应对水源突发氯苯污染的吹脱—吸附技术效能及机制研究
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摘要
随着我国社会经济的快速发展、工业化进程的高速推进和人民生活水平的日益提高，一方面水资源开发利用程度不断加大，水体污染尤其是有机物污染日趋严重且突发污染事件频发；另一方面，我国大多数供水企业的水处理工艺相对落后，难以有效应对突发性水污染事件。因此，研发适合我国大多数水厂现状的、高效经济的应急处理技术工艺具有重要的现实意义。
本文针对水源水可能突发挥发性有机物（VOCs）污染的问题，以氯苯为目标污染物，建立以曝气吹脱和粉末炭（PAC）吸附为核心的应急处理技术工艺，以氯苯作为目标物，研究曝气吹脱和PAC吸附两种技术对水中氯苯的去除效能及其影响因素，并基于两者各自特点和优势，实现两者技术耦合，结合后续常规处理工艺达到高效经济地去除水中VOCs的目的。同时，还开展了活性炭纤维（ACF）吸附吹脱气体中氯苯和水中活性炭表面氯苯脱附规律研究，旨在开发和采取相应技术措施以避免水处理过程中VOCs二次污染。
曝气吹脱对氯苯的去除效率主要受气水比和水温的影响，吹脱效率与气水比和水温具有正相关性，氯苯初始浓度和原水浊度对曝气吹脱去除率影响不大，共存其他VOCs可提高氯苯吹脱去除效率，表现出协同去除效应。曝气吹脱过程中，气水总传质系数与氯苯初始浓度呈显著线性关系，与单位面积曝气量和水温呈非线性正相关性。当采用50-100的气水比时，氯苯吹脱去除率可达83.73%-91.14%，运行成本约0.033-0.0654元/吨水，处理较为经济高效。当气水比高于100时，曝气吹脱处理变得不经济。
PAC可快速吸附水中氯苯，5min吸附量即可达到平衡吸附量的80%以上，30min吸附量可达98%以上。PAC对氯苯的吸附效能主要受PAC比表面积和搅拌混合程度影响，受水温、pH值、离子强度等因素影响不大。基于吸附速率和吸附平衡模型参数建立了基于氯苯初始浓度、PAC投量和吸附时间的吸附经验模型，可以较好地预测氯苯不同污染水平下所需的PAC投量。为验证和校核模型预测值，分别开展了小试和中试研究，最终给出了氯苯不同污染水平下所需的PAC投量。另外，中试结果表明PAC吸附阶段是水中氯苯去除的主要阶段，去除率为62.5%-98.9%；常规工艺可去除水中吸附了氯苯的PAC和其他颗粒，进一步去除水中氯苯；作为水质安全保障的最后一道关口，GAC滤柱可以去除煤砂滤池出水中微量氯苯。
曝气吹脱与PAC吸附耦合技术，可与现有水处理工艺有机结合，充分发挥吹脱和吸附两种技术各自优势，使两种技术分担了不同负荷的污染物去除任务，使得对污染物的可控超标倍数有明显增长，提高了应对水源水发生氯苯污染的处理能力，且能够到取得高效、经济的处理结果。以曝气吹脱-PAC吸附耦合技术为氯苯去除的核心技术、以常规处理单元为水处理工艺主体、以GAC滤池为末端安全关口的应急处理技术工艺，可以作为我国大多数水厂应对水源水突发氯苯污染的应急处理技术工艺。
竞争性吸附和浓差驱动作用会造成污染物在活性炭上脱附。在直接强竞争吸附物（乙苯）、堵塞孔道型大分子吸附物（PSS）的竞争吸附作用以及浓差驱动作用下，吸附在PAC上的氯苯会出现不同程度地脱附。在乙苯强竞争吸附作用下，氯苯在PAC上快速脱附，20-40min可达到脱附平衡，脱附量可达3%-63%，氯苯脱附量和脱附速率与竞争性吸附物（乙苯）浓度具有正相关性。PSS对氯苯在PAC上的吸附量和脱附量基本无影响，但吸附在PAC大孔中PSS会产生堵塞作用，降低氯苯在PAC上的脱附速率。浓差驱动会导致氯苯在PAC上脱附显著，且脱附量随着浓差梯度增大而增加。在水源水突发氯苯污染消除后，在GAC滤池后续运行中，竞争性吸附造成氯苯脱附的风险较小，而浓差驱动造成氯苯脱附风险很大，因此应在突发污染消除后，建议立即更新GAC滤池的活性炭。
吹脱气体中的氯苯可用ACF吸附去除，其吸附去除效能与ACF的BET比表面积、微孔容积、表面化学性质，以及相对湿度（RH）和温度等因素有关。BET比表面积和微孔容积越大，ACF对氯苯吸附速率和吸附量越大。RH对氯苯在ACF上吸附具有抑制作用，且随着RH增大而增强，RH高于50%时，ACF对氯苯的吸附量下降明显。水分子竞争性吸附以及其在微孔中的毛细凝结是其抑制氯苯吸附的主要原因。通过浸渍尿素或硫酸铜再在氮气流下高温处理，进行ACF表面化学改性，一方面可降低表面含氧量，减少酸性官能团含量，提高表面憎水性，减轻RH对氯苯吸附的抑制作用；另一方面，改性后ACF表面生成了含氮的碱性官能团，可提高ACF与氯苯之间的π-π色散力，提高ACF对氯苯的吸附速率和吸附量；另外，经硫酸铜浸渍再高温改性后，ACF表面会负载CuO微晶，其对VOCs具有更强的吸附力。温度对ACF吸附氯苯的效能影响显著，随着温度的升高，氯苯吸附量明显降低。
