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Sulfadimethoxine Degradation Kinetics in Manure As Affected by Initial Concentration, Moisture, and Temperature

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Sulfadimethoxine Degradation Kinetics in Manure As Affected by Initial Concentration, Moisture, and Temperature Published online October 27, 2006 Sulfadimethoxine Degradation Kinetics in Manure as Affected by Initial Concentration, Moisture, and Temperature Q.-Q. Wang, S. A. Bradford, W. Zheng, and S. R. Yates* ABSTRACT However in Europe, a new trend has developed with in- Sulfadimethoxine is a widely used sulfonamide veterinary antibiotic creased therapeutic use of antibiotics (Alder et al., 2001). and could be a source of agricultural contamination. Therefore, infor- After the application to animals, antibiotics will even- mation is needed about its degradation kinetics in manure under aer- tually enter the environment. In fish farming, antibiotics obic conditions. Based on the analysis of first-order kinetics and the are given as feed additives, resulting in a direct release assumption that sulfadimethoxine availability for degradation in ma- of antibiotics into the aquatic environment (Thurman nure could be limiting, a new kinetic model was developed and was et al., 2002). It was estimated that |70 to 80% of drugs found to fit the degradation kinetics well. The degradation rate in administered to fish enters the environment and anti- sterile manure was found to be much lower than in nonsterile manure, biotic residues with significant antibacterial activity were indicating that biodegradation was significant. In biologically active found in the sediment of fish hatcheries (Samuelsen et al., manure, the degradation rate constant decreased with increasing ini- tial concentration of sulfadimethoxine, implying that the activity of 1992). However, the major route through which veteri- the degrading microorganisms was inhibited. Increasing moisture or nary antibiotics enter the environment is the excretion temperature was found to increase sulfadimethoxine degradation in of feces and urine from medicated animals in livestock manure. Mixing manure containing high levels of sulfadimethoxine with and poultry farming, and the subsequent application of manure containing lower levels may result in more rapid degradation, contaminated manure as fertilizer into agricultural land thus greatly diminishing sulfadimethoxine contamination in manure and (Ariese et al., 2001; Boxall et al., 2003). It was found that significantly reducing sulfadimethoxine inputs into the environment. as much as |40 to 90% of the administrated antibiotics During treatment, keeping the manure moist and storing in a mod- are excreted as parent compounds by animals after erately warm place under aerobic conditions may also help to diminish medication (Halling-Sorensen et al., 2001; Winckler and sulfadimethoxine contamination. Grafe, 2001). The concentration of antibiotics in manure excreted from treated animals can be as high as several 21 OR PURPOSES OF THERAPEUTICAL TREATMENT AND GROWTH hundreds of mg kg (Migliore et al., 1997; De Liguoro FPROMOTION, veterinary antibiotics are widely adminis- et al., 2003). Soil and water contamination from manure tered to animals in the agricultural industry. It was esti- fertilization and at concentrated animal operations has mated that more than 22 million pounds of antibiotics been frequently reported (Rabolle and Spliid, 2000; Hams- were used to treat farm animals and pets in the USA dur- cher et al., 2002; Boxall et al., 2002). There is concern that ing 2002 [Animal Health Institute (AHI), 2003]. Another residual concentrations of antibiotics in agricultural soil study reports that nontherapeutical use of antibiotics for can easily reach levels similar to pesticides if the manure livestock production in the USA has exceeded 24.6 mil- loading for fertilization increases to the kilograms per lion pounds per year (Mellon et al., 2001). In Europe, the hectare level (Thiele-Bruhn, 2003). total consumption of veterinary antibiotics in 1999 was The widespread contamination of antibiotics in the estimated to be 10.3 million pounds [FEDESA (European environment may put human health and sensitive eco- Federation of Animal Health), 2001]. The application of systems at risk. First, exotic antibiotics may alter the antibiotics as growth promoters in feed additives has been composition and diversity of indigenous soil microbial forbidden in Switzerland since 1999. To date, the non- communities, which are of fundamental importance for therapeutical use of antibiotics as growth promoters in ecosystem function in nutrient cycling, decomposition, Europe is almost completely restricted and the relevant and energy flow (McCracken and Foster, 1993; Schmitt consumption is quickly declining (Thiele-Bruhn, 2003). et al., 2004). Second, exotic antibiotics may cause the for- mation of resistance, even cross and multiple resistances, in organisms in the environment (Al-Ahmad et al., 1999; Q.