生物滴滤器去除VOC的性能及其强化研究
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摘要
挥发性有机物(volatile organic compounds, VOCs)排放引起的环境污染和对人体健康的危害已引起了人们的普遍关注。VOCs的各种控制技术中,生物过滤法因其技术可靠、成本低廉和环境友好的特点而得到广泛研究和应用。然而,采用生物滴滤器(biotrickling filter, BTF)控制VOCs存在着长期运行时因填料内生物膜的过度蓄积导致性能下降,以及对疏水性VOCs难以进行有效处理的问题。同时,填料对BTF性能也有至关重要的影响。
本研究在实验室里采用两套完全相同的BTF装置(BTF1和BTF2),分别以甲苯和正己烷为模型VOCs,以网状聚氨酯海绵为填料,以城市污水处理厂的活性污泥为接种污泥,分别考察和评价了不同有机负荷、气体空床停留时间(empty bed contact times, EBCTs)、氮源及表面活性剂对其性能的影响,并对长期运行后填料上的生物膜进行了初步分析。本研究中采用气相色谱法监测VOCs浓度,并在每阶段实验中均设置了参考条件以验证的实验的可重复性和可靠性。
以甲苯为模型VOC时,BTF1和BTF2分别以整体柱状和小立方块状聚氨酯海绵为填料,在启动阶段两套BTFs对甲苯的去除效率均随停留时间而升高,BTF1在第19天达到99%以上,而BTF2却需要27天。当甲苯负荷为16g/m3h保持不变时,气体EBCT从30s降至5s时,两套BTFs对甲苯的去除效率分别从98.8%降至64.3%和98.4%降至74.1%。当气体EBCT为30s保持不变时,甲苯负荷从35增到加140g/m3·h时,两套BTFs的去除效率分别从99.1%降至77.4%和99.0%降至81.5%。在其他条件相同时,BTF2在更短的EBCT和或者更高的甲苯负荷条件下均表现出比BTF1更好的性能,而且在整个运行过程中压降更低。两BTFs内过量生物膜被清洗和废弃后,其高性能能在3-7内恢复。
在进口甲苯浓度保持不变时,以NH4CI为唯一氮源,气体EBCT从30s降至15s和7.5s时,BTF1对甲苯的去除效率从98.0%分别降到了57.9%和51.6%。保持甲苯负荷不变,以NaNO3为唯一氮源,气体EBCT从30s降至15、10和7.5s时,BTF1的去除效率从99.0%分别降到了79.8%、70.8%和61.2%。当气体EBCT为30s时,无论以NH4Cl还是以NaNO3为唯一氮源,BTF对甲苯的去除效率都随着进口甲苯负荷的增加而降低。当甲苯负荷低于70g/m3·h,采用NH4Cl为唯一氮源时,BTF具有更好的性能,但是不适合高负荷条件下的氮源。相反,在甲苯负荷高于140g/m3·h时,采取NaNO3为唯一氮源时,BTF2具有更好的性能。长期运行或进行填料清洗后,以NaNO3为唯一氮源的BTF2的性能都能在相当短的时间内恢复到高性能状态,而以NH4Cl为唯一氮源时则不能恢复。
以正己烷为模型VOC时,当气体EBCT为30s保持不变时,当进口有机负荷为15、30和60g/m3·h时,BTF相应的去除效率和去除容量分别为92.9%、86.7%、63.8%和14.3、26.1、39.3g/m3·h。当正己烷浓度为260mg/m3保持不变时,当气体EBCT为别为30s、15s和7.5s时,相应的去除效率和去除容量分别为87.0%、46.4%、31.7%和28.0、28.8、41.0g/m3·h。而且在冲击负荷下,网状聚氨酯填料中形成的生物膜表现了很的抗冲击能力,维持BTF稳定性能。
在营养液中引入Triton X-100,考察了BTF对正己烷在高负荷时的强化去除性能。在进口有机负荷为15g/m3·h时,Triton X-100的浓度为1.0和0.2mL/L,BTF的去除效率分别为40.0%和53.1%；当有机负荷为30g/m3·h时,Triton X-100的浓度为0.2和0.1mL/L,相应的去除效率分别为58.8%和81.7%。当负荷为60g/m3.h和Triton X-100浓度为0.1mL/L,BTF的去除效率达到了83.7%,相比于未引入表面活性剂时提高了20%；当营养液中取消Triton X-100,BTF的去除效率下降并稳定在72.8%。特别重要的是在整个周期(126天)运行中,引入的TritonX-100能很好的控制填料中生物膜的过度蓄积,是一种新的生物膜过度蓄积控制策略。
本论文针对BTF内填料优化、生物膜过度蓄积及控制策略、疏水性有机物处理性能及其强化等重要问题进行了研究,有助于拓宽BTF处理VOCs的适应范围和提供一种新的填料内生物膜过度蓄积的控制策略,有利于深入理解气相生物过滤过程机理,进一步为BTF和聚氨酯海绵填料的实际应用提供理论依据。
Emissions of volatile organic compounds (VOCs) resulted in environment pollution and human health threat, which have paid close attention. Among various technologies for controlling VOCs, biofiltration is bocoming an established technology because of its reliability, cost-effectiveness and environmental friendliness. However, biotrickling filters (BTFs) for VOCs treatment exist some disadvantages, such as performance decrease caused by excess biomass in media over a long period operation and BTF treat difficultly for hydrophobic VOCs. In addition, media affect BTF performance to a large extent.
