This article was downloaded by: [Eindhoven Technical University] On: 24 January 2015, At: 19:35 Publisher: Taylor & Francis Informa Ltd Registered in England and Wales Registered Number: 1072954 Registered office: Mortimer House, 37-41 Mortimer Street, London W1T 3JH, UK

Journal of Environmental Science and Health, Part B: Pesticides, Food Contaminants, and Agricultural Wastes Publication details, including instructions for authors and subscription information: http://www.tandfonline.com/loi/lesb20

Sorption and transport of five sulfonamide antibiotics in agricultural soil and soil–manure systems ab

b

b

c

b

a

Na Wang , Xinyan Guo , Jing Xu , Lijun Hao , Deyang Kong & Shixiang Gao a

State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing, China b

Nanjing Institute of Environmental Science, Ministry of Environmental Protection of China, Nanjing, China c

College of Science, China Pharmaceutical University, Nanjing, China Published online: 24 Nov 2014.

Click for updates To cite this article: Na Wang, Xinyan Guo, Jing Xu, Lijun Hao, Deyang Kong & Shixiang Gao (2015) Sorption and transport of five sulfonamide antibiotics in agricultural soil and soil–manure systems, Journal of Environmental Science and Health, Part B: Pesticides, Food Contaminants, and Agricultural Wastes, 50:1, 23-33, DOI: 10.1080/03601234.2015.965612 To link to this article: http://dx.doi.org/10.1080/03601234.2015.965612

PLEASE SCROLL DOWN FOR ARTICLE Taylor & Francis makes every effort to ensure the accuracy of all the information (the “Content”) contained in the publications on our platform. However, Taylor & Francis, our agents, and our licensors make no representations or warranties whatsoever as to the accuracy, completeness, or suitability for any purpose of the Content. Any opinions and views expressed in this publication are the opinions and views of the authors, and are not the views of or endorsed by Taylor & Francis. The accuracy of the Content should not be relied upon and should be independently verified with primary sources of information. Taylor and Francis shall not be liable for any losses, actions, claims, proceedings, demands, costs, expenses, damages, and other liabilities whatsoever or howsoever caused arising directly or indirectly in connection with, in relation to or arising out of the use of the Content. This article may be used for research, teaching, and private study purposes. Any substantial or systematic reproduction, redistribution, reselling, loan, sub-licensing, systematic supply, or distribution in any form to anyone is expressly forbidden. Terms & Conditions of access and use can be found at http:// www.tandfonline.com/page/terms-and-conditions

Journal of Environmental Science and Health, Part B (2015) 50, 23–33 Copyright © Taylor & Francis Group, LLC ISSN: 0360-1234 (Print); 1532-4109 (Online) DOI: 10.1080/03601234.2015.965612

Sorption and transport of five sulfonamide antibiotics in agricultural soil and soil–manure systems NA WANG1,2, XINYAN GUO2, JING XU2, LIJUN HAO3, DEYANG KONG2 and SHIXIANG GAO1 1

State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing, China Nanjing Institute of Environmental Science, Ministry of Environmental Protection of China, Nanjing, China 3 College of Science, China Pharmaceutical University, Nanjing, China

Downloaded by [Eindhoven Technical University] at 19:35 24 January 2015

2

Animal manure application is a main spreading route of veterinary antibiotics in soil and groundwater. The sorption and leaching behavior of five commonly used sulfonamides in five typical soil and soil/manure mixtures from China were investigated in this study. Results showed that the empirical Freundlich equation fits well the sorption behavior of selected sulfonamides (r2 was between 0.803 and 0.999, 1/n was between 0.68 and 1.44), and pH and soil organic carbon (OC) were the key impact factors to sorption and leaching. Addition of manure was found to increase the Kd values of sulfonamides in five different soils, following the rules that the more polar substances, the more increased extent of sorption after manure amendment (5.87 times for sulfadiazine with Log Kow D ¡0.09, and 2.49 times for sulfamethoxazole with Log Kow D 0.89). When the simulated rainfall amount reached 300 mL (180 mm), sulfonamides have high migration potential to the groundwater, especially in the soil with low OC and high pH. However, manure amendment increased the sorption capacity of sulfonamides in the top layer, thus it might play a role in decreasing the mobility of sulfonamides in soils. The systematic study would be more significant to assess the ecological risks and suggest considering the influence of manure amendment for the environmental fate of antibiotics. Keywords: Sulfonamides, sorption, transport, leaching, manure amendment.

