Effects of pig manure-derived dissolved organic matter on the transport of antibiotics in purple soils
LUO Fang-lin1,2, LIU Chen2, TANG Xiang-yu2, YANG Hong-wei1
1. Faculty of Geosciences and Environmental Engineering, Southwest Jiaotong University, Chengdu 610031, China; 2. Institute of Mountain Hazards and Environment, Chinese Academy of Sciences, Chengdu 610041, China
Abstract：The effects of pig manure-derived dissolved organic matter (DOM) on the sorption-desorption and leaching characteristics of florfenicol (FFC) and norfloxacin (NOR) in typical calcareous purple soils (sloping cropland and orchard) in the hilly areas of central Sichuan were studied, using batch equilibrium and packed soil column experiments. The results indicated that, FFC had weak adsorption capacity in purple soils (Kf = 0.34 and 0.85L/kg for the sloping cropland and the orchard soil, respectively), and negative desorption hysteresis was observed. When spiked simultaneously with pig manure DOM (50~200mg C/L), the adsorption of FFC increased significantly in both soils (P<0.05), while on the contrary, when pig manure DOM (200mg C/L) was introduced to the soils prior to FFC, the adsorption of FFC decreased. Despite the existence of competition for the adsorption sites, the results suggested that pig manure DOM promoted FFC's adsorption via a co-adsorption mechanism. NOR had a strong sorption capacity (Kf = 405.4 and 516.7L/kg for the sloping cropland soil and the orchard soil, respectively). In the presence of pig manure DOM, its adsorption increased a little in the cropland soil, while did not change in the orchard soil. According to the soil column breakthrough curves obtained under a simulated rainfall intensity of 20mm/h, FFC was highly mobile, and it leached out almost simultaneously with the water flow tracer Br- from the column of the cropland soil, which had an 11.03%~23.39% higher leaching capacity than that of the orchard soil. On the other hand, NOR did not penetrate, and 96.2%~98.6% of its residues were retained in 0~3cm topsoil. Being consistent with the results from the batch experiment, pig manure DOM delayed the breakthrough of FFC by 0.07~0.13 PV and increased its residues by 15.21%~25.96%, while such effect was not obvious for NOR. Based on FTIR and EEM fluorescence analysis, pig manure DOM was mainly composed of tyrosine and tryptophan, which were easy to form complex with FFC in the aqueous phase. Therefore, for the highly mobile antibiotics, manure-derived DOM may increase the retention of antibiotics in the soil through a co-adsorption mechanism; as for the hydrophobic antibiotics with strong adsorption, the effect is not significant.
罗芳林, 刘琛, 唐翔宇, 杨红薇. 猪粪溶解性有机物对紫色土中抗生素迁移的影响[J]. 中国环境科学, 2020, 40(9): 3952-3961.
LUO Fang-lin, LIU Chen, TANG Xiang-yu, YANG Hong-wei. Effects of pig manure-derived dissolved organic matter on the transport of antibiotics in purple soils. CHINA ENVIRONMENTAL SCIENCECE, 2020, 40(9): 3952-3961.
Zhang Y L, Lin S S, Dai C M, et al. Sorption-desorption and transport of trimethoprim and sulfonamide antibiotics in agricultural soil:Effect of soil type, dissolved organic matter, and pH[J]. Environmental Science and Pollution Research, 2014,21(9):5827-5835.
[2]
武淑霞,刘宏斌,黄宏坤,等.我国畜禽养殖粪污产生量及其资源化分析[J]. 中国工程科学, 2018,20(5):103-111. Wu S X, Liu H B, Huang H K,et al. Analysis on the amount and utilization of manure in livestock and poultry breeding in China[J]. Engineering Science, 2018,20(5):103-111.
[3]
Wei R, Ge F, Zhang L, et al. Occurrence of 13 veterinary drugs in animal manure-amended soils in Eastern China[J]. Chemosphere, 2016,144:2377-2383.
[4]
Zhao L, Dong Y H, Wang H. Residues of veterinary antibiotics in manures from feedlot livestock in eight provinces of China[J]. Science of the Total Environment, 2010,408(5):1069-1075.
