受氯代苯酚污染水体沉积物厌氧生物修复的应用基础研究
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摘要
厌氧生物修复技术在修复受氯代有机物污染土壤、沉积物方面具有优势。本文基于培养具有还原脱氯能力的厌氧颗粒污泥，和解析氯代芳烃(五氯酚、对氯苯胺)在沉积物中吸附／解吸特征基础上，较深入地研究了厌氧Slurry工艺修复模拟PCP污染沉积物的性能，并考察了不同操作条件对修复速率的影响。结果表明：
(1) 在EGSB反应器中分别采用含PCP和CA有机废水(反应器1#)、含CA有机废水(反应器2#)两种培养方式，研究厌氧颗粒污泥的培养历程。试验结果表明：①反应器1#连续运行180d，初始80d反应器运行稳定；当PCP和CA分别提升至30mg·L~(-1)和10mg·L~(-1)，微生物明显受到毒性抑制；在进水中仅含PCP情况下，20d后反应器运行恢复正常；180d进水PCP浓度升至60 mg·L~(-1)，去除率稳定在99％。②反应器2#进水为含CA的有机废水，连续运行410天。初始260d，进水CA浓度增至100 mg·L~(-1)，去除率达到60％，微生物未出现明显抑制情况；260～394d期间，缓慢提升CA负荷，然而CA去除率仅提升约5％；394～410d，提高反应器水力停留时间(HRT)至36h，CA去除率迅速升至80％以上。③两个反应器的污泥颗粒化进程大致可分为三个阶段：污泥适应期、颗粒污泥出现期和颗粒污泥成长期。两反应器培养出的颗粒污泥外表呈灰白色和深灰色，其粒径主要分布在1.0～2.0mm和1.5～2.5mm范围，结构较致密，颗粒内部含有丰富的产甲烷丝状菌和短杆菌。
(2) 五氯酚(PCP、有机酸)、对氯苯胺(CA、有机碱)在水体沉积物中的快速吸附、解吸试验表明：①在高浓度条件下，两种污染物的快速吸附过程均符合Parabolic扩散模型，初始浓度-吸附量曲线符合Freudlich方程，说明扩散为吸附过程的限速步骤，而且分配作用在吸附中占主导地位。而相比极性更强CA而言，PCP的分配作用更突出。②调节pH能够促进PCP、CA的解吸。其中碱性条件下(pH：9)，PCP的解吸率达到14.0％；在酸性条件下(pH：4)，CA解吸率达到最大值17.5％，这反映解吸率与污染物的离子化程度呈正相关；添加有机溶剂和表面活性剂明显促进了PCP和CA的解吸，其中乙二醇-丁醚和乙醇分别对PCP和CA的增溶效果最好，解吸率分别达到33.5％和24.9％，同时反映沉积物中PCP／CA的不可逆吸附量约占70％，生物可利用性低。
(3) 考察了分批条件下，厌氧泥浆工艺的修复性能及不同操作条件(投加厌氧脱氯颗粒污泥、共基质、有机溶剂和表面活性剂)对修复速率的影响。试验结果表明：①厌氧脱氯颗粒污泥的强化作用明显。对照处理(无颗粒污泥情况)，31d固液两相PCP降解速率为4.370
mg·kg~(-1)·d~(-1)；投加10g·kg~(-1)和30g·kg~(-1)颗粒污泥时，两相PCP降解速率分别达到7.972mg·kg~(-1)·d~(-1)
受氯代苯酚污染水体沉积物厌氧生物修复的应用基础研究
和8.oo4mgkg一’·d一’，并且随着污泥投加量的增加，沉积物中PcP快速降解时间提前;②共基
质对修复速率的影响比较复杂。在修复初期，共基质的投加促进了PCP的降解;而在中后期，
修复速率反而下降，并且投加的共基质越多，修复速率越慢;③乙醇的投加提高了固、液两
相PCP的降解，同时起到了增溶和共代谢基质的作用;非离子表面活性剂乙二醇一丁醚对 PO户
的解吸效果优于乙醇，但抑制了PCP的进一步降解。
(4)研究了机械搅拌泥浆反应器和曝氮泥浆反应器半连续运行的修复性能，两反应器均
采用两批进料方式，即在第一批修复完成后，替换150gPCP污染沉积物进行补料修复。试验
结果表明:①在一次进料阶段，两类反应器中的固液两相PCP去除率分别达到95 .9~%.5%
和97.3一98.1%，其两相PCP降解曲线均符合一级动力学方程，相关系数为0.9463一0.9886;
②在二次补料阶段，两类反应器的修复性能均明显下降，反映修复过程中，厌氧脱氯菌活性
逐渐降低;③比较分批修复和反应器修复发现，初始8d，机械搅拌反应器和曝氮反应器的修
复速率分别达到27.775mgkg’‘·“和23.728 mgkg一‘·d一‘，修复性能优于分批试验(20.o1P/
mgkg‘’·d‘’);④比较两类反应器性能发现，一次进料阶段的前8d，机械搅拌反应器的两相PcP
降解速率快于氮气搅拌反应器;而在二次补料阶段(14一25d)，曝氮反应器的两相PCP降解
速率(6 .139 mgkg一’·d一’)快于机械搅拌反应器(3 .738 mgkg一’·d-’)。
Anaerobic bioremediation is deemed appropriate for treating PCOCs-contaminated soil and sediment. This paper studied the bioremediation performance of anaerobic slurry processes, which was dependent on development of anaerobic dechloroination granular sludge and realizing PCOCs (PCP and p-CA ) adsorption and desorption in aquatic sediment. Moreover, effects of different treatments on bioremediation were invesgrated. The following results were achieved:
