially be recycled as slow-release P fertilizers once their removal capacities have been exhausted (Bansiwal et al. 2006; de-Bashan and Bashan, 2007; Bird and Drizo, 2009). In this study, we investigated the ability of a blend of four industrial byproducts—blast furnace slag, cement kiln dust, coconut-shell activated carbon—and two natural materials—zeolite (as clinoptilolite) and silica sand—to remove dissolved P and three pesticides—chlorothalonil (2,4,5,6-tetrachloro-1,3-benzenedicarbonitrile), propiconazole (1-[{2-(2,4-dichlorophenyl)-4-propyl-1,3-dioxolan-2-yl} methyl]-1H-1,2,4-triazole), and mefenoxam ((R)-2-[(2,6dimethylphenyl) methoxyacetylamino] propionic acid methyl ester)—from a tile-drained practice golf green under stormsimulated conditions. Ultimately, we aimed to indentify inexpensive materials for use in removing P and pesticides from tile drainage without compromising overall effluent water quality.
Materials and Methods Industrial Byproducts and Minerals The materials used and their sources are listed below. These materials were chosen based on their hydraulic conductivities determined in previous laboratory batch tests and as reported in the literature. Also, these materials did not leach appreciable quantities of heavy metals like Hg, Cd, and As. Each material’s properties are shown in Table 1. 1. Granulated blast furnace slag (GBFS): Lafarge North America, Illinois 2. Cement kiln dust (CKD): Larfarge North America, Michigan 3. Zeolite (clinoptilolite): St. Cloud Mining Company, New Mexico 4. Coconut shell–activated carbon (CS AC): Carbon Link Corp., Ohio 5. Silica sand (99.5%): Fairmount Minerals and Subsidiaries, Best Sand, Ohio
Site Description and Filter Design Ridgewood Country Club is a private, regulation length, 18-hole golf course located in Waco, TX, that has been in operation since 1946. The course spans a total of 0.69 km2 and has a USGA rating of 71.4 and a slope rating of 128 on Bermuda grass. Runoff and drainage from the course ultimately enters nearby Lake Waco, which is a well known, nutrient-polluted surface water body (Dworkin, 2003).
Table 1. Material properties. Material†
GBFS‡ Zeolite Silica sand CS AC CKD
Particle diameter mm 2.00−2.80 2.40−3.40 0.30−0.50 0.6−1.70 0.05), suggesting that the filter treatment does not change effluent water quality with respect to TSS. In contrast, changes in pre- and postfilter interaction EC measurements (mS cm−1) were statistically significant, suggesting that the filter media did influence EC, specifically by increasing it. However, this increase did not adversely affect overall effluent water quality (Table 2).
Upon arrival, samples were unpacked and stored below 4°C. The samples were analyzed for PO43−, chlorothalonil, mefenoxam, and propiconazole within 28 d. Before analysis, samples were vacuum filtered through a 0.45-μm pore diameter glass fiber membrane. Phosphate concentrations in water samples were determined colorimetrically by the ascorbic acid reduction method using a QuikChem 8000 FIA automated ion analyzer (Lachat Instruments, Milwaukee, WI) (Parsons et al., 1984; USEPA, 1995). The method detection limit (MDL) for PO43− was 0.003 mg L−1. Dissolved organic carbon concentrations were determined by the heated persulfate oxidation method on an Aurora 1030W Total Organic Carbon Analyzer (O I Analytical, College Station, TX) with in-line sample acidification and sparging (MDL = 0.04 mg L−1) (USEPA, 1995; Eaton et al., 1998). Total suspended solids (TSS) measurements were determined by the change in mass of a preweighed, 45-μM glass fiber filter on sample filtration (USEPA, 1995). Chlorothalonil, mefenoxam, and propiconazole residues were determined using a Saturn 2200 gas chromatography mass spectrometer (Varian, Inc., Palo Alto, CA) (USEPA, 1995); MDL values were 0.098, 0.10, and 0.01 μg L−1 for each pesticide, respectively. Before pesticide extraction, each filtered sample was fortified with 1 mL of methanol and a terbutylazine standard (final concentration = 500 μg L−1). The samples were then extracted using 10-mL Bond Elut C-18 cartridges (Varian) preconditioned with methanol. After a 45-min air-drying period, each cartridge was eluted with four 0.5-mL aliquots of ethyl acetate, dried under N2 gas, and reconstituted with 1 mL ethyl acetate containing acetonaphthalene (final concentration, 1276
Results
Table 2. Comparison between typical surface water quality parameter values and study values.† Water quality parameter‡ pH DOC, mg L−1 EC, mS cm−1 TSS,mg L−1
Typical surface water parameter values
Study values
5.8–8.6 1.00–20.0 0.05–1.5 0–263§
6.75 ± 0.32 10.42 ± 0.77 0.20 ± 0.11 2.53 ± 1.83
† From Wetzel (2001) and USEPA (2003). ‡ DOC, dissolved organic carbon; EC, electrical conductivity; TSS, total suspended solids. § Values represent the range of acceptable concentrations in discharged waters between the four states in the United States (Hawaii, Utah, North Dakota, and South Dakota) that have TSS standards. The USEPA does not regulate TSS. Journal of Environmental Quality • Volume 40 • July–August 2011
