低温热解对有机肥中抗生素及抗性基因的消减研究
Reduction of Antibiotics and Resistance Genes in Organic Fertilizers by Low-temperature Pyrolysis
-
摘要: 为研究低温热解作用下有机肥中抗生素和抗性基因(antibiotic resistance genes, ARGs)的消减规律,利用高分辨液相色谱-串联质谱技术和荧光定量PCR(real-time fluorescent quantitative polymerase chain reaction, Real-time PCR)技术分别测定热解前后有机肥中抗生素和ARGs含量。结果发现,80~250 ℃低温热解后抗生素总量降低,去除率在11.63%~47.32%之间。热解温度与抗生素熔点对有机肥中抗生素去除影响显著:热解温度越高,对抗生素的去除效果越好;抗生素熔点越低,去除越彻底。80~250 ℃低温热解对ARGs丰度和水平转移有强烈抑制作用。温度升高,对ARGs的去除效果不断增强,去除率最高可达99%;可移动元件平均去除率高达90%,在250 ℃下,几乎被完全去除;大肠杆菌指示基因uida在各个温度下的平均去除率均达到99%以上。添加硅藻土和沸石与单一有机肥相比,在80~150 ℃对抗生素和ARGs的去除分别发挥促进和抑制作用;在250 ℃显著抑制了抗生素的去除。本研究揭示了不同热解温度对抗生素和ARGs的影响,为有机肥中抗生素和ARGs的低温热解阻控技术提供理论依据。Abstract: Low-temperature pyrolysis experiments were conducted to study the dynamics of antibiotics and antibiotic resistance genes (ARGs) in organic fertilizers. The concentrations of antibiotics and ARGs before and after pyrolysis were determined by ultra-performance liquid chromatography-mass spectrometry and quantitative PCR technology, respectively. The results showed that low-temperature pyrolysis under 80~250 °C decreased the levels of antibiotics from 11.63% to 47.32%. Pyrolysis temperature and antibiotic melting point played important roles in the removal of antibiotics in organic fertilizers: the higher the pyrolysis temperature, the better the removal effect of antibiotics; the lower the melting point of the antibiotic, the more thoroughly it is removed. Meanwhile, low-temperature pyrolysis under 80~250 °C had strong inhibiting effects on abundance of ARGs and horizontal gene transfer. The removal efficiency of ARGs continuously increased up to 99% along with increasing temperature. The average removal rate of mobile genetic elements was 90%, and almost all of them were removed at 250°C. The average removal rates of uida were all above 99% within the whole pyrolysis temperature range. In comparison with organic fertilizers, the addition of diatomite and zeolite promoted and inhibited the removal of antibiotics and ARGs, respectively, at 80~150°C, and significantly inhibited the removal of antibiotics at 250°C. The results from this study revealed the influence of pyrolysis temperature on the behavior and removal of antibiotics and ARGs, thus providing a theoretical basis for future application of low-temperature pyrolysis in reducing antibiotics and ARGs in organic fertilizers.
-
Key words:
- antibiotics /
- antibiotic resistance genes /
- organic fertilizers /
- low-temperature pyrolysis /
- reduction
-
-
郭坤. 有机肥中抗生素及其抗性基因的检测和恩诺沙星对生菜内生细菌的喹诺酮抗性基因的影响[D]. 南京: 南京师范大学, 2013: 1-2 Guo K. Detection of antibiotics and their resistance genes in organic fertilizer and the effect of enrofloxacin on quinolone resistance genes of endophytic bacteria in lettuce [D]. Nanjing: Nanjing Normal University, 2013: 1 -2 (in Chinese)
李轶, 胡童, 王琳琼, 等. 环丙沙星和铜复合污染下河流底质微生物群落与抗生素抗性基因的交互关系[J]. 河海大学学报(自然科学版), 2022, 50(6): 75-84 Li Y, Hu T, Wang L Q, et al. The interactions between microbial communities and antibiotic resistance genes to ciprofloxacin and copper co-contamination in river sediments [J]. Journal of Hohai University (Natural Sciences), 2022, 50(6): 75-84 (in Chinese) Li J J, Xin Z H, Zhang Y Z, et al. Long-term manure application increased the levels of antibiotics and antibiotic resistance genes in a greenhouse soil [J]. Applied Soil Ecology, 2017, 121: 193-200 Xie W Y, Shen Q, Zhao