As the fast development of national economy, industrialization process and theescalation of people’s living standard, the water quality of drinking water sourcedecreased caused by the high development and adequate utilization of waterresources, the serious water pollution caused by organic material, and the frequentlysudden water pollution accidents. However, the relatively undeveloped watertreatment process had weak ability to cope with sudden pollution in raw water formost waterworks in china. Consequently, the study of emergency water treatmenttechnology and process had an important current significance.
Emergency water treatment technology based on air stripping and PACadsorption was established to resolve the problem of volatile organic compound(VOC) sudden pollution in raw water. Chlorobenzene (CB) was used as the targetvolatile organic compound (VOC) in this paper. Experiments were conducted tostudy efficiency and influencing factors of VOCs removal by PAC adsorption andair stripping. Based on their respective advantages and characteristics, the twotechnologies of PAC adsorption and air stripping was coupled and then combinedwith the following conventional water treatment process in order to improve VOCsremoval efficiency and decrease the operation cost. Additionally, experiments wasconducted to study the adsorption of VOCs onto ACF from the off-gas emitted byair stripping and the desorption of VOCs from PAC in water, in order to developsome technology to avoid secondary contamination.
Air-water ratio and temperature were the main factors influencing the removalof CB by air stripping, and the removal of CB was positively correlated with air-water ratio and temperature. However, the removal of CB by air stripping had littlerelationship with CB initial concentration and turbidity. Synergistic removal effectswas found between different VOCs while air stripping.
A static mass transfer kinetic model was fitted to the experimental data toobtain the overall mass transfer coefficient. The result showed that the overall masstransfer coefficient had linear increasing relationship with CB initial concentration,and had nonlinear increasing relationship with air flowrate and temperature. Adynamic air stripping model was used to study the removal efficiency at differentair-water ratio. It was found that air stripping was efficient and economical at theair-water ratio of500-100with the removal rate of83.73%-91.14%and theoperation cost of0.033-0.065Yuan/t. However, the operation cost would increasewhen the air-water ratio was more than100.
