金霉素浓度对鸡粪中温厌氧消化特性及抗生素降解的影响

强虹; 杨祎楠; 李娜; 宋亚楠; 李玉友

doi:10.11975/j.issn.1002-6819.2019.10.023

金霉素浓度对鸡粪中温厌氧消化特性及抗生素降解的影响

1.
西北农林科技大学资源环境学院，杨凌 712100
2.
日本东北大学工学部，仙台980-8579

基金项目: 陕西省重点研发计划项目资助（2018NY-004）；国家自然科学基金资助项目（51308460）

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出版历程
- 收稿日期: 2018-12-16
- 修回日期: 2019-04-14
- 发布日期: 2019-05-14

Effect of chlortetracycline concentration on mesophilic anaerobic digestion characteristics and antibiotic degradation of chicken manure

1.
College of Resource and Environment, Northwest A&F University, Yangling 712100, China
2.
School of Engineering, Tohoku University, Sendai 980-8579, Japan

摘要

摘要: 针对抗生素污染对鸡粪厌氧消化影响不明的问题，该文利用批次试验探究了不同质量浓度金霉素（chlortetracycline，CTC）（4～200 mg/L）对鸡粪中温厌氧消化过程、产气效率及抗生素降解的影响。结果表明，低浓度的CTC（质量浓度≤20 mg/L）促进了鸡粪中温厌氧消化作用，其对累积水解、酸化、乙酸化及甲烷化的最大促进率较对照（质量浓度0 mg/L）分别提高了12.69%，11.55%，11.31%和9.82%，厌氧消化有效降解了鸡粪中的CTC，降解率为59.87%～71.95%，这是因为厌氧污泥胞外聚合物（extracellular polymeric substances，EPS）由结合态（松散结合态（loosely bound EPS，LB-EPS）和紧密结合态（tightly bound EPS，TB-EPS））转化为黏液态（slime EPS，S-EPS）促进了水解作用，另外，CTC降解提供的碳源进一步促进了甲烷的生成。高浓度CTC（质量浓度≥60 mg/L）抑制了鸡粪中温厌氧消化作用，且抑制率随CTC质量浓度的增大而升高，对累积水解、酸化、乙酸化及甲烷化的最大抑制率分别为16.48%，18.54%，18.96%和19.94%，CTC的降解率为43.4%～51.44%；在此条件下污泥EPS较对照提高了13.81%～39.23%，其中EPS蛋白浓度由943.01 mg/L增加为1 083.69～1 338.20 mg/L。中温条件下CTC对鸡粪厌氧消化抑制阈值为22.16 mg/L。消化结束后，沼液和沼渣中的CTC分别占总量的0.46%～3.13%和96.87%～99.54%，表明CTC绝大部分残留在沼渣中，存在较大环境风险，所以应对沼渣进一步无害化处理后才可还田使用。
- 厌氧消化 /
- 抗生素 /
- 粪 /
- 甲烷产量 /
- 金霉素 /
- 胞外聚合物
Abstract: Abstract: Anaerobic digestion is a promising robust technology, which can not only reduce pollution of chicken manure but also produce energy, especially mesophilic anaerobic digestion of chicken manure has been widely used due to energy saving and long-term stability. In recent years, excess amount of antibiotics has been used in raising broilers to promote fast growth and prevent from diseases. The antibiotics residues problem in China rising day by day as compared to other countries, of which tetracycline antibiotic residues has been considered dangerous for living organisms. In China, it is reported that chlortetracycline residues especially in chicken manure was 563.8 mg/kg. Although, the toxicity threshold of antibiotics in soil regulated by Veterinary International Conference on Harmonization is 100 μg/kg, it has been found that, the chlortetracycline residues more than 50% of the soil sample in China has been found higher than the threshold. Anaerobic digestion technology plays an important role in degrading antibiotics resides, this process not only wasaffected by the antibiotics concentration and category, but also more importantly by substrate category. Chicken manure has greatly potential to produce higher biogas production per organic matter than swine and cattle manure, but the effect of chlortetracycline contamination on biogas production of mesophilic anaerobic digestion of that is still unclear, removal of chlortetracycline during anaerobic digestion of chicken manure also unknown. The effect of chlortetracycline on hydrolysis, acidogenesis, acetogenesis and methanogenesis during anaerobic digestion of chicken manure has not been deeply studied yet. Therefore, this study aimed to explore the effects of antibiotics on mesophilic anaerobic digestion of chicken manure. Influence of a wide range of chlortetracycline concentrations (4-200 mg/L CTC) on anaerobic digestion of chicken manure were investigated by batch experiments. The obtained results indicated that mesophilic methane production was increased when CTC concentration was less than 20 mg/L. More specifically, the ultimate increase rates of hydrolysis, acidogenesis, acetogenesis and methanogenesis for methane production were 12.69%, 11.55%, 11.31% and 9.82%, respectively. Indeed, the removal efficiency of CTC was increased from 59.87% to 71.95%. Further analysis showed that methane production was increased as a result of the transformation of extracellular polymer substances (EPS) from bound EPS (LB-EPS and TB-EPS) to slime EPS (S-EPS), which promoted the hydrolysis, In addition, the degradation of CTC produced the carbon sources for microorganisms. However, mesophilic methane production was inhibited when CTC concentration was higher than 60 mg/L. Moreover, the inhibition rate was increased with raising CTC concentration, among them the inhibitory effect of 200 mg/L CTC concentration was the strongest than others, the largest inhibition rate of 200 mg/L CTC concentration for hydrolysis, acidogenesis, acetogenesis and methanogenesis was 16.48%, 18.54%, 18.96% and 19.94%, respectively, and the removal efficiency of CTC reduced up to 43.4%-51.44%. EPS increased by 13.81%-39.23% compared with control, of which the concentration of EPS protein increased from 943.01 mg/L to 1 083.69-1 338.20 mg/L, it is assumed that bacterial resistance for CTC was increased by stimulating EPS secretion. Analysis of the distribution of residual CTC within the digester indicted that 0.46%-3.13% of CTC was existed in liquid digester, while 96.87%-99.54% of CTC was found in solid digester, which posed a significant threat to the environment. Further safe treatment was needed before solid digester used as organic fertilizer into field.
- anaerobic digestion /
- antibiotic /
- manure /
- methane production /
- chlortetracycline /
- extracellular polymeric substances

