西北黄土地区水源水库水—沉积物中石油污染特征及土壤生物修复技术研究
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摘要
石油污染的普遍性、复杂性、难降解性，使其受到众多学者的关注。西北黄土地区由于其独特的气候和土壤特征，石油物质对环境的污染方式及其治理手段也具有特殊性。本课题以西北黄土地区石油污染为研究背景，从模拟沉积物中石油污染物静态释放出发，研究不同季节条件下，石油物质在水体和沉积物中的迁移规律，得到相应的静态释放动力学模型；然后以延安地区主要供水水源地—王瑶水库为研究对象，系统地研究石油污染物在沉积物中的分布特征，分析水库各支流流域和主体河道的历年污染状况，在此基础上对土壤的生物修复技术进行了系统研究。主要研究成果如下：
（1）采用滞膜模型描述沉积物中石油污染物对上覆水体的静态释放过程，其释放动力学方程为：K_r和C_W*分别代表石油物质的释放速率常数和达到释放平衡时水相中石油物质的浓度，可以通过实验获得。静态实验结果显示，温度对沉积物中石油物质向水体中释放速率有重要影响。当沉积物石油污染强度在320mg/kg-4792mg/kg之间时，夏季的动力学参数表达式为：K_r=5.51ln(C_(S0))-0.25C_W*=0.0003C_(S0)+6.86冬季的动力学参数表达式为：K_r=3.28ln(C_(S0))+12.20C_W*=0.0005C_(S0)+4.68据此可以得到夏季和冬季的静态释放动力学方程，然后通过验证，模型可行。
（2）夏季（温度在30℃左右）的静态实验结果显示，当沉积物的石油污染强度C_(S0)分别为320mg/kg和810mg/kg时，三次释放平衡后沉积物分层分析显示，对上覆水体的污染起主要作用的有效深度为沉积物上层10cm左右；当沉积物石油污染强度在1000mg/kg以下时，污染物对上覆水体的污染可持续时间约为60天。
（3）沉积物中石油组分分析结果显示，在检测出的23种石油物质中，除二十八烷、胆固醇以及异三十烷基本不能进入上覆水体外，其余20种物质均可以不同程度的进入水体。碳原子数小于12的烷烃属于易进入水体物质，大于17的烷烃，属于难进入水体物质，在C_(12)和C_(17)之间的烷烃是水相石油污染物的主要组成部分。7种多环芳烃中，除二苯并[a, h]蒽较难进入上覆水体外，其余6种物质均属于可进入水体物质，它们对环境和人体健康有重大危害。
（4）以陕北延安供水水源地—王瑶水库为研究区域，通过对10个断面40个取样位置共400个样品的石油污染含量分析得出，王瑶水库坝前沉积物表层的石油含量在203mg/kg左右，对上覆水体水质影响较大；研究区域内的5条支流中，支流二水质最好，且流量较大，对减轻主河道污染起积极作用；其余4条支流流域污染均较为严重，其中，支流三和支流四流域内石油污染状况最为严重，对水库污染的贡献最大，支流一和支流五由于水量小对主体河段影响较小，但其污染状况有日益加深的趋势；污染较严重的支流三和支流四入口位置表层沉积物中检测出3种烷烃，9种多环芳烃，因此，王瑶水库存在潜在的多环芳烃污染。
（5）在实验室好氧条件下，通过驯化筛选，从安塞油田废弃井场石油污染土样中富集分离出5株高效石油降解菌，经形态观察和生理生化试验初步鉴定，它们分别属于假单胞菌属（Pseudomonas sp.）、邻单胞菌属（Plesionmonas sp.）、黄单胞菌属（Xanthomonas sp.）和动胶菌属（Zoogloea sp.）；5株高效菌当pH值在7左右，N/P比在4左右，石油污染强度在1000-1500mg/L之间时，均可获得较高的石油去除率，它们最佳的氮源为NH_4NO_3，但5株高效菌各自适宜的初始pH值、N/P比和石油污染强度范围有所不同。
（6）在西北黄土地区历时80天现场土壤修复试验结果显示，污染物强度对微生物的活性有重要影响。在低污染强度下土壤中的石油去除率较高，但会导致微生物由于碳源不足而生长受到限制；高污染物强度下，土壤内pH值下降程度大，对微生物产生毒害，并抑制其生长。
（7）在石油土壤的生物修复试验中，添加营养物质可以显著提高微生物生长速率和石油降解率；短期内通过加菌操作可以获得较好的石油去除效果；单一的翻耕操作导致土壤中含水率降低，抑制微生物生长，石油降解率下降。
Petroleum pollution is widespread, complex, and disdegradational. Special climate and soilcharacteristics result in the differences of petroleum pollution style to environment andpetroleum pollution treatment means in Northwest Loess Area. The study was under thebackground of petroleum pollution in Northwest Loess Area. By simulating the static releaseof the petroleum pollutants in sediments, which meaned that petroleum transferred fromsediments to superior water body, the transference rule of petroleum in water body andsediments and static dynamic models was obtained under the different season. Thedistribution characteristics of petroleum pollutants in sediments and yearly oil contaminatedstates of branch catchment basin and main waterway were studied at Wangyao reservoir,which was the main water supply source of Yan’an. And the bioremendiation technology ofoil contaminated soil was systematically studied. The main research contents and results wereas follows:
(1) The static release process of petroleum pollutants in sediments was described bystagnant film model. The release dynamic equation was as follows:K_rand C_W*, which were obtained by static experiments, were release rate constant ofpetroleum pollutants and petroleum concentration in aqueous phase under release balancerespectively. Temperature was a main factor which influenced the release rate of petroleumpollutants in sediments. When the oil contaminated concentration were between320mg/kg and4792mg/kg, the summer dynamic parameters equations were as fllows:K_r=5.51ln (C_(S0))-0.25C_W*=0.0003C_(S0)+6.86The winter dynamic parameters equations were as fllows:K_r=3.28ln (C_(S0))+12.20C_W*=0.0005C_(S0)+4.68According to these equations the summer and winter dynamic models were establishedrespectively. And the feasibility of models was verified.