(1) Two manners applied to develop anaerobic granules were studied in EGSB reactors with organic wasterwater contained PCP and CA(reacter 1#), and organic wasterwater contained CA(reacter 2#). The results showed that (1)development of anaerobic granules lasted 180d in reactor 1#, which were stable in initial 80d. But when PCP and CA concentrations of influent increased to 30mgL-1 and 10mg L-1, anaerobic biomass were inhibited by PCP and CA toxicity. In condition of adding sole-PCP, activity of the biomass recovered after 20d. When PCP influent concentration increased to 60 mg L-1, the degradation rates were stable at 99%. (2)development of anaerobic granules lasted 410d in reactor 2#. In initial 260d, CA influent concentration increased to 100 mg L-1, and the degradation rates were stable at 60%. During 260~394d, increasing CA influent concentration slowly resulted in only 5% increasing of the CA degradation rates. When HRT were increased to 36h in 394~410d, the degradation rates rise to 80%. (3)Development
processes of anaerobic granules in reactor 1# and 2# experienced three phases ,adaptive period,appearing period and growing period. Color of the granules developed in two reactors were grey and deep grey. The diameter of the granules ranged from 1.0~2.0mm and 1.5~2.5mm. The struction of these granules were dense. Microscopic examination revealed that the granules contained Methanothrix-like bacteria and Methanobacterium bacteria as prevalent species.
(2) The fast adsorption and desorption of petrachlorophenol and chloroaniline to the aquatic sediment were studied. The result indicated that (1)the adsorption in high concentration of PCP and CA were followed by the Parabolic-diffusion model, the relation between the initial concentration and adsorption obeyed the Freudlich isotherms, and the adsorption of PCP and CA was dominated by partition and diffusion. Contrasting CA with more polarity, partition of PCP was more prominent. (2)Effect of pH , organic solvents (ethanol, acetonitrile) and surfactant (EGME) on desorption of PCP/CA in sediment were also investigated. Adjustment of pH enhanced desorption of PCP/CA. In alkaline condition(pH:9), PCP desorption rates arised to 14%, and 17.5%CA desorbed in acidic condition; Organic solvents and surfactant were required to enhance PCP and CA desorption. EGME and ethanol were best condidates to enhance desorption of PCP and CA, and
33.5%PCP and 24.9%CA were desorbed from sediment. Meanwhile, 70%PCP/CA belonged to irreversible adsorption, which indexed PCP/CA in sediment had a poor bioavailability.