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参考文献(48)

[1]	刘茹飞，陈刚，王明超，等．我国典型禽畜粪便资源化技术研究[J]．再生资源与循环经济，2017，10(3)：37－40.Liu Rufei, Chen Gang, Wang Mingchao, et al. Research on resource utilization technology of livestock and poultry manure in China[J]. Recyclable Resources and Circular Economy, 2017, 10(3): 37－40. (in Chinese with English abstract)
[2]	潘君廷，马俊怡，郜天磊，等．膨润土改善鸡粪厌氧消化产酸产甲烷特性[J]．农业工程学报，2016，32(8)：246－252.Pan Junting, Ma Junyi, Gao Tianlei, et al. Improving production characteristics of methane and organic acid during anaerobic batch digestion of poultry manure by adding bentonite[J]. Transactions of the Chinese Society of Agricultural Engineering (Transactions of the CSAE), 2016, 32(8): 246－252. (in Chinese with English abstract)
[3]	支苏丽，周婧，赵润，等．畜禽粪便厌氧发酵过程抗生素抗性基因归趋及驱动因子分析[J]．农业工程学报，2019，35(1)：195－202.Zhi Suli, Zhou Jing, Zhao Run, et al. Analysis of antibiotic resistance genes fate and its drivers during anaerobic digestion of animal manure[J]. Transactions of the Chinese Society of Agricultural Engineering(Transactions of the CSAE), 2019, 35(1): 195－202. (in Chinese with English abstract)
[4]	许彩云，靳红梅，杜静，等．水力停留时间对猪粪厌氧发酵残留物中磺胺类抗生素分布的影响[J]．农业环境科学学报，2016，35(11)：2187－2194.Xu Caiyun, Jin Hongmei, Du Jing, et al. Effects of hydraulic retention time on sulfonamides distributions in anaerobic digestates of swine manure[J]. Journal of Agro-Environment Science, 2016, 35(11): 2187－2194. (in Chinese with English abstract)
[5]	尹福斌，季超，董红敏，等．畜禽粪便中残留抗生素对厌氧消化影响的研究进展[J]．中国农业科技导报，2016，18(5)：171－177.Yin Fubin, Ji Chao, Dong Hongmin, et al. Research progress on effect of antibiotic on anaerobic digestion treatment in animal manure[J]. Journal of Agricultural Science and Technology, 2016, 18(5): 171－177. (in Chinese with English abstract)
[6]	马旭光，江滔，唐琼，等．油菜秸秆和鸡粪比例及含固率对其发酵产甲烷特性的影响[J]．农业工程学报，2018，34(12)：236－244.Ma Xuguang, Jiang Tao, Tang Qiong, et al. Effect of total solid content on biogas production from rape stalk and chicken manure with different mixing ratios[J]. Transactions of the Chinese Society of Agricultural Engineering (Transactions of the CSAE), 2018, 34(12): 236－244. (in Chinese with English abstract)
[7]	张心如，毛长青，杜干英，等．成都市农村有机废弃污染物沼气潜力测算[J]．畜禽业，2017，28(5)：69－71．
[8]	李伟，吴树彪，Hamidou Bah，等．沼气工程高效稳定运行技术现状及展望[J]．农业机械学报，2015，46(7)：187－196, 202.Li Wei, Wu Shubiao, Hamidou Bah, et al. Status analysis and development prospect of biogas engineering technology[J]. Transactions of the Chinese Society for Agricultural Machinery, 2015, 46(7): 187－196, 202 (in Chinese with English abstract)
[9]	张春，郑利兵，郁达伟，等．沼液处理与资源化利用现状与展望[J]．中国沼气，2018，36(5)：36－46.Zhang Chun, Zheng Libing, Yu Dawei, et al. Current situation and prospect of biogas slurry treatment and its resource utilization[J]. China Biogas, 2018, 36(5): 36－46. (in Chinese with English abstract)
[10]	Elmund G K, Morrison S M, Grant D W, et al. Role of excreted chlortetracycline in modifying the decomposition process in feedlot waste[J]. Bulletin of Environmental Contamination & Toxicology, 1971, 6(2): 129－132.
