多环芳烃类污染物在黄土中的迁移转化
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摘要
近几十年来，随着西部黄土地区石油工业的迅速发展和事实上的粗放型经营方式，尤其是原油采炼业的大规模开发与兴建，对自然环境带来的污染日趋严重，已经导致了地表土壤、水体大面积石油污染，而石油组分中毒性最强的是芳烃类物质，尤其是以双环和三环为代表的多环芳烃毒性更大。目前，国内外对此类化合物在土壤中的迁移转化规律的研究十分重视，以期为预测多环芳烃对土壤及地下水的污染和治理这一课题提供一个理论依据。在研究这一迁移转化规律时，土壤对多环芳烃类化合物的吸附有着不可忽视的重要作用，吸附过程受诸多因素的影响，掌握其进入土壤后的归趋，就有可能通过强化或控制其某些过程，避免或减小其危害。西部黄土地区的自然环境已不同程度地遭到多环芳烃的污染，而且在今后相当长的一个时期内还有可能遭到更大的污染。因此不论是从治理已被多环芳烃污染的土壤和河流的角度，还是从保护未被污染的土壤和水资源的角度，进行多环芳烃类污染物在土壤中的迁移转化规律的研究都有助于为黄土地区的环境保护和治理提供科学依据。
第一章 多环芳烃类污染物在黄土中的迁移转化研究进展
文中较系统地评述了多环芳烃类污染物在土壤中的迁移转化研究进展，其中包括多环芳烃的形成机理和分布、迁移转化的研究现状、在土壤中的吸附和解吸，以及研究意义。引用文献68篇。
第二章 GC-MS分析玉门矿区石油污染物
玉门油田是我国开采较早的大型油田之一，经过近四十年的开发利用，在原油开采及石油化工生产过程中存在着直接或间接地向环境排放有害有机物的可能性。尤其是在采油矿区内，原油在储存、运输和装卸过程中，泄漏的固液态有毒有机物质，易对污染矿区及周边地区土壤产生持久性的影响，并随时间的推移在土壤中累积或其存在形式发生转化。利用GC-MS法对玉门矿区的管道原油、落地原油、以及被石油污染的土壤和污染地区不同地点的水样进行了有机污染物的分析。结果表明都含有美国EPA规定的优先污染物。
屠忌…类}多环芳径美污袭匆注声士功时迁参君钻
第三章蔡和菲在黄土上的吸附动力学
以蔡和菲为研究对象，对比研究了天然黄土和十六烷基三甲基澳化钱(H DTMAB)
改性的黄土对蔡和菲的吸附动力学行为。蔡和菲在阳离子表面活性剂改性黄土上吸附速
率比在天然黄土上的快至少3倍，同时吸附数据都能很好的符合一级动力学方程;吸附
速率与起始浓度、温度及黄土本身的性质有关;蔡和菲的吸附速率常数k与温度T成负
相关。蔡和菲在天然黄土和阳离子改性黄土上的吸附速率由膜扩散和孔扩散过程控制，
膜扩散是快速吸附过程，而孔扩散是慢速达到平衡过程，实验数据可以用扩散动力学方
程拟合。
第四章蔡和菲在黄土上的吸附热力学
以蔡和菲作为代表物质，探讨了其在黄土上的吸附特征，即吸附等温线和吸附热力
学，同时还研究了阳离子表面活性剂改性黄土对蔡和菲的吸附规律。比较分析了常用的
平衡吸附模型:Linear方程、Freundhch方程和1朋gmuir方程描述蔡和菲在黄土上吸附
等温线的准确性，并从热力学的角度探讨了蔡和菲在黄土上的吸附热和标准自由能的变
化，吸附是一个放热过程，标准自由能的变小是蔡和菲在黄土上吸附的推动力。
第五章玉门矿区污染黄土中原油的解吸研究
用振荡平衡法研究了玉门矿区原油污染黄土中原油的解吸行为，测得了解吸常数，
绘出了解吸等温线。利用Freundhch方程可较好地描述黄土中原油的解吸状况;黄土中
原油的解吸行为受温度、溶液的pH值和表面活性剂的影响;温度和PIl值越高，原油的
解吸量越大;阴离子表面活性剂的加入有助于原油的解吸，在相同条件下使解吸率提高
了5倍，阳离子和非离子表面活性剂的加入不利于原油解吸，但是阳离子表面活性剂的
加入有利于原油在土壤中的截留以及回收再利用。
第六章同步荧光法同时测定黄土中的菲和蔡
由于一些多环芳烃的性质相似，其混合物中各自含量的常规分析法繁琐费时。采用
硕士研究生:展惠英;专业:分析化学;研究方向:环境化学
导师:陈慧教授
展潇奥飞多万芳密类污袭匆座!煮士功必迁参羚常
了固定波长同步荧光法研究了菲和蔡同时快速分析的可能性，建立了相应的测试方案，
用于测定菲和蔡混合液在黄土中吸附行为，样品无需过滤，操作简便。
Loess soils topographically cover the vast land in northwest China where oil fields are widely exploited in the recent four decades, and resulted in the severe petroleum contamination of soils and water resources through various ways including spillage of crude oil nearby the drilling wells, leakage from storage tanks and pipelines. As a class of petroleum compounds, polycyclic aromatic hydrocarbons (PAHs) present a group of compounds with two or more fused aromatic rings that are mutagenic, carcinogenic and teratogenic, and PAHs are included in the CERLA Priority List of Hazardous Substances. At present it was specially regarded to study the transfer and transform of PAHs in domestic and international, and was expected to forecast contamination rule of PAHs in soil and grouderwater and to provide a theoretical basis of studying contamination control and remediation. At studying the rule of transfer and transform, soil sorption to the compound of PAHs have a very important function. The sorption process was