PAC can adsorb CB from water rapidly with80%and98%of the equilibrium adsorption capacity at5min and30min, respectively. PAC surface area and mixingintensity had an important influence on the adsorption efficiency by PAC, whilefactors such as temperature, pH value and ionic strength had little effect on CBremoval by PAC adsorption. Adsorption kinetics and equilibrium could besuccessfully simulated by the pseudo-second kinetic model and Freundlich model,respectively. Based on the parameters obtained from the models above, a theoreticalformula of PAC dose with initial CB concentration and adsorption time wasestablished and verified by experimental results. And the recommended PAC dosewas given based on the result above. It is concluded from pilot test that the mixtureof PAC and water and the coagulation clarification were the key process to removeCB, and the removal could reach62.5%-98.9%; the conventional treatment processcould intercept the micro flocs and particles carrying CB in water, resulting in thefurther reduce of CB; as a safety guarantee, granular activated carbon filter columnwas the last process to remove CB.
The combining technology of PAC adsorption and air stripping could integrateinto the conventional water treatment process, and take the advantage of the twotechnology. PAC adsorption and air stripping shared different CB removal load,which could improve the ability of CB removal, and obtain an efficient andeconomical outcome. Emergency treatment process, with the combining technologyof air stripping and PAC adsorption being the core, the conventional water treatmentprocess being the main part, and GAC filter being the last safety guarantee, could beused to cope with VOCs sudden pollution in source water for most waterworks inour country.
Competitive adsorption and concentration gradient drive would causecontaminant desorption from activated carbon. CB desorption happened withvarying degrees under the influence of competitive adsorption by stronglycompeting background compounds (CB) and pore-blocking background compounds(PSS), and the driving force by concentration gradient. CB desorbed rapidly fromactivated carbon, and reached equilibrium within20-40min. The percent of CBdesorption was3%-63%at equilibrium. It was found that the rate and amount of CBdesorption was positively correlated with the concentration of competitioncompounds (ethylbenzene). PSS had slightly effect on CB adsorption or desorptiononto activated carbon, while it slowed the rate of CB desorption due to the pore-blocking effect of PSS in macropore of activated carbon. The driving force byconcentration gradient influenced CB desorption notably. CB desorption amountincreased with increasing concentration gradient. The percent of CB desorption was32%and40%when the solution of CB and activated carbon equilibrium system wasdiluted to5and10times, respectively. The risk of CB desorption from activatedcarbon was assumed low when competitive adsorption existed, but very high if concentration gradient drive effect became notable, which always existed in theGAC filter having used for a sudden pollution. Therefore, these used activatedcarbon in GAC filter should be replaced if the filter would run after the suddenwater pollution.
CB in the off-gas emitted by air stripping could be removed efficiently byactivated carbon fiber (ACF) adsorption, whose removal efficiency was concernedwith BET surface area, micropore volumn and surface chemical character of ACF,relative humidity (RH) and temperature. The larger the BET surface area andmicropore volumn, the greater the adsorption rate and capacity. RH had aninhibitory effect on CB adsorption onto ACF. Moreover, with increasing RH, theinhibitory effect becomes more significant. When RH was higher than50%, CBadsorption amount reduce remarkably by more than13%. The main factorsrestraining CB adsorption onto ACF was the competitive adsorption and capillarycondensation of water molecular in micropore. Surface modification of ACF wasconducted by being impregnated with urea or copper sulphate solution and thenheated at800℃in the environment of nitrogen. On the one hand, it was proved thatsurface modification could decrease oxygen content, and reduce acid functionalgroups, and improve surface hydrophobicity of ACF surface, and then lower wateradsorption amount. As a result, the inhibitory effect of RH on CB adsorption wasrelieved. On the other hand, the generation of basic functional groups could increasethe adsorption rate and amount of CB adsorption onto ACF due to the increase in π-π dispersive interactions between the π-electron system of the carbon graphenelayers and the π-electrons of the ring of CB molecular. Additionally, the load ofcopper oxide microcrystal enhanced VOCs adsorption because of the highadsorption bond between copper oxide microcrystal and CB molecular. Temperatureis an important factor to affect CB adsorption onto ACF. Experimental resultsshowed that CB adsorption amount decreased with increasing temperature.