[11]	Zhang M, He L Y, Liu Y S, et al. Fate of veterinary antibiotics during animal manure composting[J]. Science of the Total Environment, 2019, 650: 1363－1370.
[12]	曾巧云，丁丹，檀笑．中国农业土壤中四环素类抗生素污染现状及来源研究进展[J]．生态环境学报，2018，27(9)：1774－1782．Zeng Qiaoyun, Ding dan, Tan Xiao. Pollution status and sources of tetracycline antibiotics in agricultural soil in China: A review[J]. Ecology and Environmental Sciences, 2018, 27(9): 1774－1782. (in Chinese with English abstract)
[13]	凌文翠，范玉梅，方瑶瑶，等．京津冀地区畜禽养殖业抗生素污染现状分析[J]．环境工程技术学报，2018，8(4)：390－397．Ling Wencui, FanYumei, Fang Yaoyao, et al. Antibiotics pollution of livestock and poultry breeding in Beijing-Tianjin-Hebei region[J]. Journal of Environmental Engineering Technology, 2018, 8(4): 390－397. (in Chinese with English abstract)
[14]	Peng P C, Wang Y, Liu L Y, et al. The excretion and environmental effects of amoxicillin, ciprofloxacin, and doxycycline residues in layer chicken manure[J]. Poultry Science, 2016, 95(5): 1033－1041.
[15]	张志强．设施菜田土壤四环素类抗生素污染与有机肥安全施用[D]．北京：中国农业科学院，2013．Zhang Zhiqiang. Study on Soil Tetracyclines Antibiotics Pollution and Safe Application of Manure in Greenhouse Vegetable Field[D]. Beijing: Chinese Academy of Agricultural Sciences, 2013. (in Chinese with English abstract)
[16]	王攀攀，袁巧霞，周文兵．光催化降解沼液中四环素类抗生素效果及反应动力学研究[J]．农业工程学报， 2018，34(23)：193－198．Wang Panpan, Yuan Qiaoxia, Zhou Wenbing. Study on photocatalytic degradation and reaction kinetics of tetracycline antibiotics in biogas slurry [J]. Transactions of the Chinese Society of Agricultural Engineering (Transactions of the CSAE), 2018, 34(23): 193－198. (in Chinese with English abstract)
[17]	Cheng D, Liu X, Wang L, et al. Seasonal variation and sediment-water exchange of antibiotics in a shallower large lake in North China[J]. Science of The Total Environment, 2014, 476: 266－275.
[18]	Karina Y, Ekaterina P, Fernando P, et al. Assessment of three antimicrobial residue concentrations in broiler chicken droppings as a potential risk factor for public health and environment[J]. Environmental Research and Public Health, 2019, 16(1): 24－36.
[19]	Karcy A, Balcyoelu I A. Investigation of the tetracycline, sulfonamide, and fluoroquinolone antimicrobial compounds in animal manure and agricultural soils in Turkey[J]. Science of the Total Environment, 2009, 407(16): 4652－4664.
[20]	王良，刘思路，代光胜，等．洱海流域畜禽饲料·粪便·土壤中四环素类抗生素残留分析[J]．安徽农业科学，2017，45(18)：70－72, 76.Wang Liang, Liu Silu, Dai Guangsheng, et al. Analysis of residue of tetracyclines antibiotics in livestock manures and soil in Erhai-Lake Basin[J]. Journal of Anhui Agricultural Sciences, 2017, 45(18): 70－72, 76. (in Chinese with English abstract)
[21]	郑佳伦，刘超翔，刘琳，等．畜禽养殖业主要废弃物处理工艺消除抗生素研究进展[J]．环境化学，2017，36(1)：37－47．Zheng Jialun, Liu Chaoxiang, Liu Lin, et al. Removal of antibiotics in waste and wastewater treatment facilities of animal breeding industry: A review[J]. Environmental Chemistry, 2017, 36(1): 37－47. (in Chinese with English abstract)
[22]	Mitchell S M, Ullman J L, Teel A L, et al. The effects of the antibiotics ampicillin, florfenicol, sulfamethazine, and tylosin on biogas production and their degradation efficiency during anaerobic digestion[J]. Bioresource Technology, 2013, 149: 244－252.
