石油开采区多环芳烃多介质环境行为及其生态风险研究
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摘要
随着国民经济的快速发展,未来石油供需矛盾突出,我国势必要动用更多的陆地石油地质储量以提高原油产量,这无疑会导致石油开采区逐步向低丰度、低渗透率、低产能贫矿或尾矿储量的石油资源地区转移,由此将引发更多的累积污染和更严峻的石油开采生态风险。对此,查明石油开采污染源头、掌握石油开采产生的典型污染物的迁移转化规律及其生态风险效应,将会为减少源头污染、实现清洁生产,以及污染治理与控制提供科学依据。陆地石油开采过程中产生的多环芳烃(Polycyclic aromatic hydrocarbons, PAHs)等污染物通过轻烃挥发、落地原油、含油废水排放等方式进入到大气、水体、土壤等多介质环境系统中,势必会对石油开采区及其周边环境产生无法忽视的生态影响。然而,现有研究多为针对石油开采污染物对水体、土壤或沉积物单一环境介质污染规律、机理研究,且对风险评价过程中存在的不确定性通常采用概率分析方法进行表征,而针对污染物在石油开采区多介质环境迁移转化规律及生态风险评价,并采用多种不确定性表征方法对生态风险评价中存在的不确定性进行综合定量表征的研究成果较少。本论文对选定的典型陆地石油开采区PAHs多介质环境迁移转化规律、源解析进行了初步研究,研究了土壤介质中PAHs时空分布规律,评价了土壤污染现状,揭示了土壤发光菌毒性与污染物来源间的关系,评价了研究区域内PAHs的动态综合生态风险,并建立了定量表征生态风险评价过程中多种不确定性的方法。
通过对研究区域多介质环境(大气、水、土壤、沉积物)建立稳态、动态及区间动态多介质逸度模型,研究陆地石油开采区PAHs多介质迁移转化、归趋及源解析等环境行为。研究结果表明,石油开采过程中产生的PAHs多以落地原油形式进入环境系统,并以土壤中降解为主要输出途径,土壤介质是PAHs的主要归宿。多介质环境中PAHs的苯环构成结构研究表明,空气相中多为大于4环的PAHs,水中多为2-3环PAHs,土壤中多为3环PAHs,沉积物中多为3-4环PAHs。基于本研究开发的区间动态多介质逸度模型,对1985-2010年间PAHs动态源解析结果表明,大气和土壤介质中PAHs的主要来源是高温燃烧,而水和沉积物介质中PAHs的主要来源是生物质和煤的燃烧。同时,随着陆地石油开采强度的不断增大,PAHs的来源逐渐倾向于石油源的释放。
研究表明,土壤介质是PAHs的主要归宿。因此,本研究应用主成分分析、人工神经网络等方法建立不同来源PAHs土壤发光菌生物毒性神经网络模型对土壤生物毒性进行源解析,并对不同来源PAHs对生物毒性的贡献进行定量表征。模型模拟结果显示,不同PAHs来源对土壤生物毒性的贡献分别为：交通源占13.2%、石油源占37.4%、煤燃烧占36.0%、焦油源占13.4%。此外,基于土壤介质实际采样测试分析结果,对土壤介质中PAHs的空间分布规律及污染等级进行评价,确定影响土壤PAHs污染等级的因素包括井场落地油情况、开采量、开采年限及其周边环境因素(植被状况、土壤类型等)等。计算得到研究区域内重污染、中污染及轻污染采样点分别占8.02%,8.02%和2.29%。
本研究以区间动态多介质逸度模型模拟结果为基础数据,结合模糊理论、概率分析等不确定性表征方法,通过构建模糊的环境质量标准和模糊的健康风险判定标准,构建基于区间动态多介质逸度模型的动态多介质生态风险评价方法框架,并利用所建方法对1985-2020年间研究区域内的PAHs进行动态多介质综合生态风险评价。评价结果显示,NAP和ANY具有最高的环境质量风险,均达到中等风险或低-中风险。进一步将环境质量风险评价结果与PAHs源解析相结合可以看出,本文研究区域中环境质量风险主要来自石油开采和焦炭。此外,1985-2020年间16种PAHs人体健康风险评价结果表明NAP和4环以上PAHs具有较高的人体健康风险,主要来自人体对土壤介质的暴露(>90%),包括土壤摄食(35%),吸入土壤颗粒(35%),皮肤接触土壤(25%)。最后,通过构建模糊规则库,对研究区域内PAHs综合生态风险水平进行表征,NAP、BaA、CHR、BbF、BkF、BaP、IPY和DBA具有“非常高”综合生态风险,应采取全部可能的措施来处理石油开采场地。
With the rapid development of national economy, serious contradiction between oil supply and demand would appear in the future, then China needs to use more onshore oil geological reserves to increase crude oil production, this must result in the petroleum exploitation area transfers to low permeability, low yield, and low abundance area, it must bring more cumulative pollution and worsening ecological risk. Thus, find out the oil pollution source and master the typical petroleum pollutant migration transformation rule and their ecological risk could provide scientific evidence for cleaner production and pollution management and control for petroleum exploitation pollution. The pollutants such as polycyclic aromatic hydrocarbon (PAHs) would enter into air, water, and soil compartment in the process of petroleum exploitation. However, the investigation focus more on the organic pollutant derived from petroleum exploitation in the individual environmental media such as water and soil, and lack of the multimedia environmental pollutant and risk assessment in the onshore oilfield. In this study, the multimedia