Statistical differences in the pH and DOC concentrations of pre- and postfilter interaction samples were not as clearly delineated. For example, significant changes in pH were observed on Day 1 (without filter media) and Day 2 (with filter media), thus making it difficult to discern the effects of the filter media on pH. However, despite these discrepancies, the differences observed for both runs did not negatively affect water quality. In other words, all pH and DOC values fell within their respective ranges for good effluent water quality. The pH across both runs averaged 6.75 ± 0.32 mg L−1 (SD), whereas DOC averaged 10.42 ± 0.77 mg L−1 (Table 2). Drainage inflow rates differed significantly between Day 1 (without filter media) and Day 2 (with filter media), with the higher median flow rate occurring on Day 1 (0.138 L s−1), than on Day 2 (0.108 L s−1) (P < 0.001). The differences in flow over time between the days can be seen in Fig. 2. In sequential order, peak flows for Day 1 were 0.643 L s−1 (at t = 3600 s), 0.643 L s−1 (t = 9600 s), and 0.554 L s−1 (t = 18600 s), respectively. Fig. 2. Day 1 (control, without filter media) and Day 2 (experimental, with filter media) Peak flows for Day 2 were 0.234 L s−1 (t = 2700 hydrographs. s), 0.583 L s−1 (t = 9300 s), and 0.628 L s−1 (t = In contrast, reductions in PO43−, mefenoxam, and propi16,500 s), respectively. conazole between the Day 1 and Day 2 runs were not statisPrefilter contaminant loads also differed between the 2 d. tically different (P > 0.05). Instead, it appears that the filter For example, the magnitude of the cumulative prefilter PO43− media blend added in excess of 146% of the incoming PO43− load on Day 1 was 3580 mg, whereas that of Day 2 was 3086 load to the effluent. The addition of PO43− to the effluent by mg. Conversely, the magnitudes of mefenoxam, propiconazole, the filter media will herein be referred to as “offloading.” The and chlorothalonil loads were greater on Day 2 vs. Day 1. Day cumulative PO43− load before filter interaction was 3086.10 1 prefilter cumulative loads of mefenoxam, propiconazole, and mg, whereas that of the effluent was 7605.29 mg. The total chlorothalonil were 148, 3, and 38 mg, respectively, whereas amount of PO43− offloaded per kilogram of filter media for Day those on Day 2 were 416, 10, and 98 mg, respectively. 2 was 300 mg kg−1. Influent (prefilter interaction) contaminant loading rates However, samples with flow rates below 0.037 L s−1 (the varied with drainage flow rate. Phosphate exhibited the clearest first five samples collected postirrigation) exhibited statistitrend, with its loading rate increasing as a function of flow rate cally significant reductions in PO43− between prefiltered and (Fig. 3). This trend was less clear for propiconazole, chlorothafiltered water (and compared with Day 1 samples) (P < 0.001). lonil, and mefenoxam (Fig. 3). The mean percent reduction in PO43− (with a 95% confiDespite the variability in flow rates and contaminant predence interval) for this low flow interval was 22 ± 4.5%. This filter loading rates, a real decrease in the chlorothalonil load amounted to only a 0.19% reduction in the total incoming P was observed for Day 2 (with filter media) when compared load over the course of the run and was far outweighed by the with Day 1 (without filter media) (P < 0.001). The median 146% PO43− increase in the filtered water. For flow rates greater decrease in chlorothalonil for the Day 2 load was 69% (average than 0.037 L s−1, the PO43− offloading rate was positively corand 95% confidence interval, 57 ± 13%), whereas that of the related with flow rate (Fig. 5). control was 0%. The highest reduction of chlorothalonil was 96% and occurred at time = 45 min (2700 s), flow = 0.234 Discussion L s−1, and a prefilter chlorothalonil load = 4.06 mg. Percent Previous research has identified zeolite, CS AC, GBFS, chlorothalonil removed as a function of time and flow rate is CKD, and to some extent silica sand, as suitable PO43− sorseen in Fig. 4. In general, chlorothalonil removal was very high bents (Johansson and Gustafsson, 2000; Oguz, 2004, 2005). (>80%) near peak flows. However, in this study, despite favorable drainage pH to supSignificant quantities of chlorothalonil were also removed port PO43− removal, it appears that high inflow rates, especially −1 at even higher flow rates than 0.234 L s . For example, 94 and those greater than 0.037 L s−1, limited contact time with these 87% of chlorothalonil were removed at flow rates of 0.583 L s−1 materials and thus PO43− removal. McDowell et al. (2008) and 0.540 L s−1, respectively. Furthermore, contaminant loads observed a similar high flow/short contact time trend in the at these flow rates were significantly greater than at 0.234 L s−1 end-of-fluvarium filter sock investigation previously men(t = 45 min), and thus larger absolute loads of chlorothalonil tioned. The authors also attribute the observed low P removal were removed. to the small quantity, and ultimately small surface area, of filter Agrawal et al.: Phosphorus and Pesticide Removal by Industrial Byproducts
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Fig. 3. Day 1 (control run, without filter media) and Day 2 (experimental run, with filter media) PO43−, chlorothalonil, mefenoxam, and propiconazole loading rates (mg s−1) as a function of flow rate (L s−1).