(2) The results of the static release experiments in the summer, when the temperature wasabout30℃and the oil contaminated concentration was between320mg/kg and810mg/kgrespectively in sediments, showed that the sediments effective depth, in which thepetroleum pollutants affected the water quality of superior water body, was about10cm bythree layer analysises of sediments after release balance, and showed that the secondpollution of sediments lasted for about60days, when oil contaminated concentration wasbelow1000mg/kg in sediments.
(3) The results of petroleum component analysis in sediments showed that there were23kinds compounds. Besides of octacosane, cholesterin and squalane, the rest20kinds couldenter the superior water body. The substances whose carbon number was below12easilyentered the water body, and the substances whose carbon number was over17difficultlyentered the water body. The substances whose carbon number was between12and17weremain components of petroleum pollutants in water body. Among the7kinds polycyclicaromatic hydrocarbon, besides of dibenzo [a, h] anthracene, the rest6kinds, which hadgreat dangers to environment and human health, could enter water body.
(4) The Wangyao reservoir, the main water supply source of Yan’an, was studied. All ofthe results were gained by400samples at40positions on10cross-sections. The petroleumconcentration of surface layer sediments was about203mg/kg at ante-dam in Wangyaoreservoir. There were5branches. The branch two whose water quality was the best andwater quantity was most great, improved the main waterway pollution. The rest branchcatchment basins were severely polluted. The branch one and five, whose water quantitywere little and pollution station had more and more serious tendency, had the little influenceon the main waterway water quality. But the branch three and four, whose water quality was worst and water quantity was greater, had the serious influence on the main waterway waterquality. There were three kinds diolefine and9kinds polycyclic aromatic hydrocarbon insurface sediments, which meaned that the Wangyao reservoir might be polluted by thepolycyclic aromatic hydrocarbon, at the entrance position of the branch three and four.
(5) In laboratory the5highly efficient petroleum-degrading strains were screened underaerobic condition from oil contaminated soil obtained from the abandoned well site at Ansaioilfield in Yan’an. The5strains were GX1（Pseudomonas sp.）、GX2（Plesionmonas sp.）、GX3（Xanthomonas sp.）、GX4（Pseudomonas sp.）and GX5（Zoogloea sp.）., The highdegradation rates of the5strains were obtained, when the pH value was about7, the N/Pratio was about4and the petroleum concentration was below1000mg/L. The optimalnitrogen source was NH_4NO_3. But the eligible ranges of the initial pH value, N/P ratio andthe petroleum concentration were different.
(6) The results in the field experimentation that lasted for80days in Northwest LoessArea showed that the petroleum concentration had great influence on the activity ofmicroorganism. The higher oil removal efficency rate was obtained at the lower petroleumconcentration, but the growth of microorganism was limited because of the absence ofcarbon source. At the higher petroleum concentration, the decreasing extent to the pH valuein the soil was too large and the growth of microorganism in the soil was inhibited bytoxicum.
