水源水库沉积物多相界面污染物迁移转化与污染控制研究
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摘要
沉积物内源污染是水源水库面临的突出问题。沉积物多相界面是内源污染发生的重要环境边界层。本文针对水源水库多相界面高静水压、低溶解氧、低温、贫营养等多重特性，采用现场调查与实验室模拟相结合的方法，探讨了多相界面氮及溶解性有机物（DOM）循环转化释放规律及不同静水压对该多相界面过程的动态调控过程。在此基础上，分别采用扬水曝气强化化学稳定（原位稳定化处理P、Fe、Mn等）和覆盖填料结合固定化功能微生物（降低沉积物氮及有机污染负荷）的方法初步探索了适合于水源水库沉积物原位污染控制的方法与技术。研究得到以下主要结论：
（1）水源水库氮、磷赋存形态、稳定性及对多相界面循环转化释放贡献研究结果表明：沉积物中铁/铝-磷（Fe/Al-P）是多相界面PO_4~(3-)释放的最主要来源；离子交换态氮（IEF-N），弱酸提取态氮（WAEF-N）和强氧化剂提取态氮SOEF-N是多相界面体系沉积物氮释放的主要来源。SOEF-N是可转化态氮优势存在形态，WAEF-N次之；结合能力最弱、最易释放进入上覆水体的IEF-N所占比例最少。三种无机提取态可转化态氮，均以NH_4~+-N为主要存在形式。厌氧还原条件可促进沉积物中内源磷释放进入上覆水。
（2）多相界面氮及DOM循环转化释放特性研究结果表明：厌氧条件（DO<1.0mg/L）使氨氮、总氮及DOM在上覆水中累积，影响上覆水水质；多相界面处DO为2~3mg/L时，分子量500~3200Da范围内DOM可被沉积物中微生物较为彻底分解利用；采用强化充氧措施降低沉积物氮及有机污染负荷时，控制DO=2~3mg/L既能保证上覆水水质，又可兼顾能源消耗经济利益，沉积物中总氮STN及有机质SOC的降幅分别为7.27%和21.00%；不同强化充氧条件导致表层沉积物中微生物群落结构PLFA组成显著不同，脲酶、硝酸盐还原酶、沉积物STN、SOC及多相界面DO等环境因素对沉积物中微生物群落结构差异贡献最大；碳源不足是限制多相界面反硝化的重要因素；多相界面气体产物主要由CH_4、N_2、少量CO_2和痕量H_2组成，低温条件下N_2占总体积的91.73%；常温条件下，N_2和CH_4基本各占总体积的近一半，温度对CO_2和H_2含量基本无影响。低温条件对多相界面有机质厌氧分解具有抑制作用，但有利于沉积物硝化-反硝化反应。
（3）不同静水压对多相界面氮及DOM转化过程影响研究结果表明：静水压是影响不同水深水源水库多相界面上覆水水质及沉积物中微生物群落结构的最重要因素。在0.1MPa~1.0MPa静水压条件下，高静水压促进了多相界面氮及有机质释放，对有机质降解及氨化过程具有促进作用，但对反硝化过程无明显影响。在此静水压范围内，高静水压使氨氮、硝氮、DOM等污染物在多相界面上覆水中大量积累，严重影响上覆水水质。高静水压使上覆水DOM中增加了与色氨酸相关的类蛋白荧光峰、紫外区类富里酸荧光峰及与芳香性蛋白类结构有关的荧光峰，主要由微生物增多及其增多后促进了对沉积物中有机质的降解引起；高静水压使上覆水DOC分子量分布多分散系数ρ减小，在不同反应时期表现出不同分布趋势，原有小分子量DOM被高静水压下特有微生物进一步彻底分解利用而消失；高静水压使沉积物中脱氢酶及蛋白酶活性显著增强，对脲酶及硝酸盐还原酶活性影响不大；PLFA与PCR-DGGE测定分析结果表明，不同静水压下，微生物群落在结构及遗传性方面均表现出显著差异，在0.1MPa~1.0MPa静水压范围内，高静水压下微生物群落结构多样性高于常压。
（4）原位污染控制技术：扬水曝气强化化学稳定技术可有效抑制沉积物中磷、铁的释放，平均抑制率分别可达63.2%和58.6%。随混凝剂PAC投量增大，抑制效果变好，助凝剂PAM有助于增强PAC对磷及铁的抑制效果。PAC和PAM对磷释放的抑制作用主要通过其水解产生的铝盐与释放进入上覆水体的PO_4~(3-)重新结合形成Al-P实现。该技术具有稳定、高效、长效、无二次隐患等优点。固定化高效功能微生物活性填料覆盖方法原位控制沉积物总氮及有机物效果优于活性填料覆盖与直接投菌。覆盖层中沸石起主要作用，通过吸附、离子交换等作用对多相界面大量释放的NH_4~+进行快速拦截，进而通过微生物将其降解转化，实现沸石原位清洁再生，同时从根本上降低了多相界面体系氮及有机污染负荷，实现良性循环。
Endogenous pollution happening on the sediments multi-phase interface is the mostimportant problem of drinking water reservoir. For most drinking wter reservoirs, theirsediments multi-phase interface is usually under high hydrostatic pressure, aerobic, lowtemperature and oligotrophic conditions. Moreover, considering the health effect, thepollution controlling technology for drinking water reservoirs must be elaborately selected. Inthis study, the nitrogen and dissolved organic matter fluxes on the multi-phase interface andhydrostatic pressure effects on this course were researched by field investigation andlaboratory simulation. And the pollution controlling methods suitable for drinking waterreservoirs were also studied. The crucial results and conclusions are as follows:
