单段式自热高温（微）好氧消化工艺处理城市污水厂污泥及其稳定化机理研究
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摘要
稳定化处理是污泥减量化、无害化的一个重要手段，也是污泥处理与处置的重要环节之一。污泥稳定化处理方法包括物理、化学及生物法，生物法由于运行成本低、安全可靠而被广泛采用。污泥自热高温好氧消化（ATAD）工艺属好氧消化范畴，具有污泥停留时间短、病原菌灭活效率高等优势。该工艺较好克服了传统生物稳定法污泥停留时间长、设施占地面积大等不足，因而自上世纪九十年代开始在欧洲、北美等城市污泥稳定化处理工艺中得到较快的应用与推广。目前，我国在ATAD工艺稳定化处理污泥方面研究较少，也无应用实例。
借鉴ATAD工艺已有研究基础，本课题组开发了一套新型的单段式污泥高温（微）好氧（ATMAD）消化装置，该装置在满足污泥稳定化处理效果的同时，具有结构简单、占地面积小等优势，其有效性已初步得到试验证明，但相关的污泥稳定化机理亟待深入研究。本论文从物质迁移转化规律、嗜热微生物种群多样性、有机物降解动力学等方面阐述了单段式ATMAD工艺的污泥稳定化过程与机理，并通过中试运行过程考察了ATMAD工艺的污泥稳定化效果、建立了消化体系的热平衡方程。
单段式ATMAD工艺批式运行结果表明：稳定化处理污泥时，进料污泥固体物（TS）浓度以5～6%较为适宜（挥发性固体物VS含量约3.3～4.0%）；增大曝气量有利于提高VS去除率，但不能显著促进有机物的快速降解，适宜曝气强度为1.0～1.2L/(h·L泥)；污泥稳定化过程受消化温度影响最为明显，反应器运行温度在50～60oC条件下VS去除率明显较高。污泥经高温消化后其脱水性能明显恶化，延长消化时间有利于适当改善消化污泥的脱水性能。ATMAD工艺按半间歇运行方式在55oC消化温度下稳定化处理污泥时，水力停留时间（HRT）不低于13d的消化体系VS去除率均高于38%，且粪大肠菌群与沙门氏菌均有效灭活，消化污泥达到A类污泥各项指标。
考察了污泥稳定化过程VFA组分及其浓度变化，阐述了消化体系有机组分的代谢途径与规律。消化体系上清液有机物浓度相对较高或快速增加时，生化代谢系统可通过乙酸、丙酸、丁酸等合成途径来满足消化体系对氧化态NAD+的需求；消化体系大量累积VFA时，除乙酸外，丙酸、异丁酸与异戊酸均为主要组分，其浓度远高于正丁酸与正戊酸。在曝气强度不变时，有机底物的生化代谢过程对消化体系ORP值存在明显影响。
以VS为评价指标建立了单段式ATMAD工艺的有机物降解动力学。消化体系VS降解的宏观一级动力学方程为（消化时间以d计量）：污泥水力停留时间不低于10d时，动力学公式计算值与试验测定结果相对误差均低于10%；中试系统半间歇运行过程中，理论计算值与实际值相对误差不超过6%。
分离、纯化了典型的嗜热微生物并进行了生物强化试验。分离的两株典型嗜热菌T1（No: HQ436531）与T2（No: HQ436531）分别属于Hydrogenophilaceae与Xanthomonodaceae。接种嗜热菌株有利于提高污泥稳定化初期的有机物降解效果，但微观环境对稳定化过程也存在明显影响。单独接种嗜热菌T2的反应器在整个消化过程均比空白对照反应器有更高的VS去除率。DGGE图谱表明：好氧、兼性与厌氧微生物可共存于污泥高温（微）好氧消化体系。
本论文通过中试运行考察了ATMAD工艺的污泥稳定化效果，并建立了消化体系的热平衡方程。中试系统（HRT为10d）在半间歇式操作条件下连续运行10d后，平均VS去除率为37.8%，反应器运行温度维持在58～62oC，pH值变化范围为7.8～8.2，ORP值在－325～－260mV范围内波动，氧利用率达30%左右。消化体系在60oC左右运行时，因机械能转化而产生的热量占消化体系总放热量的30.8%。可见，单段式ATMAD工艺并非完全的“自热”升温。
Sludge stabilization is an important step for sewage sludge treatment and disposal.Autothermal thermophilic aerobic digestion (ATAD) has the advantage of rapid volatilesolids (VS) reduction, short sludge retention time (SRT), and efficient pathogeninactivation, so it is a promising aerobic process that produces Class A biosolids. SinceATAD technology was first introduced in the early1970s, significant advances had beenmade in the optimization and adaption of ATAD technology for sewage sludgestabilization, and a number of ATAD units had been constructed in Europe and NorthAmerica. Although ATAD process can stabilize sewage sludge and has merits overtraditional aerobic and anaerobic digestion processes, there is no ATAD system used inChina due to lack of fundamental research in this field.