Two identical bench-scale biotrickling filters (BTFs) were employed and designated as BTF1and BTF2in this research. Toluene and hexane were chosen as model VOCs. Polyurethane sponge was used as packing media in BTF, and the activated sludge from a secondary sedimentation tank was used for seeding the BTFs. Furthermore, BTF performance was investigated and evaluated at different operating conditions such as which different organic loading rates, gas empty bed contact times (EBCTs), nitrogen resource and surfactant over a long period of continuous operation. Biofilm within the sponge media of BTF was also primarily analysis after running over a long period. In this research, gas choromatograph was used for determining the concentration of VOCs. In particular, in order to check the reproducibility and reliability of BTFs in each operation stage, a set of reference condition was used in this research.
When toluene was used as model VOC, BTF1and BTF2were packed with structured and cubic synthetic polyurethane sponges, respectively. BTF1and BTF2could start up successfully and exceeded99%in removal efficiency using19and27d, respectively. At a constant toluene loading rate of16g/(m3·h), toluene removal efficiencies decreased from98.8%to64.3%for BTF1and from98.4%to74.1%for BTF2as gas EBCT decreased from30to5s. When the toluene load increased from35to140g/(m3·h) at a gas EBCT of30s, the removal efficiencies decreased from99.1%to77.4%for BTF1and from99.0%to81.5%for BTF2. Moreover, BTF2displayed higher removal efficiency even under shorter EBCT or higher loading rate than BTF1when other operation conditions were similar, while showed lower pressure drop than BTF1during the whole period of operation. The high performance could recovery in3～7d after excessive biomass was removed from the BTFs by washing.
When NH4Cl was used as sole nitrogen resource at a constant toluene concentration, toluene removal efficiencies decreased from98.0%to57.9%and51.6%for BTF1when gas EBCT decreased from30s to15s and5s, respectively. However, NaNO3was used as sole nitrogen resource when BTF runned at a constant toluene loading rate. When gas EBCT was setted at30,15,10and7.5s, the corresponding removal efficiency reached99.0%,79.8%,70.8%and61.2%. Either NH4Cl or NaNO3was used as sole nitrogen resource at a gas EBCT of30s, the removal efficiencie for toluene decreased with increase in inlet loading rate. BTF presented a better performance when toluene load was less than70g/(m3·h) and NH4Cl used as the sole nitrogen source. In contrast, BTF2used NaNO3as the sole nitrogen source reached higher removal efficiency when toluene load was more than140g/(m3·h). Afer long period running or media washing, BTF could resume to previous high performance in a relatively short period when NaNO3was, but the BTF used NH4Cl as the sole nitrogen source could not.