F. Antibiotics and antibiotic resistance from animal manures to soil: A review [J]. European Journal of Soil Science, 2018, 69 (1): 181-195 Wang Y, Chen G X, Liang J, et al. Comparison of oxytetracycline degradation behavior in pig manure with different antibiotic addition methods [J]. Environmental Science and Pollution Research International, 2015, 22(23): 18469-18476 Li B, Yang Y, Ma L P, et al. Metagenomic and network analysis reveal wide distribution and co-occurrence of environmental antibiotic resistance genes [J]. The ISME Journal, 2015, 9(11): 2490-2502 Wang Y Z, Zhang Y L, Li J X, et al. Biogas energy generated from livestock manure in China: Current situation and future trends [J]. Journal of Environmental Management, 2021, 297: 113324 Gaballah M S, Guo J B, Sun H, et al. A review targeting veterinary antibiotics removal from livestock manure management systems and future outlook [J]. Bioresource Technology, 2021, 333: 125069 Zhang M, He L Y, Liu Y S, et al. Variation of antibiotic resistome during commercial livestock manure composting [J]. Environment International, 2020, 136: 105458 Liu B T, Yu K F, Ahmed I, et al. Key factors driving the fate of antibiotic resistance genes and controlling strategies during aerobic composting of animal manure: A review [J]. The Science of the Total Environment, 2021, 791: 148372 Cheng X Q, Zhang C, Wang Z X, et al. Tailoring nanofiltration membrane performance for highly-efficient antibiotics removal by mussel-inspired modification [J]. Journal of Membrane Science, 2016, 499: 326-334 余震, 周顺桂. 超高温好氧发酵技术: 堆肥快速腐熟与污染控制机制[J]. 南京农业大学学报, 2020, 43(5): 781-789 Yu Z, Zhou S G. Hyperthermophilic composting of organic solid wastes: Accelerated humification and pollution control mechanisms [J]. Journal of Nanjing Agricultural University, 2020, 43(5): 781-789 (in Chinese)
孟俊. 猪粪堆制、热解过程中重金属形态变化及其产物的应用[D]. 杭州: 浙江大学, 2014: 11-12 Meng J. Change of heavy metal fractions during the composting and pyrolysis processes of swine manure and the applications of its composts and biochars [D]. Hangzhou: Zhejiang University, 2014: 11 -12 (in Chinese)
王艳. 城市生活垃圾中低温热解特性研究[D]. 天津: 天津大学, 2005: 15-16 Wang Y. Characteristic studies on middle and low-temperature pyrolysis of municipal household garbage [D]. Tianjin: Tianjin University, 2005: 15 -16 (in Chinese)
田仁强, 谢胜禹, 李春星, 等. 鸡粪与农林废弃物共热解对生物炭中残留重金属和抗生素的影响[J]. 农业环境科学学报, 2019, 38(11): 2619-2631 Tian R Q, Xie S Y, Li C X, et al. Effect of co-pyrolysis of chicken manure and agricultural or forestry wastes on residual heavy metals and antibiotics in biochar [J]. Journal of Agro-Environment Science, 2019, 38(11): 2619-2631 (in Chinese)
李哲. 热碱解-水解处理剩余污泥的效果及四环素类抗性基因的变化研究[D]. 广州: 华南理工大学, 2018: 62-63 Li Z. Study on the effect of disposing residual sludge and the change of tetracyclines resistance genes by thermal-alkaline combined with hydrolysis process [D]. Guangzhou: South China University of Technology, 2018: 62 -63 (in Chinese)
Tian R Q, Li C X, Xie S Y, et al. Preparation of biochar via pyrolysis at laboratory and pilot scales to remove antibiotics and immobilize heavy metals in livestock feces [J]. Journal of Soils and Sediments, 2019, 19(7): 2891-2902 李杰, 潘兰佳, 余广炜, 等. 污泥中抗生素热解特性及动力学分析[J]. 环境工程学报, 2017, 11(9): 5213-5219 Li J, Pan L J, Yu G W, et al. Pyrolysis characteristics and kinetics analysis of several antibiotics in sludge [J]. Chinese Journal of Environmental Engineering, 2017, 11(9): 5213-5219 (in Chinese)