influenced with many factors. If these factors can be predominated, we can avoid or lessen contamination of PAHs to soil and groundwater through intensifying or controlling some factors of sorption process. The natural environment of western region was contaminated with PAHs, and it was potential to be contaminated seriously in a very long period. Studying the transfer and transform of PAHs in the soils, it can help to provided a scientific basis to protect environment and manage contamination without reference to manage the soils and water resources contaminated with PAHs or to protect the soils and water resources uncontaminated with PAHs.
Chapter 1.
Advances in the Research on the Transfer and Transform of Polycyclic
Aromatic Hydrocarbons in Loess Soils
A review is reported with 68 references about the formation mechanism and distribution of polycyclic aromatic hydrocarbons, the transfer and transform study and sorption and desorption, meantime reviewing the research significance on the transfer and transform of polycyclic aromatic hydrocarbons in soils.
Chapter 2.
Analysis of Petroleum Pollutants in Yumen's Mining Areas by Gas Chromatography and Mass Chromatography
The oil-field of Yumen is the one of the large oil-fields exploited more early in our country. Through exploiting and using in the recent four decades, it resulted in the severe petroleum contamination of soils and water resources including spillage of crude oil nearby the drilling wells, leakage from storage tanks and pipelines. Petroleum is a kind of complex mixture containing hydrocarbon and non-hydrocarbon compounds with various physical and chemical properties. Gas chromatography and mass spectrometry were used to analysis crude oil in pipline and bulk, and water samples comprising petroleum contaminants at separate sites in Yumen's mining areas. The results show that there were priority pollutants that were published by Environmental Protection Agency in the United States. More information of petroleum compounds were obtained by using gas chromatography and mass spectrometry than by traditional methods.
Chapter 3.