transport, fate, and source apportionment of PAHs in the onshore oilfield were investigated, and then the spatial distribution and pollutant grade of PAHs in the soil compartment were studied to reveal the relationship between the soil luminescent bacteria biological toxicity and the pollutant sources, the dynamic multimedia integrated ecological risks of16PAHs were assessed in the study area, and the quantitative characterization method of uncertainty in the ecological risk was established.
The multimedia environmental transport, fate, and source apportionment of PAHs in onshore oilfield were investigated through the established steady-state, dynamic-state, and interval dynamic multimedia fugacity (IDMF) model, including air, water, soil, and sediment compartment. The modeling results showed that, the primarily input pathway of PAHs enter the multimedia environments is crude oil spills on the soil, while the output pathway was the degradation of PAHs in the soil compartment. Soil was identified as the dominate sink of PAHs. The ring size distribution indicated that compounds containing more than four rings were dominant in air, two-and three-ring compounds were prevalent in water, three ring compounds were mainly in soil, and four-ring compounds were predominant in sediment. The dynamic source apportionment was taken on basis of the constructed IDMF model, it was demonstrated that high temperature combustion was the major source of PAHs in the air and soil, while biomass and coal combustion were attributed to water and sediment compartments. Besides, the modeling results showed a tended to be from petroleum sources as evidenced by the accumulation effect of PAHs and continuous oil exploitation.
The previous result has showed that, soil compartment was the main sink of PAHs in the multimedia environments. Hence, the methods of principal component analysis (PC A) and artificial neural network (ANN) were applied to identify the sources of PAHs in the soil contaminants, and an ANN model was established to investigate the contribution of the PAHs to soil biotoxicity. The modeling results revealed that the contamination sources included traffic emissions (13.2%), petroleum-related source (37.4%), coal combustion (36.0%), and coke oven source (13.4%). Besides, spatial distribution and pollution grade of PAHs in the soils were analysised based on the actual sampling and analysis of the collected soils from the six oil wells in the study oilfield. Relevant effect factors of the concentrations level were concluded as condition of ground oil, exploitation scale, exploitation time, and surrounding environment (including vegetation condition, primitive soil types, etc.). Soil pollution grade of the six oil wells were also evaluated through the method of a modified Nemerow Index Method. The evaluation result showed that the percentages of heavy pollution, moderate pollution, and slight pollution were8.02%,8.02%, and2.29%, respectively.