(3) Performance of anaerobic slurry technics was investigated in anaerobic static batch processes. To enhance bioremediation, different treatments(e.g., inoculated with ADGS, co-substrate, ethanol and surfactants addition) were used here. Results showed (1) inoculation of anaerobic dechlorination granule sludge(ADGS) enhanced the bioremediation performance. The total PCP degradation rates in solid-liquid two-phase reached 7.972mgkg-1 d-1 and 8.004 mg kg-1 d-1 when inoculated ADGS content increased to 10g kg-1 and 30g kg-1, compared to 4.370mg kg-1 d-1 in absence of ADGS in 31 days;(2)The effect of co-substance was complicated. In initial period of bioremediation, co-substance stimulated the PCP degradation, while the degradation rates turned to slow in later time. And the higher co-substance concentration was, the slower the degradation rates would be;(3)Enhancement of the desorption and degradation of PCP by ethanol was found, and non-ionic surfactant EGME also stimulated
the desorption,
(1) 在EGSB反应器中分别采用含PCP和CA有机废水(反应器1#)、含CA有机废水(反应器2#)两种培养方式，研究厌氧颗粒污泥的培养历程。试验结果表明：①反应器1#连续运行180d，初始80d反应器运行稳定；当PCP和CA分别提升至30mg·L~(-1)和10mg·L~(-1)，微生物明显受到毒性抑制；在进水中仅含PCP情况下，20d后反应器运行恢复正常；180d进水PCP浓度升至60 mg·L~(-1)，去除率稳定在99％。②反应器2#进水为含CA的有机废水，连续运行410天。初始260d，进水CA浓度增至100 mg·L~(-1)，去除率达到60％，微生物未出现明显抑制情况；260～394d期间，缓慢提升CA负荷，然而CA去除率仅提升约5％；394～410d，提高反应器水力停留时间(HRT)至36h，CA去除率迅速升至80％以上。③两个反应器的污泥颗粒化进程大致可分为三个阶段：污泥适应期、颗粒污泥出现期和颗粒污泥成长期。两反应器培养出的颗粒污泥外表呈灰白色和深灰色，其粒径主要分布在1.0～2.0mm和1.5～2.5mm范围，结构较致密，颗粒内部含有丰富的产甲烷丝状菌和短杆菌。
(2) 五氯酚(PCP、有机酸)、对氯苯胺(CA、有机碱)在水体沉积物中的快速吸附、解吸试验表明：①在高浓度条件下，两种污染物的快速吸附过程均符合Parabolic扩散模型，初始浓度-吸附量曲线符合Freudlich方程，说明扩散为吸附过程的限速步骤，而且分配作用在吸附中占主导地位。而相比极性更强CA而言，PCP的分配作用更突出。②调节pH能够促进PCP、CA的解吸。其中碱性条件下(pH：9)，PCP的解吸率达到14.0％；在酸性条件下(pH：4)，CA解吸率达到最大值17.5％，这反映解吸率与污染物的离子化程度呈正相关；添加有机溶剂和表面活性剂明显促进了PCP和CA的解吸，其中乙二醇-丁醚和乙醇分别对PCP和CA的增溶效果最好，解吸率分别达到33.5％和24.9％，同时反映沉积物中PCP／CA的不可逆吸附量约占70％，生物可利用性低。
(3) 考察了分批条件下，厌氧泥浆工艺的修复性能及不同操作条件(投加厌氧脱氯颗粒污泥、共基质、有机溶剂和表面活性剂)对修复速率的影响。试验结果表明：①厌氧脱氯颗粒污泥的强化作用明显。对照处理(无颗粒污泥情况)，31d固液两相PCP降解速率为4.370
mg·kg~(-1)·d~(-1)；投加10g·kg~(-1)和30g·kg~(-1)颗粒污泥时，两相PCP降解速率分别达到7.972mg·kg~(-1)·d~(-1)
受氯代苯酚污染水体沉积物厌氧生物修复的应用基础研究
和8.oo4mgkg一’·d一’，并且随着污泥投加量的增加，沉积物中PcP快速降解时间提前;②共基
质对修复速率的影响比较复杂。在修复初期，共基质的投加促进了PCP的降解;而在中后期，
修复速率反而下降，并且投加的共基质越多，修复速率越慢;③乙醇的投加提高了固、液两
相PCP的降解，同时起到了增溶和共代谢基质的作用;非离子表面活性剂乙二醇一丁醚对 PO户
的解吸效果优于乙醇，但抑制了PCP的进一步降解。
(4)研究了机械搅拌泥浆反应器和曝氮泥浆反应器半连续运行的修复性能，两反应器均
采用两批进料方式，即在第一批修复完成后，替换150gPCP污染沉积物进行补料修复。试验
结果表明:①在一次进料阶段，两类反应器中的固液两相PCP去除率分别达到95 .9~%.5%
和97.3一98.1%，其两相PCP降解曲线均符合一级动力学方程，相关系数为0.9463一0.9886;
②在二次补料阶段，两类反应器的修复性能均明显下降，反映修复过程中，厌氧脱氯菌活性
逐渐降低;③比较分批修复和反应器修复发现，初始8d，机械搅拌反应器和曝氮反应器的修
复速率分别达到27.775mgkg’‘·“和23.728 mgkg一‘·d一‘，修复性能优于分批试验(20.o1P/
mgkg‘’·d‘’);④比较两类反应器性能发现，一次进料阶段的前8d，机械搅拌反应器的两相PcP
降解速率快于氮气搅拌反应器;而在二次补料阶段(14一25d)，曝氮反应器的两相PCP降解
速率(6 .139 mgkg一’·d一’)快于机械搅拌反应器(3 .738 mgkg一’·d-’)。
Anaerobic bioremediation is deemed appropriate for treating PCOCs-contaminated soil and sediment. This paper studied the bioremediation performance of anaerobic slurry processes, which was dependent on development of anaerobic dechloroination granular sludge and realizing PCOCs (PCP and p-CA ) adsorption and desorption in aquatic sediment. Moreover, effects of different treatments on bioremediation were invesgrated. The following results were achieved:
