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Volatile organic compound emissions from unconventional natural gas production: Source signatures and air quality impacts.

机译:非常规天然气生产中挥发性有机化合物的排放:排放源特征和空气质量影响。

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摘要

Advances in horizontal drilling and hydraulic fracturing over the past two decades have allowed access to previously unrecoverable reservoirs of natural gas and led to an increase in natural gas production. Intensive unconventional natural gas extraction has led to concerns about impacts on air quality. Unconventional natural gas production has the potential to emit vast quantities of volatile organic compounds (VOCs) into the atmosphere. Many VOCs can be toxic, can produce ground-level ozone or secondary organic aerosols, and can impact climate. This dissertation presents the results of experiments designed to validate VOC measurement techniques, to quantify VOC emission rates from natural gas sources, to identify source signatures specific to natural gas emissions, and to quantify the impacts of these emissions on potential ozone formation and human health. Measurement campaigns were conducted in two natural gas production regions: the Denver-Julesburg Basin in northeast Colorado and the Marcellus Shale region surrounding Pittsburgh, Pennsylvania. An informal measurement intercomparison validated the canister sampling methodology used throughout this dissertation for the measurement of oxygenated VOCs. Mixing ratios of many VOCs measured during both campaigns were similar to or higher than those observed in polluted cities. Fluxes of natural gas-associated VOCs in Colorado ranged from 1.5-3 times industry estimates. Similar emission ratios relative to propane were observed for C2-C6 alkanes in both regions, and an isopentane:n-pentane ratio ≈1 was identified as a unique tracer for natural gas emissions. Source apportionment estimates indicated that natural gas emissions were responsible for the majority of C2-C8 alkanes observed in each region, but accounted for a small proportion of alkenes and aromatic compounds. Natural gas emissions in both regions accounted for approximately 20% of hydroxyl radical reactivity, which could hinder federal ozone standard compliance in downwind cities. A health risk assessment showed no increase in cancer or chronic non-cancer risk at locations near natural gas wells in Pennsylvania, but the contribution of natural gas emissions to total risk was 3-6 times higher near wells. These results will assist policy makers, natural gas producers, and citizen stakeholders in crafting effective policies to control VOC emissions from natural gas production activities.
机译:在过去的二十年中,水平钻井和水力压裂技术的进步使人们能够进入以前无法开采的天然气储层,并导致天然气产量的增加。密集的非常规天然气开采已引起人们对空气质量影响的担忧。非常规天然气生产有可能向大气排放大量挥发性有机化合物(VOC)。许多挥发性有机化合物可能有毒,会产生地面臭氧或二次有机气溶胶,并会影响气候。本文介绍了旨在验证VOC测量技术,量化天然气来源的VOC排放率,识别特定于天然气排放的来源特征以及量化这些排放对潜在臭氧形成和人体健康的影响的实验结果。在两个天然气生产地区进行了测量活动:科罗拉多州东北部的丹佛-朱尔斯堡盆地和宾夕法尼亚州匹兹堡周围的马塞勒斯页岩地区。非正式的测量比对验证了整个论文中用于测量含氧VOC的罐采样方法。两次活动期间测得的许多VOC的混合比率均与受污染城市中观察到的比率相似或更高。科罗拉多州与天然气相关的挥发性有机化合物的通量范围是行业估计的1.5至3倍。在两个区域中,对于C 2 -C 6烷烃,观察到相对于丙烷的相似排放比,并且异戊烷:正戊烷比≈ 1被确定为天然气排放的唯一示踪剂。气源分配估算表明,天然气排放是每个地区观察到的大部分C2-C8烷烃的来源,但占烯烃和芳族化合物的一小部分。两个地区的天然气排放量约占羟基自由基反应性的20%,这可能会阻碍顺风城市的联邦臭氧标准达标。健康风险评估显示,宾夕法尼亚州天然气井附近的位置癌症或慢性非癌症风险没有增加,但天然气排放对总风险的贡献是井附近的3-6倍。这些结果将帮助决策者,天然气生产商和公民利益相关者制定有效的政策,以控制天然气生产活动中的VOC排放。

著录项

  • 作者

    Swarthout, Robert F.;

  • 作者单位

    University of New Hampshire.;

  • 授予单位 University of New Hampshire.;
  • 学科 Atmospheric Chemistry.;Atmospheric Sciences.;Environmental Sciences.
  • 学位 Ph.D.
  • 年度 2014
  • 页码 172 p.
  • 总页数 172
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

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