Finally, the IDMF model assisted dynamic multimedia integrated ecological risk assessment (IDMF-DMIERA) approach framework was developed. The approach framework was on basis of the modeling results of IDMF model, combining with the uncertainty representation approaches of interval parameter, fuzzy theory, and probability analysis. And then the developed IDMF-DMIERA approach was applied to assess the PAHs dynamic ecological risk in the study area, simulated from1975-2020. The assessment results demonstrated that the highest environmental quality risk come from NAP and ANY, achieved by medium risk level of low-medium risk level. Combined the environmental quality risk assessment results and the PAH source apportionment, it was found that the environmental risks in this study mainly result from petroleum spills and coke oven, which are in accordance with the regional characteristic of the petrochemical industry base of China. Meanwhile, the dynamic multimedia human health risk of16PAHs was assessed during1985-2020, it was represented that the human health in the study area mainly from the human exposure to the soil compartment (>90%), including soil ingestion (35%), inhalation of soil particles (35%), and the skin exposure to the soil (25%). And the fuzzy rule base was constructed in order to characterize the PAHs dynamic multimedia integrated ecological risk level, the assessment results demonstrated that the "very high" ecological risk exists in NAP, BaA, CHR, BbF, BkF, BaP, IPY, and DBA, all possible measures should be taken to treat the ecological risk in the oilfield.
通过对研究区域多介质环境(大气、水、土壤、沉积物)建立稳态、动态及区间动态多介质逸度模型,研究陆地石油开采区PAHs多介质迁移转化、归趋及源解析等环境行为。研究结果表明,石油开采过程中产生的PAHs多以落地原油形式进入环境系统,并以土壤中降解为主要输出途径,土壤介质是PAHs的主要归宿。多介质环境中PAHs的苯环构成结构研究表明,空气相中多为大于4环的PAHs,水中多为2-3环PAHs,土壤中多为3环PAHs,沉积物中多为3-4环PAHs。基于本研究开发的区间动态多介质逸度模型,对1985-2010年间PAHs动态源解析结果表明,大气和土壤介质中PAHs的主要来源是高温燃烧,而水和沉积物介质中PAHs的主要来源是生物质和煤的燃烧。同时,随着陆地石油开采强度的不断增大,PAHs的来源逐渐倾向于石油源的释放。
研究表明,土壤介质是PAHs的主要归宿。因此,本研究应用主成分分析、人工神经网络等方法建立不同来源PAHs土壤发光菌生物毒性神经网络模型对土壤生物毒性进行源解析,并对不同来源PAHs对生物毒性的贡献进行定量表征。模型模拟结果显示,不同PAHs来源对土壤生物毒性的贡献分别为：交通源占13.2%、石油源占37.4%、煤燃烧占36.0%、焦油源占13.4%。此外,基于土壤介质实际采样测试分析结果,对土壤介质中PAHs的空间分布规律及污染等级进行评价,确定影响土壤PAHs污染等级的因素包括井场落地油情况、开采量、开采年限及其周边环境因素(植被状况、土壤类型等)等。计算得到研究区域内重污染、中污染及轻污染采样点分别占8.02%,8.02%和2.29%。
本研究以区间动态多介质逸度模型模拟结果为基础数据,结合模糊理论、概率分析等不确定性表征方法,通过构建模糊的环境质量标准和模糊的健康风险判定标准,构建基于区间动态多介质逸度模型的动态多介质生态风险评价方法框架,并利用所建方法对1985-2020年间研究区域内的PAHs进行动态多介质综合生态风险评价。评价结果显示,NAP和ANY具有最高的环境质量风险,均达到中等风险或低-中风险。进一步将环境质量风险评价结果与PAHs源解析相结合可以看出,本文研究区域中环境质量风险主要来自石油开采和焦炭。此外,1985-2020年间16种PAHs人体健康风险评价结果表明NAP和4环以上PAHs具有较高的人体健康风险,主要来自人体对土壤介质的暴露(>90%),包括土壤摄食(35%),吸入土壤颗粒(35%),皮肤接触土壤(25%)。最后,通过构建模糊规则库,对研究区域内PAHs综合生态风险水平进行表征,NAP、BaA、CHR、BbF、BkF、BaP、IPY和DBA具有“非常高”综合生态风险,应采取全部可能的措施来处理石油开采场地。
With the rapid development of national economy, serious contradiction between oil supply and demand would appear in the future, then China needs to use more onshore oil geological reserves to increase crude oil production, this must result in the petroleum exploitation area transfers to low permeability, low yield, and low abundance area, it must bring more cumulative pollution and worsening ecological risk. Thus, find out the oil pollution source and master the typical petroleum pollutant migration transformation rule and their ecological risk could provide scientific evidence for cleaner production and pollution management and control for petroleum exploitation pollution. The pollutants such as polycyclic aromatic hydrocarbon (PAHs) would enter into air, water, and soil compartment in the process of petroleum exploitation. However, the investigation focus more on the organic pollutant derived from petroleum exploitation in the individual environmental media such as water and soil, and lack of the multimedia environmental pollutant and risk assessment in the onshore oilfield. In this study, the multimedia transport, fate, and source apportionment of PAHs in the onshore oilfield were investigated, and then the spatial distribution and pollutant grade of PAHs in the soil compartment were studied to reveal the relationship between the soil luminescent bacteria biological toxicity and the pollutant sources, the dynamic multimedia integrated ecological risks of16PAHs were assessed in the study area, and the quantitative characterization method of uncertainty in the ecological risk was established.
