DGT分析水中四环素类抗生素自由溶解态浓度

李旭辉; 蒙耿剑; 朱伟刚; 郭瑞超

PDF(449 KB)

中国环境科学 ›› 2020, Vol. 40 ›› Issue (9) : 4058-4064.

环境生态

DGT分析水中四环素类抗生素自由溶解态浓度

李旭辉^1,2,3, 蒙耿剑^1,2,3, 朱伟刚^1,2,3, 郭瑞超^1,2,3

作者信息 +

Determination of the freely dissolved concentration of tetracyclines in water with diffusive gradients in thin-films technology(DGT)

LI Xu-hui^1,2,3, MENG Geng-jian^1,2,3, ZHU Wei-gang^1,2,3, GUO Rui-chao^1,2,3

Author information +

文章历史 +

摘要

为分析四环素类抗生素的生物有效性，本研究自制了o-DGT装置，测定了结合相的回收率以及不同温度下污染物在扩散相的扩散系数，最终将该装置应用于天然水体中四环素类抗生素自由溶解态浓度的分析.结果表明，所制备的结合相对四环素类抗生素具有较强且稳定的结合能力，其单独存在时对溶液中四环素、土霉素、金霉素的回收率分别为（104.37±4.93）%，（80.29±4.41）%和（81.52±3.93）%；25℃时，3种四环素类抗生素在所制备的扩散相中扩散系数分别是（1.08±0.05）×10^-6，（1.07±0.18）×10^-6，（1.03±0.07）×10^-6cm²/s.抗生素浓度在0.2~10mg/L时，四环素、土霉素、金霉素的C_DGT占总量分别11.69%~30.21%、10.02%~29.25%和7.44%~34.10%.所制备的o-DGT装置性能稳定，可以为测定四环素类抗生素污染物生物有效性和自由溶解态浓度提供有效的参数.

Abstract

In order to determine the bioavailability of tetracyclines (TCs), a diffusive gradients in thin-films for organic technology (o-DGT) device was developed. The diffusivity of the diffused phase and the recovery rate of the combined phase were measured at different temperatures. The results showed that the combined phase had strong and stable capacity on the exaction of TCs when solely presented with recovery rates of (104.37±4.93)%, (80.29±4.41)%, and (81.52±3.93)% for tetracycline (TC), oxytetracycline (OTC) and chlorotetracycline (CTC), respectively. The diffusion coefficients of TC, OTC, CTC were (1.08±0.05)×10^-6, (1.07±0.18)×10^-6, (1.03±0.07)×10^-6 cm²/s, respectively. With the total concentrations of TCs among 0.2~10.0mg/L, the ratios of C_DGT to total concentration in natural water were 11.69%~30.21%, 10.02%~29.25% and 7.44%~34.10% for TC, OTC, CTC, respectively. Thus, the o-DGT device showed a stable performance and could provide effective measurement parameters for the bioavailability determination of tetracyclines.

导出引用

李旭辉, 蒙耿剑, 朱伟刚, 郭瑞超. DGT分析水中四环素类抗生素自由溶解态浓度[J]. 中国环境科学. 2020, 40(9): 4058-4064

LI Xu-hui, MENG Geng-jian, ZHU Wei-gang, GUO Rui-chao. Determination of the freely dissolved concentration of tetracyclines in water with diffusive gradients in thin-films technology(DGT)[J]. China Environmental Science. 2020, 40(9): 4058-4064