Introduction Large amounts of veterinary antibiotics are used globally to treat the disease and protect the health of animals. The usage of veterinary antibiotics in China (including nontherapeutic uses as feed additives) is greater than that in most other countries. In a survey of 2007, almost half of the 210,000 tons of antibiotics produced in China ended up in livestock, which was about 10 times higher than that in the United States and about 300 times higher than that in the United Kingdom.[1] Sulfonamides are synthetic veterinary antibiotics that are most widely used veterinary antibiotics in China, European Union, and some developing countries because of their low costs.[2,3] Chemical structures of selected sulfonamides are shown in Figure 1, and their pKa1 and pKa2 indicate the ampholytic features of sulfonamides, which are listed in Table 1.[4] Address correspondence to Shixiang Gao, State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing 210093, China; E-mail: [email protected] Received June 11, 2014. Color versions of one or more of the figures in the article can be found online at www.tandfonline.com/lesb.

Sulfonamides are poorly absorbed in animal tissues, and subsequently, approximately 50% are excreted as a parent compound and approximately 30% as acetyl conjugate.[5] Furthermore, it is reported that the N-acetyl derivative of sulfonamide antibiotics can be deacetylated to the parent compound during manure storage.[6] After repeated manure application, sulfonamides with their metabolites tend to persist and accumulate in soils and are then released to groundwater and surface water by infiltration and runoff, respectively.[7–10] Long-term exposure to low concentrations of these antibiotics could be toxic to nontarget terrestrial and aquatic organisms.[1,11] Therefore, investigation of the sorption and leaching behavior of these antibiotics in soils is a first logical step to assess the ecological risks and then develop pollution control strategies. Recently, some studies focusing on soil sorption and desorption of sulfonamides showed that sorbent properties may play a significant role in soil sorption. However, the sorption study of sulfonamides in soil remains incomplete because some studies were carried out only in soils without manure[12,13]; some studies were limited only to sorption, and supporting leaching studies are lacking.[14–16] Accordingly, the overall aim of the present study was to investigate the sorption and leaching behavior of five commonly

Downloaded by [Eindhoven Technical University] at 19:35 24 January 2015

24

Wang et al.

Fig. 1. Chemical structure of studied sulfonamides (SDZ: sulfadiazine, SMR: sulfamerazine, SMZ: sulfamethazine, SDM: sulfadimethoxine, SMX: sulfamethoxazole).

used sulfonamides in five typical soil and soil/manure mixtures from China to assess the potential mobility of sulfonamides to surface and groundwater. The effects of soil physicochemical properties, presence of manure, soil organic carbon (OC), and pH on the sorption and leaching of sulfonamides were also investigated.

Materials and methods Reagents, chemicals, and materials

(SMX) were obtained from Dr. Ehrenstorfer Inc. (Augsburg, Germany). Sulfamethoxazole-d4 (SMX-d4) was obtained from Toronto Research Chemicals Inc. (North York, Ontario, Canada). Methanol and acetone (HPLC grade) were obtained from Merck (Darmstadt, Germany). Calcium chloride dihydrate (CaCl2¢2H2O >99% purity) and phosphoric acid (analytical reagent grade) were purchased from Nanjing Chemical Reagent Co., Ltd. (Nanjing, China). Diatomite (10–20 orders) was obtained from Dionex (Dionex, Sunnyvale, CA, USA). Deionized water was purified by an onsite Milli-Q high performance reverse osmosis system (Millipore, Boston, MA, USA).

Sulfadiazine (SDZ), sulfamerazine (SMR), sulfamethazine (SMZ), sulfadimethoxine (SDM), and sulfamethoxazole Soils Table 1. pKa of studied sulfonamides. pKa Antibiotics

Acidic: 25 C

Alkalic: 25 C

SDZ SMR SMZ SDM SMX

6.81 § 0.10 7.35 § 0.10 7.89 § 0.10 6.21 § 0.50 5.81 § 0.50

1.64 § 0.10 1.64 § 0.10 1.69 § 0.10 3.00 § 0.10 1.39 § 0.10

Five soils (Soils J, D, W, S, and N) were selected to conduct these experiments; the OC content, fine earth particle size distribution, pH, and cation exchange capacity (CEC) of which were variable (Table 2). The freshly dried topsoils (0–20 cm) were collected through vacuum freeze-drying, sieved (

Sorption and transport of five sulfonamide antibiotics in agricultural soil and soil-manure systems.

Animal manure application is a main spreading route of veterinary antibiotics in soil and groundwater. The sorption and leaching behavior of five comm...
639KB Sizes 1 Downloads 12 Views