[5]
Golet E M, Xifra I, Siegrist H, Alder A C, et al. Environmental exposure assessment of fluoroquinolone antibacterial agents from sewage to soil[J]. Environmental Science and Techno-logy, 2003, 37(15):3243-3249.
[6]
吴东明,任常琦,李勤奋,等.溶解性有机质对铁铝土吸附2,4-D的影响[J]. 中国环境科学, 2018,38(3):1090-1098. Wu D M, Ren C Q, Li Q F, et al. Influence of dissolved organic matter on sorption of 2,4-dichlorophenoxyacetic acid in ferralsol[J]. China Environmental Science, 2018,38(3):1090-1098.
[7]
Teixidó M, Medeiros J, Beltrán J L, et al. Sorption of enrofloxacin and ciprofloxacin in agricultural soils:Effect of organic matter[J]. Adsorption Science & Technology, 2014,32(2/3):153-163.
[8]
范菲菲,朱健,韦时宏.外源溶解性有机质对兽药土霉素在黄壤中吸附-解吸行为的影响[J]. 湖北农业科学, 2015,54(1):53-58. Fan F F, Zhu J, Wei S H, et al. Effects of dissolved organic matter on the adsorption-desorption of oxytetracycline on yellow soil[J]. Hubei Agricultural Sciences, 2015,54(1):53-58.
[9]
黎明,王彬,朱静平,等.川西平原还田秸秆DOM对矿物细颗粒吸附SMX的影响[J]. 中国环境科学, 2016,36(11):3441-3448. Li M, Wang B, Zhu J P, et al. Effect of DOM derived from straw in West Sichuan plain on fine mineral particle adsorbing SMX[J]. China Environmental Science, 2016,36(11):3441-3448.
[10]
徐文秀,韦杰,李进林,等.三峡库区紫色土坡耕地表土的可蚀性研究[J]. 水土保持通报, 2019,39(3):7-11. Xu W X, Wei J, L J L, et al. Topsoil erodibility on purple soil sloping farmlands in three gorges reservoir area[J]. Bulletin of Soil and Water Conservation, 2019,39(3):7-11.
[11]
Su Z A, Zhang J H, Nie X J. Effect of soil erosion on soil properties and crop yields on slopes in the Sichuan Basin, China[J]. Pedosphere, 2010,20(6):736-746.
[12]
娄义宝,史东梅,金慧,等.西南紫色土坡耕地农作物-耕层质量适宜性的耦合度诊断[J]. 中国农业科学, 2019,52(4):661-675. Lou Y B, Shi D M, Jin H, et al. Coupling degree diagnosis on suitability evaluation of cultivated-layer quality for slope farmland in purple hilly region of South-Western China[J]. Scientia Agricultura Sinica, 2019,52(4):661-675.
[13]
王畅,李余杰,张智,等.氟喹诺酮类抗生素在农业紫色土中的吸附研究[J]. 土壤, 2018,50(5):958-964. Wang C, Li Y J, Zhang Z, et al. Sorption of fluoroquinolone antibiotics in agricultural purple soils[J]. Soils, 2018,50(5):958-964.
[14]
阴文敏,关卓,刘琛,等.生物炭施用及老化对紫色土中抗生素吸附特征的影响[J]. 环境科学, 2019,40(6):2920-2929. Yin W M, Guan Z, Liu C, et al. Effects of biochar application and ageing on the adsorption of antibiotics in purple soil[J]. Environmental Science, 2019,40(6):2920-2929.
[15]
周志强,刘琛,杨红薇,等.生物质炭对磺胺类抗生素在坡耕地紫色土中吸附-解吸及淋溶过程的影响[J]. 土壤, 2018,50(2):353-360. Zhou Z Q, Liu C, Yang H W, et al. Effects of biochar application on sorption-desorption process and leaching behaviour of sulfonamide antibiotics[J]. Soils, 2018,50(2):353-360.
[16]
苏思慧,何江涛,杨蕾.北京东南郊土壤剖面氟喹诺酮类抗生素分布特征[J]. 环境科学, 2014,35(11):4257-4266. Su S H, He J T, Yang L, et al. Contamination characteristics of fluoroquinolones in different kinds of soil profiles in southeast suburb of Beijing[J]. Environmental Science, 2014,35(11):4257-4266.