[23]	Kolz A C, Moorman T B, Ong S K, et al. Degradation and metabolite production of tylosin in anaerobic and aerobic swine-manure lagoons[J]. Water Environment Research, 2005, 77(1): 49－56.
[24]	Alvarez J A, Otero L, Lema J M, et al. The effect and fate of antibiotics during the anaerobic digestion of pig manure[J]. Bioresource Technology, 2010, 101(22): 8581－8586.
[25]	Arikan O A. Degradation and metabolization of chlortetracycline during the anaerobic digestion of manure from medicated calves[J]. Journal of Hazardous Materials, 2008, 158(2): 485－490.
[26]	Stone J J, Clay S A, Zhu Z, et al. Effect of antimicrobial compounds tylosin and chlortetracycline during batch anaerobic swine manure digestion[J]. Water Research, 2009, 43(18): 4740－4750.
[27]	Sanz J L, Rodríguez N, Amils R. The action of antibiotics on the anaerobic digestion process[J]. Applied Microbiology & Biotechnology, 1997, 46: 587－592.
[28]	Withey J M, Mugo S M, Zhou T, et al. Depletion of hormones and antimicrobials in cattle manure using thermophilic anaerobic digestion[J]. Journal of Chemical Technology & Biotechnology, 2016, 91(9): 2404－2411.
[29]	Yin F, Dong H, Chao J, et al. Effects of anaerobic digestion on chlortetracycline and oxytetracycline degradation efficiency for swine manure[J]. Waste Management, 2016, 56: 540－546.
[30]	乔玮，熊林鹏，毕少杰，等．梯度提高进料浓度对鸡粪连续中温发酵产甲烷的影响[J]．农业工程学报，2018，34(9)：233－239.Qiao Wei, Xiong Linpeng, Bi Shaojie, et al. Effect of gradually raising feeding total solid on methane production during continuous mesophilic fermentation of chicken manures[J]. Transactions of the Chinese Society of Agricultural Engineering (Transactions of the CSAE), 2018, 34(9): 233－239. (in Chinese with English abstract)
[31]	APHA. Standard methods for the examination of water and waste water[S]. Washington DC: American Public Health Association, 1995.
[32]	强虹，李玉友，裴梦富．COD/SO42(对青霉素菌渣厌氧消化影响[J]．环境科学，2018，39(7)：3443－3451.Qiang Hong, Li Yuyou, Pei Mengfu. Effect of COD/SO42( ratio on anaerobic digestion of penicillin bacterial residue[J]. Environmental Science, 2018, 39(7): 3443－3451. (in Chinese with English abstract)
[33]	Frolund B, Palmgren R, Keiding K, et al. Extraction of extracellular polymers from activated sludge using a cation exchange resin[J]. Water Research, 1996, 30(8): 1749－1758.
[34]	Zhen G Y, Lu X Q, Li Y Y, et al. Innovative combination of electrolysis and Fe(II)-activated persulfate oxidation for improving the dewaterability of waste activated sludge[J]. Bioresource Technology, 2013, 136(3): 654－663.
[35]	罗庆，孙丽娜，胡筱敏. 固相萃取-高效液相色谱法测定畜禽粪便中罗红霉素和3种四环素类抗生素[J]．分析试验室，2014，33(8)：885－888．Luo Qing, Sun Lina, Hu Xiaomin. Simultaneous determination of roxithromycin and three tetracyclines in manure by high-performance liquid chromatography with a diode-array detector[J]. Chinese Journal of Analysis Laboratory, 2014, 33(8): 885－888. (in Chinese with English abstract)