The conventional ATAD systems are normally two－stage process. In China, a one－stage ATAD digestion device has been developed due to its simple units and small areaoccupation, and it is named as ATMAD system due to micro－aerobic operationcondition. Bench－scale experiments have revealed that a one－stage ATMAD systemcould achieve the same stabilization effects as two－stage ATAD process, so it haspresented potential application for sewage sludge stabilization in small－and medium－sized wastewater treatment plants (WWTPs). To better understand stabilizationmechanism of one－stage ATMAD process and provide recommendations for its practicaloperation, this project mainly focused on following aspects:(1) optimizing operationparameters of one－stage ATMAD system;(2) investigating digestion efficacy (includingVS removal and pathogen inactivation) and the release of nutrition components as wellas dewatering characteristics of the digested sludge;(3) examining microbial diversity during digestion process;(4) proposing biochemical metabolic pathway;(5) setting up alarge－scale ATMAD digester to examine digestion efficacy of one－stage ATMADprocess and to analyze heat balance.
The optimal parameters of one－stage ATMAD process are5～6%total solids (TS),1.0～1.2L/(h·L sludge) aeration intensity, and50～60oC digestion temperature. Higheraeration moderately favores VS removal, however it has adverse impact on autothermalthermophilic condition. Digestion temperature is a major parameter for sludgestabilization, a one－stage ATMAD system could achieve more efficient digestionefficacy with moderate increase of thermophilic temperature, but ATMAD system shallattain low VS removal as digestion temperature is up to65oC. Thermophilic digestionresults in poor dewaterability of the digested sludge, and longer SRT is helpful tomoderately improve the dewaterability. Semi－continuous operation of one－stageATMAD digester at TS level5～6%, aeration intensity1.0～1.2L/(h·L sludge), andtemperature55oC indicated that at least13－day HRT（hydraulic retention time）isrequired to achieve above38%VS removal, and pathogen inactivation of the digestedsludge also meet the requirements of Class A biosolids.
As the concentration of organic matter rapidly increases during ATMAD process,aeration is unable to meet the demand of oxygen, and the system maintains low oxidationreduction potential (ORP). As a result, digestion system could regulate its metabolicpathways to produce acetic, propionic, butyric acids and other volatile fatty acids (VFA)constituents in order to meet the demand for NAD+. Based on the variation of VFA andfundamental theories of aerobic and anaerobic digestions, a biochemical model isproposed. As aeration density is constant, the biochemical metabolic process of substratehas significant impact on ORP level.
VS can be regarded as a suitable indicator for biodegradation kinetics of organicmatter, and VS concentration can be expressed asRelative error is less than6%between the determined results and the calculated valuesfor a large－scale ATMAD digester as kinetics equation is used during semi－continuous operation process.
Two representative thermophilic strains T1(No: HQ436531) and T2(No: HQ436531) were isolated, and16S rRNA gene analysis indicated that they belongedto Hydrogenophilaceae and Xanthomonodaceae, respectively. Inoculation with thermo－philic strains can speed up the degradation of organic matter during the early stage ofthermophilic aerobic digestion, and both specific thermophilic strains and micro－environment significantly affect VS removal. Strains T2can completely acclimatize itselfto thermophilic digestion and favor digestion process. According to DGGE profiles,aerobic, anaerobic or facultative microbes can co－exist in thermophilic aerobic digester,which jointly constitute microbial community and contribute to sludge stabilization.