[17]
Liu W F, Zhang J, Zhang C L, et al. Sorption of norfloxacin by lotus stalk-based activated carbon and iron-doped activated alumina:Mechanisms, isotherms and kinetics[J]. Chemical Engineering Journal, 2011,171(2):431-438.
[18]
Yang W B, Lu Y P, Zheng F F, et al. Adsorption behavior and mechanisms of norfloxacin onto porous resins and carbon nanotube[J]. Chemical Engineering Journal, 2012,179:112-118.
[19]
吴敏,宁平,刘书言.土壤有机质对诺氟沙星的吸附特征[J]. 环境化学, 2013,32(1):112-117. Wu M, Ning P, Liu S Y. Adsorption characteristics of norfloxacin in soil organic matter fractions[J]. Environmental Chemistry, 2013,32(1):112-117.
[20]
Doretto K M, Peruchi L M, Rath S. Sorption and desorption of sulfadimethoxine, sulfaquinoxaline and sulfamethazine antimicrobials in Brazilian soils[J]. Science of the Total Environment, 2014,476-477:406-414.
[21]
Watson K W, Luxmoore R J. Estimating macroporosity in a forest watershed by use of tension infiltrometer[J]. Soil Science Society of America Journal, 1986,50(3):578-582.
[22]
雷文娟,唐翔宇,关卓,等.不同类型耕地紫色土中3,5,6-三氯-2-吡啶醇迁移试验与模拟[J]. 农业工程学报, 2015,31(5):132-138. Lei W J, Tang X Y, Guan Z, et al. Experiment and model simulation of 3,5,6-TCP transport in different farmland purple soils[J]. Transactions of the Chinese Society of Agricultural Engineering (Transactions of the CSAE), 2015,31(5):132-138.
[23]
Elabd H, Jury W A, Cliath M M, et al. Spatial variability of pesticide absorption parameters[J]. Environmental Science and Technology, 1986,20(3):256-260.
[24]
凌婉婷,徐建民,高彦征,等.溶解性有机质对土壤中有机污染物环境行为的影响[J]. 应用生态学报, 2004,15(2):326-330. Ling W T, Xu J M, Gao Y Z, et al. Influence of dissolved organic matter(DOM) on environmental behaviors of organic pollutants in soils[J]. Chinese Journal of Applied Ecology, 2004,15(2):326-330.
[25]
Raber B, Kögel-Knabner I. Influence of origin and properties of dissolved organic matter on the partition of polycyclic aromatic hydrocarbons (PAHs)[J]. European Journal of Soil Science, 1997, 48(3):443-455.
[26]
Bai L, Zhao Z, Wang C, et al. Multi-spectroscopic investigation on the complexation of tetracycline with dissolved organic matter derived from algae and macrophyte[J]. Chemosphere, 2017,187:421-429.
[27]
张会群,贾妍艳,方荷婷,等.硫酸盐还原菌活性污泥胞外聚合物对环丙沙星的吸附机制[J]. 环境科学, 2018,39(10):4653-4660. Zhang H Q, Jia Y Y, Fang H T, et al. Adsorption mechanisms of ciprofloxacin by extracellular polymeric substances of sulfate-reducing bacteria sludge[J]. Environmental Science, 2018,39(10):4653-4660.
[28]
Seliger H, Göldner E, Kittel I, et al. Two-carrier liquid-phase synthesis of main-chain liquid crystalline oligomers and characterization of the products[J]. Fresenius' Journal of Analytical Chemistry, 1995,351(2/3):62-73.
[29]
陈薇薇,陈涛,杨平,等.共存Cu2+ 影响下土霉素在黑土上的吸附行为[J]. 江苏农业科学, 2017,45(18):240-244. Chen W W, Chen T, Yang P, et al. Effect of coexistent Cu2+ on adsorption of oxytetracycline (OTC) onto black soil[J]. Jiangsu Agricultural Sciences, 2017,45(18):240-244.
[30]
提清清,高增文,季慧慧,等.抗生素在土壤中的吸附行为研究进展[J]. 土壤, 2017,49(3):437-445. Ti Q Q, Gao Z W, Ji H H, et al. Adsorption of antibiotics in soils:A review[J]. Soils, 2017,49(3):437-445.