陈原, 张庚庚, 施宇震, 等. 高硅沸石吸附水中有机微污染物的研究进展[J]. 广州化工, 2022, 50(7): 11-14 Chen Y, Zhang G G, Shi Y Z, et al. Research progress on adsorption of organic micro pollutants in water by high silica zeolite [J]. Guangzhou Chemical Industry, 2022, 50(7): 11-14 (in Chinese)
郭志伟, 赵宝龙, 郑志宏, 等. 碳化改性硅藻土对四环素的吸附[J]. 环境工程, 2022, 40(5): 44-52 Guo Z W, Zhao B L, Zheng Z H, et al. Preparation of modified diatomite via carbonization and its adsorption performance on tetracycline [J]. Environmental Engineering, 2022, 40(5): 44-52 (in Chinese)
Zhou G X, Qiu X W, Wu X Y, et al. Horizontal gene transfer is a key determinant of antibiotic resistance genes profiles during chicken manure composting with the addition of biochar and zeolite [J]. Journal of Hazardous Materials, 2021, 408: 124883 Wei Y, Gu J, Wang X J, et al. Elucidating the beneficial effects of diatomite for reducing abundances of antibiotic resistance genes during swine manure composting [J]. Science of the Total Environment, 2022, 821: 153199 董颖博, 张圆, 林海, 等. 焙烧温度对天然沸石物化性能的影响[J]. 中国有色金属学报, 2017, 27(7): 1520-1526 Dong Y B, Zhang Y, Lin H, et al. Effects of calcination temperature on physicochemical properties of natural zeolite [J]. The Chinese Journal of Nonferrous Metals, 2017, 27(7): 1520-1526 (in Chinese)
郭绍英. 焙烧改性硅藻土处理垃圾渗滤液[J]. 环境科学与管理, 2012, 37(11): 101-103 Guo S Y. Treatment of landfill leachate by roasting-modified diatomite [J]. Environmental Science and Management, 2012, 37(11): 101-103 (in Chinese)
Zhou L J, Ying G G, Liu S, et al. Simultaneous determination of human and veterinary antibiotics in various environmental matrices by rapid resolution liquid chromatography-electrospray ionization tandem mass spectrometry [J]. Journal of Chromatography A, 2012, 1244: 123-138 刘叶新, 周志洪, 区晖, 等. 珠江广州河段沉积物中典型抗生素的污染特征[J]. 华南师范大学学报(自然科学版), 2018, 50(4): 48-54 Liu Y X, Zhou Z H, Ou H, et al. Occurrence of typical antibiotics in sediments of Guangzhou section of the Pearl River [J]. Journal of South China Normal University (Natural Science Edition), 2018, 50(4): 48-54 (in Chinese) 葛丽炜, 夏颖, 刘书悦, 等. 热解温度和时间对马弗炉制备生物炭的影响[J]. 沈阳农业大学学报, 2018, 49(1): 95-100 Ge L W, Xia Y, Liu S Y, et al. Effect of pyrolysis temperature and time on biochar production in a muffle furnace [J]. Journal of Shenyang Agricultural University, 2018, 49(1): 95-100 (in Chinese)
He L Y, Liu Y S, Su H C, et al. Dissemination of antibiotic resistance genes in representative broiler feedlots environments: Identification of indicator ARGs and correlations with environmental variables [J]. Environmental Science & Technology, 2014, 48(22): 13120-13129 何轮凯, 张敏, 刘有胜, 等. 长期施用粪肥的土壤中抗生素耐药基因的消减规律[J]. 华南师范大学学报(自然科学版), 2018, 50(1): 1-10, 130 He L K, Zhang M, Liu Y S, et al. Dynamics of antibiotic resistance genes in soil chronically fertilized by swine manure [J]. Journal of South China Normal University (Natural Science Edition), 2018, 50(1): 1-10, 130 (in Chinese) Madsen L, Aarestrup F M, Elmerdahl Olsen J. Characterisation of streptomycin resistance determinants in Danish isolates of Salmonella typhimurium [J]. Veterinary Microbiology, 2000, 75(1): 73-82 Ram J L, Ritchie R P, Fang J W, et al. Sequence-based source tracking of Escherichia coli based on genetic diversity of beta-glucuronidase [J]. Journal of Environmental Quality, 2004, 33(3): 1024-1032 Sidrach-Cardona R, Hijosa-Valsero M, Marti E, et al. Prevalence of antibiotic-resistant fecal bacteria in a river impacted by both an antibiotic production plant and urban treated discharges [J]. Science of the Total Environment, 2014, 488-489: 220-227 Li C X, Xie S Y, Wang Y, et al. Simultaneous heavy metal immobilization and antibiotics removal during synergetic treatment of sewage sludge and pig manure [J]. Environmental Science and Pollution Research, 2020, 27(24): 30323-30332 韩森, 朱小梅. 