【作者】 陈敏；

【导师】 何若；

【作者基本信息】 浙江大学 ， 环境工程， 2017， 硕士

【摘要】 垃圾填埋场恶臭污染是公众环境投诉的主要问题,是造成填埋场"邻避效应"的主要原因之一。垃圾填埋处理过程中产生的含硫气体是引起填埋场恶臭污染的主要原因,其中甲硫醇（methanthiol,CH₃SH）因其臭阈值极低,对填埋场的恶臭污染有着重要影响。鉴于此,本论文以富含有含硫氨基酸的鱼肉和猪肉垃圾为材料,研究了厌氧降解过程中鱼肉和猪肉垃圾的CH₃SH产生情况、含硫化合物的转化及其微生物群落结构的演替特征;同时以城镇生活垃圾中可生物降解的组分为材料,研究了在厌氧降解过程中各类垃圾的CH₃SH产生速率和产生量,并结合我国各省份生活垃圾的填埋情况,预测了我国填埋垃圾CH₃SH的产生潜能,为生活垃圾处置过程中恶臭气体的环境风险评估以及污染控制技术的选择提供理论依据。主要结论如下:（1）有机垃圾厌氧降解过程中硫元素主要以气体的形式释放出来。鱼肉垃圾厌氧降解产气主要有CH₃SH、H₂S、甲硫醚（dimethyl sulfide,DMS）、二甲基二硫醚（dimethyl disulfide,DMDS）、CH₃CH₂SH、二甲基三硫醚（dimethyl tisulfide,DMTS）、CS2等含硫气体;而猪肉垃圾厌氧降解产气中主要为CH₃SH、H₂S、DMDS、DMTS等含硫恶臭气体。其中CH₃SH是鱼肉和猪肉垃圾厌氧降解产气中主要的含硫化合物。（2）鱼肉和猪肉垃圾厌氧降解中CH₃SH浓度呈现先增加后而下降的趋势,两类垃圾厌氧产气中CH₃SH的浓度可高达4.96～5.25%。与猪肉垃圾相比,鱼肉垃圾中蛋氨酸、半胱氨酸和总氨基酸降解较快。鱼肉垃圾厌氧降解CH₃SH累积产气量为28.12 L kgdw^-1,显著高于猪肉垃圾的累积产生量。（3）Miseq测序分析表明Proteobacteria、Firmicutes、Fusobacteria、Bacteroidetes和Actinobacteria是鱼肉和猪肉垃圾厌氧降解过程中主要的微生物。其中,Proteobacteria是初始鱼肉和猪肉垃圾中的优势微生物,随着鱼肉和猪肉垃圾厌氧降解的进行,Proteobacteria的丰度呈现下降趋势,Firmicutes、Fusobacteria和Bacteroidetes则成为优势微生物。Acinetobacter、Clostridium、Proteus、Thiobacillus、Hyphomicrobium和Pseudomonas是鱼肉和猪肉垃圾厌氧降解过程中主要硫代谢微生物,其中Acinetobacter是初始鱼肉和猪肉中主要的硫代谢微生物,而Clostridium是鱼肉和猪肉厌氧降解过程中主要的硫代谢微生物。（4）鱼肉垃圾中微生物的多样性随着厌氧降解呈现减少趋势,而猪肉垃圾中微生物的多样性呈现增长趋势。鱼肉和猪肉垃圾厌氧降解过程中微生物组成与初始样品截然不同。由于鱼肉和猪肉垃圾组成成份的不同,其厌氧降解微生物群落结构也不同,并随着厌氧降解时间呈现动态变化。鱼肉和猪肉垃圾厌氧降解过程中环境因子对种群结构的影响依次为:C/N>TS>总氨基酸>S^2->Cys≈Met>SO₄^2->TOC。其中C/N、TS、总氨基酸、S^2-、Cys和Met对样品菌群结构的变化有显著影响（P<0.1）。（5）城镇生活垃圾厌氧降解过程中,CH₃SH的产生主要集中在前期阶段（实验前24天）。在该阶段米饭、面食、蔬菜和纸类垃圾的CH₃SH累积产生量占实验期间总产生量的92.4～96.7%,鱼肉和猪肉混合垃圾的CH₃SH累积产生量占总产生量的79.7%,庭院垃圾和纤维垃圾的CH₃SH累积产生量占总产生量的63.1～67.6%。在城镇生活垃圾中,鱼肉和猪肉垃圾CH₃SH的产生量最大,可高出蔬菜、面食、米饭、布类、纸类等垃圾5～6个数量级,是主要的CH₃SH产生源。（6）结合实验各垃圾的CH₃SH产生量及我国各省份的生活垃圾填埋情况,我国各省份填埋垃圾的CH₃SH产生潜能预测表明我国填埋垃圾CH₃SH的产生主要发生在沿海省份,其中广东省最高(8.85×10⁴ m³ yr^-1),其次是上海市(5.37×10⁴ m³ yr^-1)。浙江省、江苏省、福建省、北京市以及辽宁省的填埋垃圾CH₃SH的产生潜能为3.19×10⁴～4.94×10⁴m³ yr^-1。内陆省市的CH₃SH产生潜能相对较低,为2.2×10³～9.74×10³ m³ yr^-1。更多还原