本文针对水源水可能突发挥发性有机物（VOCs）污染的问题，以氯苯为目标污染物，建立以曝气吹脱和粉末炭（PAC）吸附为核心的应急处理技术工艺，以氯苯作为目标物，研究曝气吹脱和PAC吸附两种技术对水中氯苯的去除效能及其影响因素，并基于两者各自特点和优势，实现两者技术耦合，结合后续常规处理工艺达到高效经济地去除水中VOCs的目的。同时，还开展了活性炭纤维（ACF）吸附吹脱气体中氯苯和水中活性炭表面氯苯脱附规律研究，旨在开发和采取相应技术措施以避免水处理过程中VOCs二次污染。
曝气吹脱对氯苯的去除效率主要受气水比和水温的影响，吹脱效率与气水比和水温具有正相关性，氯苯初始浓度和原水浊度对曝气吹脱去除率影响不大，共存其他VOCs可提高氯苯吹脱去除效率，表现出协同去除效应。曝气吹脱过程中，气水总传质系数与氯苯初始浓度呈显著线性关系，与单位面积曝气量和水温呈非线性正相关性。当采用50-100的气水比时，氯苯吹脱去除率可达83.73%-91.14%，运行成本约0.033-0.0654元/吨水，处理较为经济高效。当气水比高于100时，曝气吹脱处理变得不经济。
PAC可快速吸附水中氯苯，5min吸附量即可达到平衡吸附量的80%以上，30min吸附量可达98%以上。PAC对氯苯的吸附效能主要受PAC比表面积和搅拌混合程度影响，受水温、pH值、离子强度等因素影响不大。基于吸附速率和吸附平衡模型参数建立了基于氯苯初始浓度、PAC投量和吸附时间的吸附经验模型，可以较好地预测氯苯不同污染水平下所需的PAC投量。为验证和校核模型预测值，分别开展了小试和中试研究，最终给出了氯苯不同污染水平下所需的PAC投量。另外，中试结果表明PAC吸附阶段是水中氯苯去除的主要阶段，去除率为62.5%-98.9%；常规工艺可去除水中吸附了氯苯的PAC和其他颗粒，进一步去除水中氯苯；作为水质安全保障的最后一道关口，GAC滤柱可以去除煤砂滤池出水中微量氯苯。
曝气吹脱与PAC吸附耦合技术，可与现有水处理工艺有机结合，充分发挥吹脱和吸附两种技术各自优势，使两种技术分担了不同负荷的污染物去除任务，使得对污染物的可控超标倍数有明显增长，提高了应对水源水发生氯苯污染的处理能力，且能够到取得高效、经济的处理结果。以曝气吹脱-PAC吸附耦合技术为氯苯去除的核心技术、以常规处理单元为水处理工艺主体、以GAC滤池为末端安全关口的应急处理技术工艺，可以作为我国大多数水厂应对水源水突发氯苯污染的应急处理技术工艺。
竞争性吸附和浓差驱动作用会造成污染物在活性炭上脱附。在直接强竞争吸附物（乙苯）、堵塞孔道型大分子吸附物（PSS）的竞争吸附作用以及浓差驱动作用下，吸附在PAC上的氯苯会出现不同程度地脱附。在乙苯强竞争吸附作用下，氯苯在PAC上快速脱附，20-40min可达到脱附平衡，脱附量可达3%-63%，氯苯脱附量和脱附速率与竞争性吸附物（乙苯）浓度具有正相关性。PSS对氯苯在PAC上的吸附量和脱附量基本无影响，但吸附在PAC大孔中PSS会产生堵塞作用，降低氯苯在PAC上的脱附速率。浓差驱动会导致氯苯在PAC上脱附显著，且脱附量随着浓差梯度增大而增加。在水源水突发氯苯污染消除后，在GAC滤池后续运行中，竞争性吸附造成氯苯脱附的风险较小，而浓差驱动造成氯苯脱附风险很大，因此应在突发污染消除后，建议立即更新GAC滤池的活性炭。
吹脱气体中的氯苯可用ACF吸附去除，其吸附去除效能与ACF的BET比表面积、微孔容积、表面化学性质，以及相对湿度（RH）和温度等因素有关。BET比表面积和微孔容积越大，ACF对氯苯吸附速率和吸附量越大。RH对氯苯在ACF上吸附具有抑制作用，且随着RH增大而增强，RH高于50%时，ACF对氯苯的吸附量下降明显。水分子竞争性吸附以及其在微孔中的毛细凝结是其抑制氯苯吸附的主要原因。通过浸渍尿素或硫酸铜再在氮气流下高温处理，进行ACF表面化学改性，一方面可降低表面含氧量，减少酸性官能团含量，提高表面憎水性，减轻RH对氯苯吸附的抑制作用；另一方面，改性后ACF表面生成了含氮的碱性官能团，可提高ACF与氯苯之间的π-π色散力，提高ACF对氯苯的吸附速率和吸附量；另外，经硫酸铜浸渍再高温改性后，ACF表面会负载CuO微晶，其对VOCs具有更强的吸附力。温度对ACF吸附氯苯的效能影响显著，随着温度的升高，氯苯吸附量明显降低。
As the fast development of national economy, industrialization process and theescalation of people’s living standard, the water quality of drinking water sourcedecreased caused by the high development and adequate utilization of waterresources, the serious water pollution caused by organic material, and the frequentlysudden water pollution accidents. However, the relatively undeveloped watertreatment process had weak ability to cope with sudden pollution in raw water formost waterworks in china. Consequently, the study of emergency water treatmenttechnology and process had an important current significance.