When hexane was used as model VOC, when the hexane load increased from15to30,60g/(m3·h) at a gas EBCT of30s, the corresponding removal efficiencies and elimination capacities were92.9%,86.7%,63.8%and14.3、26.1、39.3g/(m3·h), respectively. At a constant hexane concentration of260mg/m3, removal efficiencies and elimination capacities were87.0%,46.4%,31.7%and28.028.8、41.0g/(m·h) when gas EBCT decreased from30to15s and7.5s, respectively. Moreover, biofilm formed in reticulated polyurethane sponges could resist shorck loading, and BTF could also maintain stable performance after long period operation.
The effect of surfactant on BTF performance for hexane removal was also investigated in this research. When the concentration of was1.0and0.2mL/L at influent organic loading rate of15g/(m3·h), the removal efficiencies reached40.0%and53.1%, respectively. When the hexane load increased to30g/(m3·h) at Triton X-100concentration of0.2and0.1mL/L, the corresponding removal efficiencies were58.8%and81.7%. At a constant Triton X-100concentration of0.1mL/L, the removal efficiency increased to83.7%under the hexane load of60g/(m3·h), and it was higer than the value in chapter5at the same condition. Subsequently, the removal efficiency decreased and stabilized at72.8%after the surfactant removed from nutrition solution. Particularly, during the whole duration of126days, Triton X-100introduced could control efficiently excess biofilm growth, which will be a novel control strategy for biofilm control.
This dissertation researched on the optimization of packing materials, excessive accumulation and control strategy for biofilm, the removal performance of hydrophobic VOCs over a long period. These reseach results would contribute to expand the adaptation range of VOCs removl by BTF, and provide a novel control strategy for excessive accumulation of biofilm with media. At the same time, it is helpful for understanding the mechanisms of gas biofiltration process.This study provides theriotical basis on the practical application of BTF and polyurethane sponges.
本研究在实验室里采用两套完全相同的BTF装置(BTF1和BTF2),分别以甲苯和正己烷为模型VOCs,以网状聚氨酯海绵为填料,以城市污水处理厂的活性污泥为接种污泥,分别考察和评价了不同有机负荷、气体空床停留时间(empty bed contact times, EBCTs)、氮源及表面活性剂对其性能的影响,并对长期运行后填料上的生物膜进行了初步分析。本研究中采用气相色谱法监测VOCs浓度,并在每阶段实验中均设置了参考条件以验证的实验的可重复性和可靠性。
以甲苯为模型VOC时,BTF1和BTF2分别以整体柱状和小立方块状聚氨酯海绵为填料,在启动阶段两套BTFs对甲苯的去除效率均随停留时间而升高,BTF1在第19天达到99%以上,而BTF2却需要27天。当甲苯负荷为16g/m3h保持不变时,气体EBCT从30s降至5s时,两套BTFs对甲苯的去除效率分别从98.8%降至64.3%和98.4%降至74.1%。当气体EBCT为30s保持不变时,甲苯负荷从35增到加140g/m3·h时,两套BTFs的去除效率分别从99.1%降至77.4%和99.0%降至81.5%。在其他条件相同时,BTF2在更短的EBCT和或者更高的甲苯负荷条件下均表现出比BTF1更好的性能,而且在整个运行过程中压降更低。两BTFs内过量生物膜被清洗和废弃后,其高性能能在3-7内恢复。