-Q. Wang, S.A. Bradford, W. Zheng, and S.R. Yates USDA-ARS, Sengelov et al., 2003) and possibly threaten human and U.S. Salinity Lab., 450 W. Big Springs Rd., Riverside, CA 92507. animal health by diminishing the success of antibiotic W. Zheng, Dep. of Environmental Sciences, Univ. of California, Riv- treatment. Evidence has been presented that antibiotic erside, CA 92521. Q.-Q. Wang, Dep. of Chemistry, Delaware State Univ., Dover, DE 19901. The use of trade, firm, or corporation names resistant genes from microorganisms in the environment in this publication is for the information and convenience of the can be transferred directly to humans (Rhodes et al., 2000). reader. Such use does not constitute an official endorsement or ap- Third, widespread contamination of veterinary antibiotics proval by the United States Department of Agriculture or the Ag- exposes humans and animals to a constant low concentra- ricultural Research Service of any product or service to the exclusion Reproduced from Journal of Environmental Quality. Publishedof by ASA, CSSA, others and SSSA. All copyrights reserved. that may be suitable. Received 8 May 2006. *Corresponding tion of antibiotics. Leaching and runoff of antibiotics from author ([email protected]). manure-fertilized lands is threatening the quality of drink- ing water (Hirsch et al., 1999; Kolpin et al., 2002). Though Published in J. Environ. Qual. 35:2162–2169 (2006). the effects of long-term exposure to low concentrations of Technical Reports: Organic Compounds in the Environment doi:10.2134/jeq2006.0178 antibiotics are not yet clear, the potential danger result- ª ASA, CSSA, SSSA ing from veterinary antibiotic contamination to human 677 S. Segoe Rd., Madison, WI 53711 USA and animal health cannot be neglected. 2162 WANG ET AL.: SULFADIMETHOXINE DEGRADATION KINETICS IN MANURE 2163 Focusing on eliminating the contamination caused by (certified), and sodium azide (certified) were purchased from veterinary antibiotics, numerous studies have been per- Fisher (Fair Lawn, NJ). Acetone (HPLC grade) was purchased formed to investigate the degradation of antibiotics in from Burdick & Jackson (Muskegon, MI). manure (Kuhne et al., 2000; Teeter and Meyerhoff, 2003), Steer manure (Earthgro, Marysville, OH 43041) was pur- soil (Gilbertson et al., 1990; Marengo et al., 1997), and chased from K-Mart at Riverside, CA. Manure was sieved using a 4-mm sieve and then air-dried in the laboratory at 258C water (Alexy et al., 2004; Boreen et al., 2004). Aerobic for 2 d. The moisture content was determined to be 39%. Ma- conditions were always found to be beneficial to the deg- nure pH measured at manure/water ratio 5 1:2 (in wet weight) radation of antibiotics in manure and water (Kuhne et al., was 8.37. Organic carbon content and maximum water-holding 2000; Ingerslev et al., 2001). Along with degradation and capacity were 14 and 155%, respectively. transport of veterinary antibiotics in the subsurface, ad- sorption of antibiotics in soil with and without manure Sorption Experiments has also been investigated (Rabolle and Spliid, 2000; Sulfadimethoxine sorption in manure was determined using Thiele-Bruhn and Aust, 2004). the batch equilibration procedure. All experiments were per- Rather than developing technologies to enhance the formed in triplicates. Sulfadimethoxine solutions at 5 concen- degradation of antibiotics in soil and to prevent them trations ranging from 35.3 to 158.6 mM were prepared in water from contaminating surface and ground water, a more with 0.01 M NaCl and 0.2% NaN3. Ten mL of sulfadimethoxine effective and practical way to reduce contamination from solutions were added into 20-mL serum bottles with 5.00 g (wet veterinary antibiotics would be eliminating the antibi- weight) sterile manure. The bottles were sealed with aluminum otics in the manure before its application to agricultural caps with Teflon-coated butyl rubber septa, and were shaken land as fertilizer (Wang et al., 2006). However, the deg- horizontally in a reciprocating shaker (Eberbach, Ann Arbor, radation kinetics of antibiotics in manure, as well as the MI) at a vigorous rate for 3 h at 25 6 0.58C. A portion of slurry effects of various factors on degradation kinetics, has from each bottle was transferred into 1.5-mL polypropylene rarely been investigated. A simple first-order model has centrifuge tube and centrifuged at 14 000 rpm for 3 min in a microcentrifuge (Spintron, Meuchen, NJ). Supernatant from generally been used to fit the degradation kinetics of each tube and the original sulfadimethoxine solutions were antibiotics even though the fitting results were poor in analyzed using HPLC to obtain the sulfadimethoxine concen- almost every case (Gilbertson et al., 1990; Ingerslev and tration. Blank controls were also analyzed. A preliminary Halling-Sorensen,
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