(7) In the field experimentation, adding nutrient was good to the growth ofmicroorganism and the oil removal efficency rate. By seeding highly efficientpetroleum-degrading strains, the higher oil removal efficency rate was obtained in the shortterm. The growth of microorganism was inhibited and the oil degradation rate decreasedbecause the simple plowing induced decreasing of water content in the soil.
（1）采用滞膜模型描述沉积物中石油污染物对上覆水体的静态释放过程，其释放动力学方程为：K_r和C_W*分别代表石油物质的释放速率常数和达到释放平衡时水相中石油物质的浓度，可以通过实验获得。静态实验结果显示，温度对沉积物中石油物质向水体中释放速率有重要影响。当沉积物石油污染强度在320mg/kg-4792mg/kg之间时，夏季的动力学参数表达式为：K_r=5.51ln(C_(S0))-0.25C_W*=0.0003C_(S0)+6.86冬季的动力学参数表达式为：K_r=3.28ln(C_(S0))+12.20C_W*=0.0005C_(S0)+4.68据此可以得到夏季和冬季的静态释放动力学方程，然后通过验证，模型可行。
（2）夏季（温度在30℃左右）的静态实验结果显示，当沉积物的石油污染强度C_(S0)分别为320mg/kg和810mg/kg时，三次释放平衡后沉积物分层分析显示，对上覆水体的污染起主要作用的有效深度为沉积物上层10cm左右；当沉积物石油污染强度在1000mg/kg以下时，污染物对上覆水体的污染可持续时间约为60天。
（3）沉积物中石油组分分析结果显示，在检测出的23种石油物质中，除二十八烷、胆固醇以及异三十烷基本不能进入上覆水体外，其余20种物质均可以不同程度的进入水体。碳原子数小于12的烷烃属于易进入水体物质，大于17的烷烃，属于难进入水体物质，在C_(12)和C_(17)之间的烷烃是水相石油污染物的主要组成部分。7种多环芳烃中，除二苯并[a, h]蒽较难进入上覆水体外，其余6种物质均属于可进入水体物质，它们对环境和人体健康有重大危害。
（4）以陕北延安供水水源地—王瑶水库为研究区域，通过对10个断面40个取样位置共400个样品的石油污染含量分析得出，王瑶水库坝前沉积物表层的石油含量在203mg/kg左右，对上覆水体水质影响较大；研究区域内的5条支流中，支流二水质最好，且流量较大，对减轻主河道污染起积极作用；其余4条支流流域污染均较为严重，其中，支流三和支流四流域内石油污染状况最为严重，对水库污染的贡献最大，支流一和支流五由于水量小对主体河段影响较小，但其污染状况有日益加深的趋势；污染较严重的支流三和支流四入口位置表层沉积物中检测出3种烷烃，9种多环芳烃，因此，王瑶水库存在潜在的多环芳烃污染。
（5）在实验室好氧条件下，通过驯化筛选，从安塞油田废弃井场石油污染土样中富集分离出5株高效石油降解菌，经形态观察和生理生化试验初步鉴定，它们分别属于假单胞菌属（Pseudomonas sp.）、邻单胞菌属（Plesionmonas sp.）、黄单胞菌属（Xanthomonas sp.）和动胶菌属（Zoogloea sp.）；5株高效菌当pH值在7左右，N/P比在4左右，石油污染强度在1000-1500mg/L之间时，均可获得较高的石油去除率，它们最佳的氮源为NH_4NO_3，但5株高效菌各自适宜的初始pH值、N/P比和石油污染强度范围有所不同。
（6）在西北黄土地区历时80天现场土壤修复试验结果显示，污染物强度对微生物的活性有重要影响。在低污染强度下土壤中的石油去除率较高，但会导致微生物由于碳源不足而生长受到限制；高污染物强度下，土壤内pH值下降程度大，对微生物产生毒害，并抑制其生长。
（7）在石油土壤的生物修复试验中，添加营养物质可以显著提高微生物生长速率和石油降解率；短期内通过加菌操作可以获得较好的石油去除效果；单一的翻耕操作导致土壤中含水率降低，抑制微生物生长，石油降解率下降。
Petroleum pollution is widespread, complex, and disdegradational. Special climate and soilcharacteristics result in the differences of petroleum pollution style to environment andpetroleum pollution treatment means in Northwest Loess Area. The study was under thebackground of petroleum pollution in Northwest Loess Area. By simulating the static releaseof the petroleum pollutants in sediments, which meaned that petroleum transferred fromsediments to superior water body, the transference rule of petroleum in water body andsediments and static dynamic models was obtained under the different season. Thedistribution characteristics of petroleum pollutants in sediments and yearly oil contaminatedstates of branch catchment basin and main waterway were studied at Wangyao reservoir,which was the main water supply source of Yan’an. And the bioremendiation technology ofoil contaminated soil was systematically studied. The main research contents and results wereas follows:
(1) The static release process of petroleum pollutants in sediments was described bystagnant film model. The release dynamic equation was as follows:K_rand C_W*, which were obtained by static experiments, were release rate constant ofpetroleum pollutants and petroleum concentration in aqueous phase under release balancerespectively. Temperature was a main factor which influenced the release rate of petroleumpollutants in sediments. When the oil contaminated concentration were between320mg/kg and4792mg/kg, the summer dynamic parameters equations were as fllows:K_r=5.51ln (C_(S0))-0.25C_W*=0.0003C_(S0)+6.86The winter dynamic parameters equations were as fllows:K_r=3.28ln (C_(S0))+12.20C_W*=0.0005C_(S0)+4.68According to these equations the summer and winter dynamic models were establishedrespectively. And the feasibility of models was verified.