在进口甲苯浓度保持不变时,以NH4CI为唯一氮源,气体EBCT从30s降至15s和7.5s时,BTF1对甲苯的去除效率从98.0%分别降到了57.9%和51.6%。保持甲苯负荷不变,以NaNO3为唯一氮源,气体EBCT从30s降至15、10和7.5s时,BTF1的去除效率从99.0%分别降到了79.8%、70.8%和61.2%。当气体EBCT为30s时,无论以NH4Cl还是以NaNO3为唯一氮源,BTF对甲苯的去除效率都随着进口甲苯负荷的增加而降低。当甲苯负荷低于70g/m3·h,采用NH4Cl为唯一氮源时,BTF具有更好的性能,但是不适合高负荷条件下的氮源。相反,在甲苯负荷高于140g/m3·h时,采取NaNO3为唯一氮源时,BTF2具有更好的性能。长期运行或进行填料清洗后,以NaNO3为唯一氮源的BTF2的性能都能在相当短的时间内恢复到高性能状态,而以NH4Cl为唯一氮源时则不能恢复。
以正己烷为模型VOC时,当气体EBCT为30s保持不变时,当进口有机负荷为15、30和60g/m3·h时,BTF相应的去除效率和去除容量分别为92.9%、86.7%、63.8%和14.3、26.1、39.3g/m3·h。当正己烷浓度为260mg/m3保持不变时,当气体EBCT为别为30s、15s和7.5s时,相应的去除效率和去除容量分别为87.0%、46.4%、31.7%和28.0、28.8、41.0g/m3·h。而且在冲击负荷下,网状聚氨酯填料中形成的生物膜表现了很的抗冲击能力,维持BTF稳定性能。
在营养液中引入Triton X-100,考察了BTF对正己烷在高负荷时的强化去除性能。在进口有机负荷为15g/m3·h时,Triton X-100的浓度为1.0和0.2mL/L,BTF的去除效率分别为40.0%和53.1%；当有机负荷为30g/m3·h时,Triton X-100的浓度为0.2和0.1mL/L,相应的去除效率分别为58.8%和81.7%。当负荷为60g/m3.h和Triton X-100浓度为0.1mL/L,BTF的去除效率达到了83.7%,相比于未引入表面活性剂时提高了20%；当营养液中取消Triton X-100,BTF的去除效率下降并稳定在72.8%。特别重要的是在整个周期(126天)运行中,引入的TritonX-100能很好的控制填料中生物膜的过度蓄积,是一种新的生物膜过度蓄积控制策略。
本论文针对BTF内填料优化、生物膜过度蓄积及控制策略、疏水性有机物处理性能及其强化等重要问题进行了研究,有助于拓宽BTF处理VOCs的适应范围和提供一种新的填料内生物膜过度蓄积的控制策略,有利于深入理解气相生物过滤过程机理,进一步为BTF和聚氨酯海绵填料的实际应用提供理论依据。
Emissions of volatile organic compounds (VOCs) resulted in environment pollution and human health threat, which have paid close attention. Among various technologies for controlling VOCs, biofiltration is bocoming an established technology because of its reliability, cost-effectiveness and environmental friendliness. However, biotrickling filters (BTFs) for VOCs treatment exist some disadvantages, such as performance decrease caused by excess biomass in media over a long period operation and BTF treat difficultly for hydrophobic VOCs. In addition, media affect BTF performance to a large extent.
Two identical bench-scale biotrickling filters (BTFs) were employed and designated as BTF1and BTF2in this research. Toluene and hexane were chosen as model VOCs. Polyurethane sponge was used as packing media in BTF, and the activated sludge from a secondary sedimentation tank was used for seeding the BTFs. Furthermore, BTF performance was investigated and evaluated at different operating conditions such as which different organic loading rates, gas empty bed contact times (EBCTs), nitrogen resource and surfactant over a long period of continuous operation. Biofilm within the sponge media of BTF was also primarily analysis after running over a long period. In this research, gas choromatograph was used for determining the concentration of VOCs. In particular, in order to check the reproducibility and reliability of BTFs in each operation stage, a set of reference condition was used in this research.