【Abstract】 Landfill odor pollution is one of the major problems of public environmental complaints,which is one of the main reasons that cause the NIMBY effect（Not-In-My-Back-Yard）.Sulfur compounds are the main sources of odor in landfills.Because of the extremely low odor threshold,CH₃SH has significant effect on landfill odor pollution.In this study,fish and pork waste which were rich in sulfur amino acids were used as the experimental materials.The production of CH₃SH,conversion of sulfur compounds and succession characteristics of microbial community were investigated during the anaerobic degradation of the fish and pork waste.Meanwhile,the production rate and yield of CH₃SH were studied during the anaerobic degradation used the biodegradable components of municipal solid waste（MSW）as the experimental materials.Based on the production of MSW in various provinces in China,the CH₃SH production potential of landfills was predicted.These results would be helpful to assess environmental risk of odor gases produced from landfills and develop techniques to control the odor pollution in landfills.The main results are as follows:（1）Sulfur reduction in the solid phase was mainly converted into gases during the anaerobic degradation of MSW.H₂S,CS2,CH₃SH,CH₃CH₂SH,dimethyl sulfide,dimethyl disulfide and dimethyl tisulfide were the main sulfur gases produced from the anaerobic degradation of fish waste,while H₂S,CH₃SH,dimethyl disulfide and dimethyl tisulfide were the main sulfur gases produced from the anaerobic degradation of pork waste.（2）During the anaerobic degradation of fish and pork waste,the CH₃SH concentration showed a trend of decline after a peak.The maximum of the CH₃SH concentration was 4.96-5.25%during the anaerobic degradation of the two wastes.Compared with the pork waste,methionine,cysteine and total amino acids in the fish waste were degraded more quickly.The cumulative production of CH₃SH from the fish waste was 28.12 L kgdw^-1,which was significantly higher than that from the pork waste.（3）Miseq sequencing analysis showed that Proteobacteria,Firmicutes,Fusobacteria,Bacteroidetes and Actinobacteria dominated in the fish and pork waste during the anaerobic degradation.Among them,Proteobacteria was the main microbe in the fresh fish and pork waste.With the anaerobic degradation of the fish and pork waste,the abundance of Proteobacteria showed a trend of decline,while Firmicutes,Fusobacteria and Bacteroidetes became the main microbes.Acinetobacter,Clostridium,Proteus,Thiobacillus,Hyphomicrobium and Pseudomonas were the main microbes of sulfur metabolism during the fish and pork waste degradation.Acinetobacter was the main microbe of initial sulfur metabolism,while Clostridium was the main microbe of whole sulfur metabolism in the fish and pork waste.（4）With the process of anaerobic degradation,the diversity of microorganisms in the fish waste declined,while it increased in the pork waste.The microbial community was different between the fish and pork waste during the anaerobic degradation.Because of the different composition of the fish and pork waste,the microbial community structure was also different between two wastes,which varied with the time of the anaerobic degradation.During the anaerobic degradation of fish and pork waste,the environmental factors affected the microbial community structure of waste with the following order of importance:C/N>TS>total amino acids>S^2->Cys ≈ Met>SO42->TOC.Among them,C/N,TS,total amino acids,S^2-,Cys and Met had significant influence on the microbial community structure（P<0.1）.（5）The CH₃SH was mainly produced in the initial stage（in the first 24 days）of the anaerobic degradation of MSW.During the initial stage,the total cumulative CH₃SH production accounted for 92.4-96.7%of the total production from the rice,flour food,vegetable and toilet paper waste,accounted for 79.7%of that from the fish and meat waste,and 63.1-67.6%of that from the yard waste and cellulose textile waste.CH₃SH was mainly produced from the anaerobic degradation of the fish and pork waste,which was 5-6 orders of magnitudes higher than that from the rice,flour food,vegetable,toilet paper and cellulose textile waste.（6）Based on the CH₃SH production from the experimental waste and the landfilled amount of MSW in provinces in China,the CH₃SH production from landfills was predicted.The results showed that the CH₃SH production potential was higher in the coastal provinces in China,of which the highest CH₃SH production potential(8.85×10⁴ m³ yr^-1)was observed in Guangdong province,followed by Shanghai(5.37×10⁴ m³ yr^-1).The CH₃SH production potential from landfills in Zhejiang,Jiangsu,Fujian,Beijing and Liaoning was 3.19×10⁴-4.94×10⁴ m³ yr^-1.The CH₃SH production potential from landfills in inland provinces was relatively lower,which was 2.2×10³-9.74×10³ m³ yr^-1.更多还原