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题名: 猪粪生物处理过程中残留四环素类抗生素与重金属铜的迁移转化
作者: 吴晓凤
学位类别: 硕士
答辩日期: 2011
授予单位: 中国科学院研究生院
授予地点: 北京
导师: 魏源送
关键词: 猪粪 ; Swine manure ; 四环素类抗生素TCs及代谢产物 ; Tetracyclines and degradation products ; 重金属铜Cu ; Cu ; 迁移转化 ; Behavior
其他题名: The Behavior of Residual Tetracyclines and Cu during the Biological Treatment of Swine Manure
中文摘要:       集约化畜禽养殖场的推广和兴起,产生了大量的畜禽粪便。残留在畜禽粪便中的兽用抗生素和重金属随着畜禽粪便的农田利用而带来了严重的环境污染。如何有效控制和削减兽用抗生素和重金属的复合污染风险,是畜禽粪便安全农用面临的严峻挑战。堆肥和厌氧消化是畜禽粪便广为应用的资源化和无害化处理方法。因此,本文以畜禽养殖业中最常用的四环素类抗生素TCs和微量重金属添加剂铜Cu为研究对象,考察猪粪生物处理过程(堆肥和厌氧消化)中TCs和Cu的迁移转化,以期为畜禽粪便生物处理过程中TCs和Cu的有效去除和安全转化提供科学依据和技术支持。 首先完善了畜禽粪便中TCs及其代谢产物同时检测的分析方法(UPLC-MS/MS)。四环素TC、土霉素OTC和金霉素CTC的回收率分别为71~89%、66~94% 和66~84%;去甲基金霉素DMCTC的回收率为52~64%;差向异构产物的回收率在32~51%之间;脱水及差向脱水产物的回收率低于30%;检出限和定量限分别在1.668~17.270 μg/kg和5.561~57.567 μg/kg范围内,表明该方法具有较高的灵敏度; 然后开展了规模化堆肥现场调查,初步明确了堆肥过程中TCs与Cu的迁移转化行为特征。并且中试规模猪粪堆肥研究证实了堆肥能够有效地去除粪便中残留的TCs,其中CTC、OTC和TC的去除率分别达到了74%、92%和70%;简单和改良型一级反应动力学模型都能很好地模拟堆肥过程中三种母体TCs的降解过程,但改良模型拟合的效果更佳,得出CTC、OTC和TC的半衰期分别为8.2、1.1和10.0天。规模化堆肥现场调查和中试规模猪粪堆肥研究均表明,重金属Cu主要以稳定的有机结合态形式存在,且堆肥过程对总Cu的浓度及其形态分布都有一定的影响。 初步考察了猪粪批式厌氧消化过程中TCs和Cu的迁移转化行为。与对照组相比,接种对厌氧消化过程中固相TCs的去除并没有表现出明显的促进作用;液相中TCs的含量为μg/L级别,表明TCs更易被吸附于固相体系中;厌氧消化过程中Cu从液相迁移到固相中而导致固相中铜的富集,而Cu逐渐从不稳定态向稳定态转化。
英文摘要:       A large amount of animal manure has been produced with the development of confined animal feeding operations (CAFOs). The residual veterinary antibiotics and heavy metals in animal manure have caused serious environmental pollution with manure used as fertilizers in agricultural land. It is a big issue to control and reduce the risk aroused by complex pollution of veterinary antibiotics and heavy metals in animal manure for its safe land application. It is well known that both composting and anaerobic digestion are widely used biological technologies to treat and resource animal manure. In this study, the most commonly used tetracyclines (TCs) and Cu in animal husbandry were selected, and our purpose is to support integrated management of animal manure in China by investigating the fate and behaviour of residual TCs and Cu during composting and anaerobic digestion of swine manure. Firstly, a method using ultra performance liquid chromatography with tandem mass spectrometry (UPLC-MS/MS) was developed to simultaneously determine TCs and their degradation products in swine manure. With the developed UPLC-MS/MS method, recoveries of TC, OTC and CTC were 71~89%、66~94% and 66~84%, respectively. The recovery of demeclocycline was in the range of 52~64%, and for the epimers, they varied between 32% and 51% while the anhydro-tetracyclines and their corresponding epimers showed poor recoveries below 30%. The limit of detection and quantitation for the three tetracyclines and their degradation products were in the range of 1.668~17.270 μg/kg and 5.561~57.567 μg/kg, respectively, indicating a high sensitivity for this method. Results of both a field survey of a full-scale animal manure composting and a pilot scale swine manure composting clearly showed that composting is an effective way to remove TCs. The removal rates of CTC, OTC and TC in the pilot scale swine manure composting were 74%, 92% and 70%, respectively. Both the simple and adjusted first-order kinetic models successfully fit the degradation process of CTC, OTC and TC, but the adjusted first-order kinetic model fit much better with the calculated half-lives of 8.2, 1.1 and 10.0 days, respectively. In addition, both the large-scale and pilot scale composting suggested that Cu was predominately existed in the more stable form of combining with organics, and composting had some effects on total Cu concentration and its speciation to some degree. Finally, the behaviour of TCs and Cu during batch swine manure anaerobic digestion were preliminarily investigated. Compared with the control group, there was no obvious influence of inoculum in promoting TCs’ removal rates in solid phase. The concentrations of TCs in liquid phase were found at the level of μg/L, indicating that TCs were more likely to be absorbed by solid matrices. During the anaerobic digestion, the transferring behavior of Cu from liquid to solid phase occurred and thus resulted in a phenomenon of Cu condensation. The results of Cu speciation indicated that Cu was moving toward the more stable fraction of bounding to organics during anaerobic digestion.
内容类型: 学位论文
URI标识: http://ir.rcees.ac.cn/handle/311016/35092
Appears in Collections:水污染控制技术研究室_学位论文

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Recommended Citation:
吴晓凤. 猪粪生物处理过程中残留四环素类抗生素与重金属铜的迁移转化[D]. 北京. 中国科学院研究生院. 2011.
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