中图分类号： X171

参考文献

[1] D'Angelo E, Martin A. Tetracycline desorption kinetics in municipal biosolids and poultry litter amendments determined by diffusive gradients in thin films (DGT)[J]. Chemosphere, 2018,209:232-239.
[2] Yue Y, Shen C, Ge Y. Biochar accelerates the removal of tetracyclines and their intermediates by altering soil properties[J]. Journal of Hazardous Materials, 2019,380:120821.
[3] Mitchell S M, Ullman J L, Bary A, et al. Antibiotic degradation during thermophilic composting[J]. Water Air Soil Pollution, 2015,226(13):2-12.
[4] Popowska M, Rzeczycka M, Miernik A., et al. Influence of soil use on prevalence of tetracycline, streptomycin, and erythromycin resistance and associated resistance genes[J]. Antimicrob Agents & Chemotherapy, 2012,56(3):1434-1443.
[5] Liang Y, Pei M, Wang D, et al. Improvement of soil ecosystem multifunctionality by dissipating manure-induced antibiotics and resistance genes[J]. Environmental Science & Technology, 2017, (51)9:4988-4998.
[6] Allen H K, Donato J, Wang H H, et al. Call of the wild:Antibiotic resistance genes in natural environments[J]. Nature Reviews Microbiology, 2010,8(4):251-259.
[7] Vikesland P J, Pruden A, Alvarez P J J, et al. Toward a comprehensive strategy to mitigate dissemination of environmental sources of antibiotic resistance[J]. Environmental Science & Technology, 2017, 51(22):13061-13069.
[8] Martínez J L, Coque T M, Baquero F. What is a resistance gene? Ranking risk in resistomes[J]. Nature Reviews Microbiology, 2014,13(2):116-123.
[9] Feng L, Cheng Y, Zhang Y, et al. Distribution and human health risk assessment of antibiotic residues in large-scale drinking water sources in chongqing area of the Yangtze river[J]. Environmental Research 2020,185:109386.
[10] Gray A D, Todd D, Hershey A E. The seasonal distribution and concentration of antibiotics in rural streams and drinking wells in the piedmont of north Carolina[J]. Science of the Total Environment, 2020,710:136286.
[11] Li F, Chen L, Chen W, et al. Antibiotics in coastal water and sediments of the east china sea:Distribution, ecological risk assessment and indicators screening[J]. Marine Pollution Bulletin, 2020,151:110810.
[12] Van Boeckel T P, Pires J, Silvester R, et al. Global trends in antimicrobial resistance in animals in low-and middle-income countries[J]. Science, 2019,365(6459).
[13] Zhang Q Q, Ying G G, Pan C G, et al. Comprehensive evaluation of antibiotics emission and fate in the River Basins of China:Source analysis, multimedia modeling, and linkage to bacterial resistance[J]. Environmental Science & Technology, 2015,49(11):6772-6782.
[14] Granados-Chinchilla F, Rodríguez C. Bioavailability of in-feed tetracyclines is influenced to a greater extent by crude protein rather than calcium[J]. Animal Feed Science and Technology, 2014,198:323-332.
[15] Tasho R P, Cho J Y, Veterinary antibiotics in animal waste, its distribution in soil and uptake by plants:a review[J]. Science of the Total Environment, 2016,563-564:366-376.
[16] He P J, Yu Z F, Shao L M, et al. Fate of antibiotics and antibiotic resistance genes in a full-scale restaurant food waste treatment plant:Implications of the roles beyond heavy metals and mobile genetic elements[J]. Journal of Environmental Sciences, 2019,85(SI):17-34.
[17] Escher B I, Hermens J L M. Internal exposure:Linking bioavailability to effects[J]. Environmental Science & Technology, 2004,38(23):455A-462A.
[18] Davison W, Zhang H. Progress in understanding the use of diffusive gradients in thin films (DGT) back to basics[J]. Environmental Chemistry, 2012,9(1):1-13.
[19] Davison W, Zhang H. In situ speciation measurements of trace components in natural waters using thin-film gels[J]. Nature, 1994, 367(6463):546-548.
[20] Harper M P, Davison W, Zhang H, et al. Kinetics of metal exchange between solids and solutions in sediments and soils interpreted from DGT measured fluxes[J]. Geochemical et Cosmochimica Acta, 1998,62(16):2757-2770.
[21] Zhang C, Ding S, Xu D, et al. Bioavailability assessment of phosphorus and metals in soils and sediments:A review of diffusive gradients in thin films (DGT)[J]. Environmental Monitoring and Assessment, 2014,186(11):7367-7378.
[22] 罗军,王晓蓉,张昊,等.梯度扩散薄膜技术(DGT)的理论及其在环境中的应用:工作原理、特性与在土壤中的应用[J]. 农业环境科学学报, 2011,30(2):205-213. Luo J, Wang X R, Zhang H, et al. Theory and application of diffusive gradients in Thin Films in soil.[J]. Journal of Agro-Environment Science, 2011,30(2):205-213.
[23] 宋宁宁,王芳丽,赵玉杰,等.基于梯度薄膜扩散技术评估黑麦草吸收Cd的研究[J]. 中国环境科学, 2012,32(10):1826-1831. Song N N, Wang F L, Zhao Y J, et al. Assessment of cadmium bioavailability to ryegrass in soils by diffusive gradients in thin films[J]. China Environmental Science, 2012,32(10):1826-1831.
[24] 孙琴,徐律,丁士明,等.薄膜扩散梯度技术测量砷的影响因素及其应用[J]. 中国环境科学, 2016,36(5):1482-1490. Sun Q, Xu L, Ding S M, et al. Environmental influences on the measurement of dissolved arsenic using Zr-oxide DGT[J]. China Environmental Science, 2016,36(5):1482-1490.
[25] Chen C E, Zhang H, Ying G G, et al. Evidence and recommendations to support the use of a novel passive water sampler to quantify antibiotics in wastewaters[J]. Environmental Science & Technology, 2013,47(23):13587-13593.
[26] Chen C E, Zhang H, Ying G G, et al. Passive sampling:A cost-effective method for understanding antibiotic fate, behaviour and impact[J]. Environment International, 2015,85:284-291.
[27] Challis J K, Hanson M L, Wong C S. Development and calibration of an organic-diffusive gradients in thin films aquatic passive sampler for a diverse suite of polar organic contaminants[J]. Analytical Chemistry, 2016,88(21):10583-10591.
[28] Ren S Y, Tao J, Tan F, et al. Diffusive gradients in thin films based on mof-derived porous carbon binding gel for in-situ measurement of antibiotics in waters[J]. Science of the Total Environment, 2018, 645:482-490.
[29] You N, Yao H, Wang Y, et al. Development and evaluation of diffusive gradients in thin films based on nano-sized zinc oxide particles for the in situ sampling of tetracyclines in pig breeding wastewater[J]. Science of the Total Environment, 2019,651:1653-1660.
[30] Heringa M B, Hermens J L M. Measurement of free concentrations using negligible depletion-solid phase microextraction (nd-SPME)[J]. Trends in Analytical Chemistry, 2003,22(9):575-587.