Emergency water treatment technology based on air stripping and PACadsorption was established to resolve the problem of volatile organic compound(VOC) sudden pollution in raw water. Chlorobenzene (CB) was used as the targetvolatile organic compound (VOC) in this paper. Experiments were conducted tostudy efficiency and influencing factors of VOCs removal by PAC adsorption andair stripping. Based on their respective advantages and characteristics, the twotechnologies of PAC adsorption and air stripping was coupled and then combinedwith the following conventional water treatment process in order to improve VOCsremoval efficiency and decrease the operation cost. Additionally, experiments wasconducted to study the adsorption of VOCs onto ACF from the off-gas emitted byair stripping and the desorption of VOCs from PAC in water, in order to developsome technology to avoid secondary contamination.
Air-water ratio and temperature were the main factors influencing the removalof CB by air stripping, and the removal of CB was positively correlated with air-water ratio and temperature. However, the removal of CB by air stripping had littlerelationship with CB initial concentration and turbidity. Synergistic removal effectswas found between different VOCs while air stripping.
A static mass transfer kinetic model was fitted to the experimental data toobtain the overall mass transfer coefficient. The result showed that the overall masstransfer coefficient had linear increasing relationship with CB initial concentration,and had nonlinear increasing relationship with air flowrate and temperature. Adynamic air stripping model was used to study the removal efficiency at differentair-water ratio. It was found that air stripping was efficient and economical at theair-water ratio of500-100with the removal rate of83.73%-91.14%and theoperation cost of0.033-0.065Yuan/t. However, the operation cost would increasewhen the air-water ratio was more than100.