(1)Fe/Al-P in the sediments was the most importan source for PO_4~(3-)release. Andnitrogen release were mainly coming from the IEF-N, WAEF-N and SOEF-N forms insediments. SOEF-N was the preponderant form of transferable nitrogen and is followed byWAEF-N. IEF-N, which can released into overlying water most easily, covered the least oftransferable nitrogen. Aerobic and reductive condition can accelerate PO_4~(3-)release.
(2)NH_4~+, TN and DOC cumulated in large quantities in overlying water under aerobiccondition, which deteriorated the water quality badly. When the DO in multi-phase interfacewas2~3mg/L, the DOC with molecular weights of500~3200Da can be decomposeddrastically by the microorganisms in the sediments and the STN and SOC contents in thesediments can be reduced by7.27%and21.00%respectively. Different DO concentration inthe multi-phase interface will effect some enzymes activities, STN, and SOC in the sediments,thus the microbial community structures in the sediments shown by PLFAs were remarkablydifferent. being devoid of suitable carbon source was the most important limiting effect fordenitrification on the multi-phase interface. The gas products on the multi-phase interfacemainly included of CH_4, N_2, CO_2and H_2. Under low temperature, N_2covered91.73%of total gas volume and under room temperature N_2and CH_4each covered nearly half of total gasvolume. Low temperature can inhibit microorganisms decomposing organic matter andpromote microorganisms nitrification and denitrification.
(3) Hydrostatic pressure was the most important effect factor to overlying water quality andmicrobial community structures in sediments. Under0.1MPa~1.0MPa, high hydrostaticpressure can promote nitrogen and organic matter release and deteriorate overlying waterquality. Furthermore, under high hydrostatic pressure, the polydispersity of DOMρreduced and DOC with low molecular weights were decomposed by microorganisms anddispersed in overlying water. Under different hydrostatic pressure, the microbial communitystructure in the sediments were different. The microbial community diversity under highhydrostatic pressure was much richer than under low hydrostatic pressure.