Sorption Kinetics of Naphthalene and Phenanthrene in Loess Soils
Naphthalene and phenanthrene were chosen as organic contaminant indicators in loess soil modified by the cation surfactant hexadecyltrimethylammonium (HDTMA) bromide. The kinetic behavior of sorption during transport in both natural and modified loess soil was studied. The results indicated that sorption rate in the cation surfactant modified loess soils was at least 3 times faster than that of the natural soil. A first-order kinetics model fitted the sorption data well for both soils. The sorption rates of the two organic compounds were related to their primary residuai quantity on the soils. The rate constants, however, displayed negative correlation with increasing temperature. Sorption rates of naphthalene and phenanthrene on loess soils and and the modified loess soils with a cation surfactant hexadecyltrimethylammonium (HDTMA) bromid
第一章 多环芳烃类污染物在黄土中的迁移转化研究进展
文中较系统地评述了多环芳烃类污染物在土壤中的迁移转化研究进展，其中包括多环芳烃的形成机理和分布、迁移转化的研究现状、在土壤中的吸附和解吸，以及研究意义。引用文献68篇。
第二章 GC-MS分析玉门矿区石油污染物
玉门油田是我国开采较早的大型油田之一，经过近四十年的开发利用，在原油开采及石油化工生产过程中存在着直接或间接地向环境排放有害有机物的可能性。尤其是在采油矿区内，原油在储存、运输和装卸过程中，泄漏的固液态有毒有机物质，易对污染矿区及周边地区土壤产生持久性的影响，并随时间的推移在土壤中累积或其存在形式发生转化。利用GC-MS法对玉门矿区的管道原油、落地原油、以及被石油污染的土壤和污染地区不同地点的水样进行了有机污染物的分析。结果表明都含有美国EPA规定的优先污染物。
屠忌…类}多环芳径美污袭匆注声士功时迁参君钻
第三章蔡和菲在黄土上的吸附动力学
以蔡和菲为研究对象，对比研究了天然黄土和十六烷基三甲基澳化钱(H DTMAB)
改性的黄土对蔡和菲的吸附动力学行为。蔡和菲在阳离子表面活性剂改性黄土上吸附速
率比在天然黄土上的快至少3倍，同时吸附数据都能很好的符合一级动力学方程;吸附
速率与起始浓度、温度及黄土本身的性质有关;蔡和菲的吸附速率常数k与温度T成负
相关。蔡和菲在天然黄土和阳离子改性黄土上的吸附速率由膜扩散和孔扩散过程控制，
膜扩散是快速吸附过程，而孔扩散是慢速达到平衡过程，实验数据可以用扩散动力学方
程拟合。
第四章蔡和菲在黄土上的吸附热力学
以蔡和菲作为代表物质，探讨了其在黄土上的吸附特征，即吸附等温线和吸附热力
学，同时还研究了阳离子表面活性剂改性黄土对蔡和菲的吸附规律。比较分析了常用的
平衡吸附模型:Linear方程、Freundhch方程和1朋gmuir方程描述蔡和菲在黄土上吸附
等温线的准确性，并从热力学的角度探讨了蔡和菲在黄土上的吸附热和标准自由能的变
化，吸附是一个放热过程，标准自由能的变小是蔡和菲在黄土上吸附的推动力。
第五章玉门矿区污染黄土中原油的解吸研究
用振荡平衡法研究了玉门矿区原油污染黄土中原油的解吸行为，测得了解吸常数，
绘出了解吸等温线。利用Freundhch方程可较好地描述黄土中原油的解吸状况;黄土中
原油的解吸行为受温度、溶液的pH值和表面活性剂的影响;温度和PIl值越高，原油的
解吸量越大;阴离子表面活性剂的加入有助于原油的解吸，在相同条件下使解吸率提高
了5倍，阳离子和非离子表面活性剂的加入不利于原油解吸，但是阳离子表面活性剂的
加入有利于原油在土壤中的截留以及回收再利用。
第六章同步荧光法同时测定黄土中的菲和蔡
由于一些多环芳烃的性质相似，其混合物中各自含量的常规分析法繁琐费时。采用
硕士研究生:展惠英;专业:分析化学;研究方向:环境化学
导师:陈慧教授
展潇奥飞多万芳密类污袭匆座!煮士功必迁参羚常
了固定波长同步荧光法研究了菲和蔡同时快速分析的可能性，建立了相应的测试方案，
用于测定菲和蔡混合液在黄土中吸附行为，样品无需过滤，操作简便。
Loess soils topographically cover the vast land in northwest China where oil fields are widely exploited in the recent four decades, and resulted in the severe petroleum contamination of soils and water resources through various ways including spillage of crude oil nearby the drilling wells, leakage from storage tanks and pipelines. As a class of petroleum compounds, polycyclic aromatic hydrocarbons (PAHs) present a group of compounds with two or more fused aromatic rings that are mutagenic, carcinogenic and teratogenic, and PAHs are included in the CERLA Priority List of Hazardous Substances. At present it was specially regarded to study the transfer and transform of PAHs in domestic and international, and was expected to forecast contamination rule of PAHs in soil and grouderwater and to provide a theoretical basis of studying contamination control and remediation. At studying the rule of transfer and transform, soil sorption to the compound of PAHs have a very important function. The sorption process was