A large－scale digester was designed with effective volume of10m3, and semi－continuous operation was conducted at10－day HRT to evaluate the effectiveness of one－stage ATMAD process and to analyze the heat balance of digestion system. From11to20d after start－up, digestion temperature fluctuated moderately between58and62oC,average VS removal was37.8%, the pH and ORP were7.8～8.2and－325～－260mV,respectively, and oxygen utilization coefficient was about30%. The heat derived frommechanical mixing energy contributed30.8%of the total heat release, so one－stageATMAD system is not completely self－heating.
借鉴ATAD工艺已有研究基础，本课题组开发了一套新型的单段式污泥高温（微）好氧（ATMAD）消化装置，该装置在满足污泥稳定化处理效果的同时，具有结构简单、占地面积小等优势，其有效性已初步得到试验证明，但相关的污泥稳定化机理亟待深入研究。本论文从物质迁移转化规律、嗜热微生物种群多样性、有机物降解动力学等方面阐述了单段式ATMAD工艺的污泥稳定化过程与机理，并通过中试运行过程考察了ATMAD工艺的污泥稳定化效果、建立了消化体系的热平衡方程。
单段式ATMAD工艺批式运行结果表明：稳定化处理污泥时，进料污泥固体物（TS）浓度以5～6%较为适宜（挥发性固体物VS含量约3.3～4.0%）；增大曝气量有利于提高VS去除率，但不能显著促进有机物的快速降解，适宜曝气强度为1.0～1.2L/(h·L泥)；污泥稳定化过程受消化温度影响最为明显，反应器运行温度在50～60oC条件下VS去除率明显较高。污泥经高温消化后其脱水性能明显恶化，延长消化时间有利于适当改善消化污泥的脱水性能。ATMAD工艺按半间歇运行方式在55oC消化温度下稳定化处理污泥时，水力停留时间（HRT）不低于13d的消化体系VS去除率均高于38%，且粪大肠菌群与沙门氏菌均有效灭活，消化污泥达到A类污泥各项指标。
考察了污泥稳定化过程VFA组分及其浓度变化，阐述了消化体系有机组分的代谢途径与规律。消化体系上清液有机物浓度相对较高或快速增加时，生化代谢系统可通过乙酸、丙酸、丁酸等合成途径来满足消化体系对氧化态NAD+的需求；消化体系大量累积VFA时，除乙酸外，丙酸、异丁酸与异戊酸均为主要组分，其浓度远高于正丁酸与正戊酸。在曝气强度不变时，有机底物的生化代谢过程对消化体系ORP值存在明显影响。
以VS为评价指标建立了单段式ATMAD工艺的有机物降解动力学。消化体系VS降解的宏观一级动力学方程为（消化时间以d计量）：污泥水力停留时间不低于10d时，动力学公式计算值与试验测定结果相对误差均低于10%；中试系统半间歇运行过程中，理论计算值与实际值相对误差不超过6%。
分离、纯化了典型的嗜热微生物并进行了生物强化试验。分离的两株典型嗜热菌T1（No: HQ436531）与T2（No: HQ436531）分别属于Hydrogenophilaceae与Xanthomonodaceae。接种嗜热菌株有利于提高污泥稳定化初期的有机物降解效果，但微观环境对稳定化过程也存在明显影响。单独接种嗜热菌T2的反应器在整个消化过程均比空白对照反应器有更高的VS去除率。DGGE图谱表明：好氧、兼性与厌氧微生物可共存于污泥高温（微）好氧消化体系。
本论文通过中试运行考察了ATMAD工艺的污泥稳定化效果，并建立了消化体系的热平衡方程。中试系统（HRT为10d）在半间歇式操作条件下连续运行10d后，平均VS去除率为37.8%，反应器运行温度维持在58～62oC，pH值变化范围为7.8～8.2，ORP值在－325～－260mV范围内波动，氧利用率达30%左右。消化体系在60oC左右运行时，因机械能转化而产生的热量占消化体系总放热量的30.8%。可见，单段式ATMAD工艺并非完全的“自热”升温。
Sludge stabilization is an important step for sewage sludge treatment and disposal.Autothermal thermophilic aerobic digestion (ATAD) has the advantage of rapid volatilesolids (VS) reduction, short sludge retention time (SRT), and efficient pathogeninactivation, so it is a promising aerobic process that produces Class A biosolids. SinceATAD technology was first introduced in the early1970s, significant advances had beenmade in the optimization and adaption of ATAD technology for sewage sludgestabilization, and a number of ATAD units had been constructed in Europe and NorthAmerica. Although ATAD process can stabilize sewage sludge and has merits overtraditional aerobic and anaerobic digestion processes, there is no ATAD system used inChina due to lack of fundamental research in this field.