When toluene was used as model VOC, BTF1and BTF2were packed with structured and cubic synthetic polyurethane sponges, respectively. BTF1and BTF2could start up successfully and exceeded99%in removal efficiency using19and27d, respectively. At a constant toluene loading rate of16g/(m3·h), toluene removal efficiencies decreased from98.8%to64.3%for BTF1and from98.4%to74.1%for BTF2as gas EBCT decreased from30to5s. When the toluene load increased from35to140g/(m3·h) at a gas EBCT of30s, the removal efficiencies decreased from99.1%to77.4%for BTF1and from99.0%to81.5%for BTF2. Moreover, BTF2displayed higher removal efficiency even under shorter EBCT or higher loading rate than BTF1when other operation conditions were similar, while showed lower pressure drop than BTF1during the whole period of operation. The high performance could recovery in3～7d after excessive biomass was removed from the BTFs by washing.
When NH4Cl was used as sole nitrogen resource at a constant toluene concentration, toluene removal efficiencies decreased from98.0%to57.9%and51.6%for BTF1when gas EBCT decreased from30s to15s and5s, respectively. However, NaNO3was used as sole nitrogen resource when BTF runned at a constant toluene loading rate. When gas EBCT was setted at30,15,10and7.5s, the corresponding removal efficiency reached99.0%,79.8%,70.8%and61.2%. Either NH4Cl or NaNO3was used as sole nitrogen resource at a gas EBCT of30s, the removal efficiencie for toluene decreased with increase in inlet loading rate. BTF presented a better performance when toluene load was less than70g/(m3·h) and NH4Cl used as the sole nitrogen source. In contrast, BTF2used NaNO3as the sole nitrogen source reached higher removal efficiency when toluene load was more than140g/(m3·h). Afer long period running or media washing, BTF could resume to previous high performance in a relatively short period when NaNO3was, but the BTF used NH4Cl as the sole nitrogen source could not.
When hexane was used as model VOC, when the hexane load increased from15to30,60g/(m3·h) at a gas EBCT of30s, the corresponding removal efficiencies and elimination capacities were92.9%,86.7%,63.8%and14.3、26.1、39.3g/(m3·h), respectively. At a constant hexane concentration of260mg/m3, removal efficiencies and elimination capacities were87.0%,46.4%,31.7%and28.028.8、41.0g/(m·h) when gas EBCT decreased from30to15s and7.5s, respectively. Moreover, biofilm formed in reticulated polyurethane sponges could resist shorck loading, and BTF could also maintain stable performance after long period operation.
The effect of surfactant on BTF performance for hexane removal was also investigated in this research. When the concentration of was1.0and0.2mL/L at influent organic loading rate of15g/(m3·h), the removal efficiencies reached40.0%and53.1%, respectively. When the hexane load increased to30g/(m3·h) at Triton X-100concentration of0.2and0.1mL/L, the corresponding removal efficiencies were58.8%and81.7%. At a constant Triton X-100concentration of0.1mL/L, the removal efficiency increased to83.7%under the hexane load of60g/(m3·h), and it was higer than the value in chapter5at the same condition. Subsequently, the removal efficiency decreased and stabilized at72.8%after the surfactant removed from nutrition solution. Particularly, during the whole duration of126days, Triton X-100introduced could control efficiently excess biofilm growth, which will be a novel control strategy for biofilm control.
This dissertation researched on the optimization of packing materials, excessive accumulation and control strategy for biofilm, the removal performance of hydrophobic VOCs over a long period. These reseach results would contribute to expand the adaptation range of VOCs removl by BTF, and provide a novel control strategy for excessive accumulation of biofilm with media. At the same time, it is helpful for understanding the mechanisms of gas biofiltration process.This study provides theriotical basis on the practical application of BTF and polyurethane sponges.
引文
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