influenced with many factors. If these factors can be predominated, we can avoid or lessen contamination of PAHs to soil and groundwater through intensifying or controlling some factors of sorption process. The natural environment of western region was contaminated with PAHs, and it was potential to be contaminated seriously in a very long period. Studying the transfer and transform of PAHs in the soils, it can help to provided a scientific basis to protect environment and manage contamination without reference to manage the soils and water resources contaminated with PAHs or to protect the soils and water resources uncontaminated with PAHs.
Chapter 1.
Advances in the Research on the Transfer and Transform of Polycyclic
Aromatic Hydrocarbons in Loess Soils
A review is reported with 68 references about the formation mechanism and distribution of polycyclic aromatic hydrocarbons, the transfer and transform study and sorption and desorption, meantime reviewing the research significance on the transfer and transform of polycyclic aromatic hydrocarbons in soils.
Chapter 2.
Analysis of Petroleum Pollutants in Yumen's Mining Areas by Gas Chromatography and Mass Chromatography
The oil-field of Yumen is the one of the large oil-fields exploited more early in our country. Through exploiting and using in the recent four decades, it resulted in the severe petroleum contamination of soils and water resources including spillage of crude oil nearby the drilling wells, leakage from storage tanks and pipelines. Petroleum is a kind of complex mixture containing hydrocarbon and non-hydrocarbon compounds with various physical and chemical properties. Gas chromatography and mass spectrometry were used to analysis crude oil in pipline and bulk, and water samples comprising petroleum contaminants at separate sites in Yumen's mining areas. The results show that there were priority pollutants that were published by Environmental Protection Agency in the United States. More information of petroleum compounds were obtained by using gas chromatography and mass spectrometry than by traditional methods.
Chapter 3.
Sorption Kinetics of Naphthalene and Phenanthrene in Loess Soils
Naphthalene and phenanthrene were chosen as organic contaminant indicators in loess soil modified by the cation surfactant hexadecyltrimethylammonium (HDTMA) bromide. The kinetic behavior of sorption during transport in both natural and modified loess soil was studied. The results indicated that sorption rate in the cation surfactant modified loess soils was at least 3 times faster than that of the natural soil. A first-order kinetics model fitted the sorption data well for both soils. The sorption rates of the two organic compounds were related to their primary residuai quantity on the soils. The rate constants, however, displayed negative correlation with increasing temperature. Sorption rates of naphthalene and phenanthrene on loess soils and and the modified loess soils with a cation surfactant hexadecyltrimethylammonium (HDTMA) bromid
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[65] Z Li, Y Shi. The solubilization and desorption of biosurfactants to bioremediation. J
Biotechnology, 1996,12:238-241.
[66] J F Lee, J R Crum and S A Boyd. Enhanced retention of organic contaminants by soills exchanged with organic cations. Environ Sci Technol, 1989, 23:1365-1372.
[67] S A Boyd, W F Jaynes and B S Ross. Immobilization of organic contaminatants by organoclays. Organic Substances And Sediments In Water, 1991,1:181-200.
[68] W F Jaynes and S A Boyd. Hydrophobicity of siloxane surfaces in smectite as revealed by aromatic hydrocarbon adsorption from water. Clays Miner, 1991,39:428-436.
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