喹诺酮类药物诺氟沙星的热稳定性研究[J]. 中国新药杂志, 2007, 16(14): 1104-1107 Han S, Zhu X M. Thermal analysis of norfloxacin [J]. Chinese Journal of New Drugs, 2007, 16(14): 1104-1107 (in Chinese)
胡慧敏. 生物质材料固定化微生物及其降解土壤中磺胺类抗生素的研究[D]. 广州: 华南农业大学, 2017: 51-53 Hu H M. The research of biomass material immobilized microorganism and its degradation of sulfonamides in soil [D]. Guangzhou: South China Agricultural University, 2017: 51 -53 (in Chinese)
Böer T M, Procópio J V, Nascimento T G, et al. Correlation of thermal analysis and pyrolysis coupled to GC-MS in the characterization of tacrolimus [J]. Journal of Pharmaceutical and Biomedical Analysis, 2013, 73: 18-23 李玮. 大环内酯类抗生素热稳定性及分解动力学研究[J]. 药物分析杂志, 2010, 30(8): 1544-1547 Li W. Studies on the thermal kinetics of thermal decomposition and stability of macrolide drugs [J]. Chinese Journal of Pharmaceutical Analysis, 2010, 30(8): 1544-1547 (in Chinese)
Yu Y S, Chen L J, Fang Y, et al. High temperatures can effectively degrade residual tetracyclines in chicken manure through composting [J]. Journal of Hazardous Materials, 2019, 380: 120862 Kimbell L K, Kappell A D, McNamara P J. Effect of pyrolysis on the removal of antibiotic resistance genes and class Ⅰ integrons from municipal wastewater biosolids [J]. Environmental Science: Water Research & Technology, 2018, 4(11): 1807-1818 Ma Y J, Wilson C A, Novak J T, et al. Effect of various sludge digestion conditions on sulfonamide, macrolide, and tetracycline resistance genes and class Ⅰ integrons [J]. Environmental Science & Technology, 2011, 45(18): 7855-7861 Liao H P, Lu X M, Rensing C, et al. Hyperthermophilic composting accelerates the removal of antibiotic resistance genes and mobile genetic elements in sewage sludge [J]. Environmental Science & Technology, 2018, 52(1): 266-276 Xu F, Liu Y L, Du W C, et al. Response of soil bacterial communities, antibiotic residuals, and crop yields to organic fertilizer substitution in North China under wheat-maize rotation [J]. Science of the Total Environment, 2021, 785: 147248 武晓春. 卧式电阻炉的设计与应用[J]. 现代制造技术与装备, 2020(4): 94-95 Wu X C. Design and application of horizontal resistance furnace [J]. Modern Manufacturing Technology and Equipment, 2020 (4): 94-95 (in Chinese)
孙晓兵, 穆玉芹, 吕金根, 等. 箱式电阻炉热处理生产中的降本增效案例及创新思维[J]. 金属加工(热加工), 2019(3): 1-3, 11 Sun X B, Mu Y Q, Lv J G, et al. Reduction and efficiency cases and innovative thinking in heat treatment production of box-type resistance furnace [J]. MW Metal Forming, 2019(3): 1-3, 11 (in Chinese) 江尧忠. 工业电炉[M]. 北京: 清华大学出版社, 1993: 520-530 高采文. 基于因子分析的改进雷达图及其在综合评价中的应用[J]. 山西师范大学学报(自然科学版), 2013, 27(4): 19-22 Gao C W. Improved radar chart based on factor analysis and its application in comprehensive evaluating [J]. Journal of Shanxi Normal University (Natural Science Edition), 2013, 27(4): 19-22 (in Chinese) -
![WeChat](http://eekw.rcees.ac.cn//eekw-data/stdlxb/2023/1/PIC/wechat_cnf9a2c8f4-ba32-48a5-a0f2-41358ed694cf.jpg)
计量
- 文章访问数: 2294
- HTML全文浏览数: 2294
- PDF下载数: 70
- 施引文献: 0