The conventional ATAD systems are normally two－stage process. In China, a one－stage ATAD digestion device has been developed due to its simple units and small areaoccupation, and it is named as ATMAD system due to micro－aerobic operationcondition. Bench－scale experiments have revealed that a one－stage ATMAD systemcould achieve the same stabilization effects as two－stage ATAD process, so it haspresented potential application for sewage sludge stabilization in small－and medium－sized wastewater treatment plants (WWTPs). To better understand stabilizationmechanism of one－stage ATMAD process and provide recommendations for its practicaloperation, this project mainly focused on following aspects:(1) optimizing operationparameters of one－stage ATMAD system;(2) investigating digestion efficacy (includingVS removal and pathogen inactivation) and the release of nutrition components as wellas dewatering characteristics of the digested sludge;(3) examining microbial diversity during digestion process;(4) proposing biochemical metabolic pathway;(5) setting up alarge－scale ATMAD digester to examine digestion efficacy of one－stage ATMADprocess and to analyze heat balance.
The optimal parameters of one－stage ATMAD process are5～6%total solids (TS),1.0～1.2L/(h·L sludge) aeration intensity, and50～60oC digestion temperature. Higheraeration moderately favores VS removal, however it has adverse impact on autothermalthermophilic condition. Digestion temperature is a major parameter for sludgestabilization, a one－stage ATMAD system could achieve more efficient digestionefficacy with moderate increase of thermophilic temperature, but ATMAD system shallattain low VS removal as digestion temperature is up to65oC. Thermophilic digestionresults in poor dewaterability of the digested sludge, and longer SRT is helpful tomoderately improve the dewaterability. Semi－continuous operation of one－stageATMAD digester at TS level5～6%, aeration intensity1.0～1.2L/(h·L sludge), andtemperature55oC indicated that at least13－day HRT（hydraulic retention time）isrequired to achieve above38%VS removal, and pathogen inactivation of the digestedsludge also meet the requirements of Class A biosolids.
As the concentration of organic matter rapidly increases during ATMAD process,aeration is unable to meet the demand of oxygen, and the system maintains low oxidationreduction potential (ORP). As a result, digestion system could regulate its metabolicpathways to produce acetic, propionic, butyric acids and other volatile fatty acids (VFA)constituents in order to meet the demand for NAD+. Based on the variation of VFA andfundamental theories of aerobic and anaerobic digestions, a biochemical model isproposed. As aeration density is constant, the biochemical metabolic process of substratehas significant impact on ORP level.
VS can be regarded as a suitable indicator for biodegradation kinetics of organicmatter, and VS concentration can be expressed asRelative error is less than6%between the determined results and the calculated valuesfor a large－scale ATMAD digester as kinetics equation is used during semi－continuous operation process.
Two representative thermophilic strains T1(No: HQ436531) and T2(No: HQ436531) were isolated, and16S rRNA gene analysis indicated that they belongedto Hydrogenophilaceae and Xanthomonodaceae, respectively. Inoculation with thermo－philic strains can speed up the degradation of organic matter during the early stage ofthermophilic aerobic digestion, and both specific thermophilic strains and micro－environment significantly affect VS removal. Strains T2can completely acclimatize itselfto thermophilic digestion and favor digestion process. According to DGGE profiles,aerobic, anaerobic or facultative microbes can co－exist in thermophilic aerobic digester,which jointly constitute microbial community and contribute to sludge stabilization.
A large－scale digester was designed with effective volume of10m3, and semi－continuous operation was conducted at10－day HRT to evaluate the effectiveness of one－stage ATMAD process and to analyze the heat balance of digestion system. From11to20d after start－up, digestion temperature fluctuated moderately between58and62oC,average VS removal was37.8%, the pH and ORP were7.8～8.2and－325～－260mV,respectively, and oxygen utilization coefficient was about30%. The heat derived frommechanical mixing energy contributed30.8%of the total heat release, so one－stageATMAD system is not completely self－heating.
引文
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