The multimedia environmental transport, fate, and source apportionment of PAHs in onshore oilfield were investigated through the established steady-state, dynamic-state, and interval dynamic multimedia fugacity (IDMF) model, including air, water, soil, and sediment compartment. The modeling results showed that, the primarily input pathway of PAHs enter the multimedia environments is crude oil spills on the soil, while the output pathway was the degradation of PAHs in the soil compartment. Soil was identified as the dominate sink of PAHs. The ring size distribution indicated that compounds containing more than four rings were dominant in air, two-and three-ring compounds were prevalent in water, three ring compounds were mainly in soil, and four-ring compounds were predominant in sediment. The dynamic source apportionment was taken on basis of the constructed IDMF model, it was demonstrated that high temperature combustion was the major source of PAHs in the air and soil, while biomass and coal combustion were attributed to water and sediment compartments. Besides, the modeling results showed a tended to be from petroleum sources as evidenced by the accumulation effect of PAHs and continuous oil exploitation.
The previous result has showed that, soil compartment was the main sink of PAHs in the multimedia environments. Hence, the methods of principal component analysis (PC A) and artificial neural network (ANN) were applied to identify the sources of PAHs in the soil contaminants, and an ANN model was established to investigate the contribution of the PAHs to soil biotoxicity. The modeling results revealed that the contamination sources included traffic emissions (13.2%), petroleum-related source (37.4%), coal combustion (36.0%), and coke oven source (13.4%). Besides, spatial distribution and pollution grade of PAHs in the soils were analysised based on the actual sampling and analysis of the collected soils from the six oil wells in the study oilfield. Relevant effect factors of the concentrations level were concluded as condition of ground oil, exploitation scale, exploitation time, and surrounding environment (including vegetation condition, primitive soil types, etc.). Soil pollution grade of the six oil wells were also evaluated through the method of a modified Nemerow Index Method. The evaluation result showed that the percentages of heavy pollution, moderate pollution, and slight pollution were8.02%,8.02%, and2.29%, respectively.
Finally, the IDMF model assisted dynamic multimedia integrated ecological risk assessment (IDMF-DMIERA) approach framework was developed. The approach framework was on basis of the modeling results of IDMF model, combining with the uncertainty representation approaches of interval parameter, fuzzy theory, and probability analysis. And then the developed IDMF-DMIERA approach was applied to assess the PAHs dynamic ecological risk in the study area, simulated from1975-2020. The assessment results demonstrated that the highest environmental quality risk come from NAP and ANY, achieved by medium risk level of low-medium risk level. Combined the environmental quality risk assessment results and the PAH source apportionment, it was found that the environmental risks in this study mainly result from petroleum spills and coke oven, which are in accordance with the regional characteristic of the petrochemical industry base of China. Meanwhile, the dynamic multimedia human health risk of16PAHs was assessed during1985-2020, it was represented that the human health in the study area mainly from the human exposure to the soil compartment (>90%), including soil ingestion (35%), inhalation of soil particles (35%), and the skin exposure to the soil (25%). And the fuzzy rule base was constructed in order to characterize the PAHs dynamic multimedia integrated ecological risk level, the assessment results demonstrated that the "very high" ecological risk exists in NAP, BaA, CHR, BbF, BkF, BaP, IPY, and DBA, all possible measures should be taken to treat the ecological risk in the oilfield.
引文
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