(2) The results of the static release experiments in the summer, when the temperature wasabout30℃and the oil contaminated concentration was between320mg/kg and810mg/kgrespectively in sediments, showed that the sediments effective depth, in which thepetroleum pollutants affected the water quality of superior water body, was about10cm bythree layer analysises of sediments after release balance, and showed that the secondpollution of sediments lasted for about60days, when oil contaminated concentration wasbelow1000mg/kg in sediments.
(3) The results of petroleum component analysis in sediments showed that there were23kinds compounds. Besides of octacosane, cholesterin and squalane, the rest20kinds couldenter the superior water body. The substances whose carbon number was below12easilyentered the water body, and the substances whose carbon number was over17difficultlyentered the water body. The substances whose carbon number was between12and17weremain components of petroleum pollutants in water body. Among the7kinds polycyclicaromatic hydrocarbon, besides of dibenzo [a, h] anthracene, the rest6kinds, which hadgreat dangers to environment and human health, could enter water body.
(4) The Wangyao reservoir, the main water supply source of Yan’an, was studied. All ofthe results were gained by400samples at40positions on10cross-sections. The petroleumconcentration of surface layer sediments was about203mg/kg at ante-dam in Wangyaoreservoir. There were5branches. The branch two whose water quality was the best andwater quantity was most great, improved the main waterway pollution. The rest branchcatchment basins were severely polluted. The branch one and five, whose water quantitywere little and pollution station had more and more serious tendency, had the little influenceon the main waterway water quality. But the branch three and four, whose water quality was worst and water quantity was greater, had the serious influence on the main waterway waterquality. There were three kinds diolefine and9kinds polycyclic aromatic hydrocarbon insurface sediments, which meaned that the Wangyao reservoir might be polluted by thepolycyclic aromatic hydrocarbon, at the entrance position of the branch three and four.
(5) In laboratory the5highly efficient petroleum-degrading strains were screened underaerobic condition from oil contaminated soil obtained from the abandoned well site at Ansaioilfield in Yan’an. The5strains were GX1（Pseudomonas sp.）、GX2（Plesionmonas sp.）、GX3（Xanthomonas sp.）、GX4（Pseudomonas sp.）and GX5（Zoogloea sp.）., The highdegradation rates of the5strains were obtained, when the pH value was about7, the N/Pratio was about4and the petroleum concentration was below1000mg/L. The optimalnitrogen source was NH_4NO_3. But the eligible ranges of the initial pH value, N/P ratio andthe petroleum concentration were different.
(6) The results in the field experimentation that lasted for80days in Northwest LoessArea showed that the petroleum concentration had great influence on the activity ofmicroorganism. The higher oil removal efficency rate was obtained at the lower petroleumconcentration, but the growth of microorganism was limited because of the absence ofcarbon source. At the higher petroleum concentration, the decreasing extent to the pH valuein the soil was too large and the growth of microorganism in the soil was inhibited bytoxicum.
(7) In the field experimentation, adding nutrient was good to the growth ofmicroorganism and the oil removal efficency rate. By seeding highly efficientpetroleum-degrading strains, the higher oil removal efficency rate was obtained in the shortterm. The growth of microorganism was inhibited and the oil degradation rate decreasedbecause the simple plowing induced decreasing of water content in the soil.
引文
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