PAC can adsorb CB from water rapidly with80%and98%of the equilibrium adsorption capacity at5min and30min, respectively. PAC surface area and mixingintensity had an important influence on the adsorption efficiency by PAC, whilefactors such as temperature, pH value and ionic strength had little effect on CBremoval by PAC adsorption. Adsorption kinetics and equilibrium could besuccessfully simulated by the pseudo-second kinetic model and Freundlich model,respectively. Based on the parameters obtained from the models above, a theoreticalformula of PAC dose with initial CB concentration and adsorption time wasestablished and verified by experimental results. And the recommended PAC dosewas given based on the result above. It is concluded from pilot test that the mixtureof PAC and water and the coagulation clarification were the key process to removeCB, and the removal could reach62.5%-98.9%; the conventional treatment processcould intercept the micro flocs and particles carrying CB in water, resulting in thefurther reduce of CB; as a safety guarantee, granular activated carbon filter columnwas the last process to remove CB.
The combining technology of PAC adsorption and air stripping could integrateinto the conventional water treatment process, and take the advantage of the twotechnology. PAC adsorption and air stripping shared different CB removal load,which could improve the ability of CB removal, and obtain an efficient andeconomical outcome. Emergency treatment process, with the combining technologyof air stripping and PAC adsorption being the core, the conventional water treatmentprocess being the main part, and GAC filter being the last safety guarantee, could beused to cope with VOCs sudden pollution in source water for most waterworks inour country.
Competitive adsorption and concentration gradient drive would causecontaminant desorption from activated carbon. CB desorption happened withvarying degrees under the influence of competitive adsorption by stronglycompeting background compounds (CB) and pore-blocking background compounds(PSS), and the driving force by concentration gradient. CB desorbed rapidly fromactivated carbon, and reached equilibrium within20-40min. The percent of CBdesorption was3%-63%at equilibrium. It was found that the rate and amount of CBdesorption was positively correlated with the concentration of competitioncompounds (ethylbenzene). PSS had slightly effect on CB adsorption or desorptiononto activated carbon, while it slowed the rate of CB desorption due to the pore-blocking effect of PSS in macropore of activated carbon. The driving force byconcentration gradient influenced CB desorption notably. CB desorption amountincreased with increasing concentration gradient. The percent of CB desorption was32%and40%when the solution of CB and activated carbon equilibrium system wasdiluted to5and10times, respectively. The risk of CB desorption from activatedcarbon was assumed low when competitive adsorption existed, but very high if concentration gradient drive effect became notable, which always existed in theGAC filter having used for a sudden pollution. Therefore, these used activatedcarbon in GAC filter should be replaced if the filter would run after the suddenwater pollution.
CB in the off-gas emitted by air stripping could be removed efficiently byactivated carbon fiber (ACF) adsorption, whose removal efficiency was concernedwith BET surface area, micropore volumn and surface chemical character of ACF,relative humidity (RH) and temperature. The larger the BET surface area andmicropore volumn, the greater the adsorption rate and capacity. RH had aninhibitory effect on CB adsorption onto ACF. Moreover, with increasing RH, theinhibitory effect becomes more significant. When RH was higher than50%, CBadsorption amount reduce remarkably by more than13%. The main factorsrestraining CB adsorption onto ACF was the competitive adsorption and capillarycondensation of water molecular in micropore. Surface modification of ACF wasconducted by being impregnated with urea or copper sulphate solution and thenheated at800℃in the environment of nitrogen. On the one hand, it was proved thatsurface modification could decrease oxygen content, and reduce acid functionalgroups, and improve surface hydrophobicity of ACF surface, and then lower wateradsorption amount. As a result, the inhibitory effect of RH on CB adsorption wasrelieved. On the other hand, the generation of basic functional groups could increasethe adsorption rate and amount of CB adsorption onto ACF due to the increase in π-π dispersive interactions between the π-electron system of the carbon graphenelayers and the π-electrons of the ring of CB molecular. Additionally, the load ofcopper oxide microcrystal enhanced VOCs adsorption because of the highadsorption bond between copper oxide microcrystal and CB molecular. Temperatureis an important factor to affect CB adsorption onto ACF. Experimental resultsshowed that CB adsorption amount decreased with increasing temperature.
引文
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