material used. In contrast, Korkusuz et al. (2005) averaged 44% PO43− removal from wastewater, flowing at 2.1 L s−1, by using over 11 Mg of slag. On an even larger scale, Shilton et al. (2006) used nearly 19 Gg slag over a 5-yr period to capture 77% P from wastewaters averaging flows of 1389 L s−1 (retention time on the filters was approximately 3 d). Although these last two studies used slag-based filters, the results nonetheless support the idea that a very large quantity of filter media is necessary to accommodate high incoming flows. Thus, it may be that the current study’s filter system should be completely redesigned or modified to incorporate significantly larger quantities of the investigated filter materials. The 0.19% PO43− removal was dwarfed by the 146% increase in the effluent PO43− load beyond the 0.037 L s−1 flow threshold. The quantity of PO43− offloaded per kilogram of filter media was significantly greater than that observed in bench-scale, leachate batch experiments conducted before this study for the same blend (refer to USEPA [2008] for batch experiment method). The materials in the current study 1278
offloaded approximately 300 mg PO43− per kilogram of filter media, compared with 5 mg kg−1 in the batch experiments. In the batch experiments, a fixed volume of water was in contact with the filter blend in slowly rotating Teflon test tubes such that flow out of the system did not occur. Because this same water was always in contact with the filter media, flow rate was considered to be negligible compared with the current study. Thus it appears that flow rate affected not only the efficacy of contaminant removal but also the degree of PO43− offloading. It is not known which material or materials in the filter blend are offloading PO43−. Because this blend is unique to this study, it has not been characterized by others. However, PO43− offloading has been observed for some filter media constituents, namely slag. Shilton et al. (2006), for example, documented an increase in effluent PO43− after 5 yr of slag-based, continuous filtration because of filter saturation. Whether the authors observed a large initial flush of PO43− is unknown. With respect to the current study, further investigation is needed to determine which filter media constituent or constituents Journal of Environmental Quality • Volume 40 • July–August 2011
are offloading PO43−, whether it continues to offload PO43− over time before saturation, and how much PO43− can be accommodated before filter saturation. Chlorothalonil removal was extremely high for high incoming flows, which is in contrast to the observations reported by King et al. (2010). In their investigation, the highest percent removals of chlorothalonil were seen during the rising and receding limbs of the generated hydrographs. The reason for chlorothalonil’s behavior in the present study is unclear, but it may be due to the different types of materials used (with the exception of zeolite) in the present study versus those used by King et al. (2010). The variability in pesticide removal in the present study is a reflection of not only the high incoming flow rates and the amount of material used but also of each pesticide’s physical and chemical properties (Lyman et al., 1990; Mackay et al., 2006). The water solubili−1 ties (Cs) and partition coefficients (log Koc) of Fig. 4. Flow rate (L s ) and percent removal of chlorothalonil over time (s). mefenoxam (Cs = 100 mg L−1; log Koc = 1.46– 2.46) and propiconazole (Cs = 26 g L−1; log Koc = 2.59– 3.06) differ significantly from those of chlorothalonil (Cs = 0.6 mg L−1; log Koc = 3.20–4.15) and may thus account for their comparatively insignificant removal (Gardner and Branham, 2001; Marrs and Ballantyne, 2004). That is, propiconazole and mefenoxam are significantly more soluble than chlorothalonil, whereas chlorothalonil exhibits a greater tendency to sorb to soils. Again, optimizing the filter blend or changing the design could improve propiconazole and mefenoxam removal. Although the GBFS, CS AC, CKD, sand, and zeolite filter blend removed chlorothalonil but not PO43−, mefenoxam, or propiconazole, it should still be pursued for large-scale implementation, especially because of the ease of acquisition of its constituents and good performance in prior batch experiments and other larger-scale investigations. Moreover, with the exception of PO43− offloading, the blend did not adversely affect effluent Fig. 5. Filter blend PO43− offloading rate (the rate at which the filter materials add 3− −1 −1 water quality. Further investigation is needed to determine PO4 to the incoming drainage water) (mg s ) vs. flow rate (L s ). the optimum blend of byproducts and minerals needed de-Bashan, L.E., and Y. Bashan. 2007. Fertilizer potential of phosphorus reto remove significant quantities of PO43−, chlorothalonil, and covered from wastewater treatments. p. 179–184. In E. Velazquez-Perez and C. Rodriguez-Barrueco (ed.) First international meeting on micromefenoxam as well as other contaminants of interest. In general, bial phosphate solubilization series: Developments in plant and soil scilarger quantities of the filter material or a new filter design are ences. Springer, Dordrecht, The Netherlands. needed to accommodate the green’s high drainage flows to allow Bhargava, D.S., and S.B. Sheldarkar. 1993. Use of TNSAC in phosphate adsorption studies and relationships. Water Res. 27:303–312. for sufficient contact time for contaminant removal.
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Journal of Environmental Quality • Volume 40 • July–August 2011