(4)Water lifting aerator combined with chemical stabilization can inhibit PO_4~(3-)and Fe2+release effectively, and the inhibit efficiencies can reach63.2%and58.6%respectively. Thehigher the PAC concentration was, the better the inhibiting efficiency was, and PAM additioncan strengthen the inhibiting efficiency significantly. The mechanism was that thehydrolyzing products can combine with PO_4~(3-)and form Al-P. The active capping materialcovered by especially selectived biofilm was more effective than capping material orfunctional microbes was singled used. The zeolites in the capping layers can adsrob the NH_4~+and the biofilm covering on the zeolites then decomposed them. Simultaneously the zeoliteswere renewed. Therefore the polluting load of STN and SOC in the sediments can bereduced.
（1）水源水库氮、磷赋存形态、稳定性及对多相界面循环转化释放贡献研究结果表明：沉积物中铁/铝-磷（Fe/Al-P）是多相界面PO_4~(3-)释放的最主要来源；离子交换态氮（IEF-N），弱酸提取态氮（WAEF-N）和强氧化剂提取态氮SOEF-N是多相界面体系沉积物氮释放的主要来源。SOEF-N是可转化态氮优势存在形态，WAEF-N次之；结合能力最弱、最易释放进入上覆水体的IEF-N所占比例最少。三种无机提取态可转化态氮，均以NH_4~+-N为主要存在形式。厌氧还原条件可促进沉积物中内源磷释放进入上覆水。
（2）多相界面氮及DOM循环转化释放特性研究结果表明：厌氧条件（DO<1.0mg/L）使氨氮、总氮及DOM在上覆水中累积，影响上覆水水质；多相界面处DO为2~3mg/L时，分子量500~3200Da范围内DOM可被沉积物中微生物较为彻底分解利用；采用强化充氧措施降低沉积物氮及有机污染负荷时，控制DO=2~3mg/L既能保证上覆水水质，又可兼顾能源消耗经济利益，沉积物中总氮STN及有机质SOC的降幅分别为7.27%和21.00%；不同强化充氧条件导致表层沉积物中微生物群落结构PLFA组成显著不同，脲酶、硝酸盐还原酶、沉积物STN、SOC及多相界面DO等环境因素对沉积物中微生物群落结构差异贡献最大；碳源不足是限制多相界面反硝化的重要因素；多相界面气体产物主要由CH_4、N_2、少量CO_2和痕量H_2组成，低温条件下N_2占总体积的91.73%；常温条件下，N_2和CH_4基本各占总体积的近一半，温度对CO_2和H_2含量基本无影响。低温条件对多相界面有机质厌氧分解具有抑制作用，但有利于沉积物硝化-反硝化反应。
（3）不同静水压对多相界面氮及DOM转化过程影响研究结果表明：静水压是影响不同水深水源水库多相界面上覆水水质及沉积物中微生物群落结构的最重要因素。在0.1MPa~1.0MPa静水压条件下，高静水压促进了多相界面氮及有机质释放，对有机质降解及氨化过程具有促进作用，但对反硝化过程无明显影响。在此静水压范围内，高静水压使氨氮、硝氮、DOM等污染物在多相界面上覆水中大量积累，严重影响上覆水水质。高静水压使上覆水DOM中增加了与色氨酸相关的类蛋白荧光峰、紫外区类富里酸荧光峰及与芳香性蛋白类结构有关的荧光峰，主要由微生物增多及其增多后促进了对沉积物中有机质的降解引起；高静水压使上覆水DOC分子量分布多分散系数ρ减小，在不同反应时期表现出不同分布趋势，原有小分子量DOM被高静水压下特有微生物进一步彻底分解利用而消失；高静水压使沉积物中脱氢酶及蛋白酶活性显著增强，对脲酶及硝酸盐还原酶活性影响不大；PLFA与PCR-DGGE测定分析结果表明，不同静水压下，微生物群落在结构及遗传性方面均表现出显著差异，在0.1MPa~1.0MPa静水压范围内，高静水压下微生物群落结构多样性高于常压。
（4）原位污染控制技术：扬水曝气强化化学稳定技术可有效抑制沉积物中磷、铁的释放，平均抑制率分别可达63.2%和58.6%。随混凝剂PAC投量增大，抑制效果变好，助凝剂PAM有助于增强PAC对磷及铁的抑制效果。PAC和PAM对磷释放的抑制作用主要通过其水解产生的铝盐与释放进入上覆水体的PO_4~(3-)重新结合形成Al-P实现。该技术具有稳定、高效、长效、无二次隐患等优点。固定化高效功能微生物活性填料覆盖方法原位控制沉积物总氮及有机物效果优于活性填料覆盖与直接投菌。覆盖层中沸石起主要作用，通过吸附、离子交换等作用对多相界面大量释放的NH_4~+进行快速拦截，进而通过微生物将其降解转化，实现沸石原位清洁再生，同时从根本上降低了多相界面体系氮及有机污染负荷，实现良性循环。
Endogenous pollution happening on the sediments multi-phase interface is the mostimportant problem of drinking water reservoir. For most drinking wter reservoirs, theirsediments multi-phase interface is usually under high hydrostatic pressure, aerobic, lowtemperature and oligotrophic conditions. Moreover, considering the health effect, thepollution controlling technology for drinking water reservoirs must be elaborately selected. Inthis study, the nitrogen and dissolved organic matter fluxes on the multi-phase interface andhydrostatic pressure effects on this course were researched by field investigation andlaboratory simulation. And the pollution controlling methods suitable for drinking waterreservoirs were also studied. The crucial results and conclusions are as follows:
(1)Fe/Al-P in the sediments was the most importan source for PO_4~(3-)release. Andnitrogen release were mainly coming from the IEF-N, WAEF-N and SOEF-N forms insediments. SOEF-N was the preponderant form of transferable nitrogen and is followed byWAEF-N. IEF-N, which can released into overlying water most easily, covered the least oftransferable nitrogen. Aerobic and reductive condition can accelerate PO_4~(3-)release.
(2)NH_4~+, TN and DOC cumulated in large quantities in overlying water under aerobiccondition, which deteriorated the water quality badly. When the DO in multi-phase interfacewas2~3mg/L, the DOC with molecular weights of500~3200Da can be decomposeddrastically by the microorganisms in the sediments and the STN and SOC contents in thesediments can be reduced by7.27%and21.00%respectively. Different DO concentration inthe multi-phase interface will effect some enzymes activities, STN, and SOC in the sediments,thus the microbial community structures in the sediments shown by PLFAs were remarkablydifferent. being devoid of suitable carbon source was the most important limiting effect fordenitrification on the multi-phase interface. The gas products on the multi-phase interfacemainly included of CH_4, N_2, CO_2and H_2. Under low temperature, N_2covered91.73%of total gas volume and under room temperature N_2and CH_4each covered nearly half of total gasvolume. Low temperature can inhibit microorganisms decomposing organic matter andpromote microorganisms nitrification and denitrification.
(3) Hydrostatic pressure was the most important effect factor to overlying water quality andmicrobial community structures in sediments. Under0.1MPa~1.0MPa, high hydrostaticpressure can promote nitrogen and organic matter release and deteriorate overlying waterquality. Furthermore, under high hydrostatic pressure, the polydispersity of DOMρreduced and DOC with low molecular weights were decomposed by microorganisms anddispersed in overlying water. Under different hydrostatic pressure, the microbial communitystructure in the sediments were different. The microbial community diversity under highhydrostatic pressure was much richer than under low hydrostatic pressure.
(4)Water lifting aerator combined with chemical stabilization can inhibit PO_4~(3-)and Fe2+release effectively, and the inhibit efficiencies can reach63.2%and58.6%respectively. Thehigher the PAC concentration was, the better the inhibiting efficiency was, and PAM additioncan strengthen the inhibiting efficiency significantly. The mechanism was that thehydrolyzing products can combine with PO_4~(3-)and form Al-P. The active capping materialcovered by especially selectived biofilm was more effective than capping material orfunctional microbes was singled used. The zeolites in the capping layers can adsrob the NH_4~+and the biofilm covering on the zeolites then decomposed them. Simultaneously the zeoliteswere renewed. Therefore the polluting load of STN and SOC in the sediments can bereduced.
引文
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