(1) Two manners applied to develop anaerobic granules were studied in EGSB reactors with organic wasterwater contained PCP and CA(reacter 1#), and organic wasterwater contained CA(reacter 2#). The results showed that (1)development of anaerobic granules lasted 180d in reactor 1#, which were stable in initial 80d. But when PCP and CA concentrations of influent increased to 30mgL-1 and 10mg L-1, anaerobic biomass were inhibited by PCP and CA toxicity. In condition of adding sole-PCP, activity of the biomass recovered after 20d. When PCP influent concentration increased to 60 mg L-1, the degradation rates were stable at 99%. (2)development of anaerobic granules lasted 410d in reactor 2#. In initial 260d, CA influent concentration increased to 100 mg L-1, and the degradation rates were stable at 60%. During 260~394d, increasing CA influent concentration slowly resulted in only 5% increasing of the CA degradation rates. When HRT were increased to 36h in 394~410d, the degradation rates rise to 80%. (3)Development
processes of anaerobic granules in reactor 1# and 2# experienced three phases ,adaptive period,appearing period and growing period. Color of the granules developed in two reactors were grey and deep grey. The diameter of the granules ranged from 1.0~2.0mm and 1.5~2.5mm. The struction of these granules were dense. Microscopic examination revealed that the granules contained Methanothrix-like bacteria and Methanobacterium bacteria as prevalent species.
(2) The fast adsorption and desorption of petrachlorophenol and chloroaniline to the aquatic sediment were studied. The result indicated that (1)the adsorption in high concentration of PCP and CA were followed by the Parabolic-diffusion model, the relation between the initial concentration and adsorption obeyed the Freudlich isotherms, and the adsorption of PCP and CA was dominated by partition and diffusion. Contrasting CA with more polarity, partition of PCP was more prominent. (2)Effect of pH , organic solvents (ethanol, acetonitrile) and surfactant (EGME) on desorption of PCP/CA in sediment were also investigated. Adjustment of pH enhanced desorption of PCP/CA. In alkaline condition(pH:9), PCP desorption rates arised to 14%, and 17.5%CA desorbed in acidic condition; Organic solvents and surfactant were required to enhance PCP and CA desorption. EGME and ethanol were best condidates to enhance desorption of PCP and CA, and
33.5%PCP and 24.9%CA were desorbed from sediment. Meanwhile, 70%PCP/CA belonged to irreversible adsorption, which indexed PCP/CA in sediment had a poor bioavailability.
(3) Performance of anaerobic slurry technics was investigated in anaerobic static batch processes. To enhance bioremediation, different treatments(e.g., inoculated with ADGS, co-substrate, ethanol and surfactants addition) were used here. Results showed (1) inoculation of anaerobic dechlorination granule sludge(ADGS) enhanced the bioremediation performance. The total PCP degradation rates in solid-liquid two-phase reached 7.972mgkg-1 d-1 and 8.004 mg kg-1 d-1 when inoculated ADGS content increased to 10g kg-1 and 30g kg-1, compared to 4.370mg kg-1 d-1 in absence of ADGS in 31 days;(2)The effect of co-substance was complicated. In initial period of bioremediation, co-substance stimulated the PCP degradation, while the degradation rates turned to slow in later time. And the higher co-substance concentration was, the slower the degradation rates would be;(3)Enhancement of the desorption and degradation of PCP by ethanol was found, and non-ionic surfactant EGME also stimulated
the desorption,
引文
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