[36]	张惠艳，李艳菊，顾金刚，等．高效液相色谱法测定药渣中残留金霉素[J]．分析试验室，2014，33(10)：1130－1134．Zhang Huiyan, Li Yanju, Gu Jingang, et al. Residual chlortetracycline measurement by high performance liquid chromatography[J]. Chinese Journal of Analysis Laboratory, 2014, 33(10): 1130－1134. (in Chinese with English abstract)
[37]	Li Q, Qiao W, Wang X, et al. Kinetic characterization of thermophilic and mesophilic anaerobic digestion for coffee grounds and waste activated sludge[J]. Waste Management, 2015, 36: 77－85.
[38]	Lay J J, Li Y Y, Noike T. Mathematical model for methane production from landfill bioreactor[J]. Journal of Environmental Engineering, 1998, 124(8): 730－736.
[39]	Wang R, Zhang J, Liu J, et al. Effects of chlortetracycline, Cu and their combination on the performance and microbial community dynamics in swine manure anaerobic digestion[J]. Journal of Environmental Sciences, 2018, 67(5): 206－215.
[40]	范超，王欣，刘伟，等．抗生素对鸡粪厌氧发酵过程影响的实验研究[J]．黑龙江科学，2016，7(22)：1－3,19.Fan Chao, Wang Xin, Liu Wei, et al. Study on the impact of the antibiotics on fowl manure anaerobic fermentation[J]. Heilongjiang Science, 2016, 7(22): 1－3,19. (in Chinese with English abstract)
[41]	Reyes-Contreras C, Vidal G. Methanogenic toxicity evaluation of chlortetracycline hydrochloride[J]. Electronic Journal of Biotechnology, 2015, 18(6): 445－ 450.
[42]	宋悦，魏亮亮，赵庆良，等．活性污泥胞外聚合物的组成与结构特点及环境行为[J]．环境保护科学，2017，43(2)：35－40.Song Yue, Wei Liangliang, Zhao Qingliang, et al. Chemical structure and environmental behavior of extracellular polymeric substances in Sludge: A review[J]. Environmental Protection Science, 2017,43(2): 35－40. (in Chinese with English abstract)
[43]	Lu X, Zhen G, Liu Y, et al. Long-term effect of the antibiotic cefalexin on methane production during waste activated sludge anaerobic digestion[J]. Bioresource Technology, 2014, 169(5): 644－651.
[44]	张微．四环素与胞外聚合物的相互作用及其对污泥耐药性的影响[D]．上海：东华大学，2014．Zhang Wei. Interaction between Tetracycline and Extracellular Polymers Substance(EPS) and its Effect on Activated Sludge Drug Resistance[D]. Shanghai: Donghua University, 2014. (in Chinese with English abstract)
[45]	李冬，吴青，梁瑜海，等．不同基质条件对亚硝化污泥胞外聚合物的影响[J]．哈尔滨工业大学学报，2015，47(4)：81－86.Li Dong, Wu Qing, Liang Yuhai, et al. Effect of substrate concentration and type on the content of extracellular polymeric substances in the nitrification sludge[J]. Journal of Harbin Institute of Technology, 2015, 47(4): 81－86. (in Chinese with English abstract)
[46]	Wang Q, Li J J, Yu H G, et al. Interaction mechanism between stratified extracellular polymeric substances (EPS) from activated sludge and claforan in domestic wastewater[J]. Desalination and Water Treatment. 2018, 125: 271－277.
[47]	Qi X, Gunawan P, Xu R, et al. Cefalexin-immobilized multi-walled carbon nanotubes show strong antimicrobial and anti-adhesion properties[J]. Chemical Engineering Science, 2012, 84(52): 552－556.
[48]	张翔宇，李茹莹，季民．污水生物处理中抗生素的去除机制及影响因素[J]．环境科学，2018，39(11)：5276－5288.Zhang Xiangyu, Li Ruying, Ji Min. Mechanisms and influencing factors of antibiotic removal in sewage biological treatment[J]. Environmental Science, 2018, 39(11): 5276－5288. (in Chinese with English abstract)

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