Knowledge Resource Center for Ecological Environment in Arid Area
| 大气颗粒物长距离传输源的定量研究 | |
| 其他题名 | Quantification of Long-Range Transported Source Contributions to Airborne Fine Particulate Matters |
| REZA BASHIRI KHUZESTANI | |
| 出版年 | 2018 |
| 学位类型 | 博士 |
| 导师 | 张元勋 |
| 学位授予单位 | 中国科学院大学 |
| 中文摘要 | 大气中的细颗粒物(PM2.5)主要由污染源直接排放进入大气，或经大气光化学反应而二次生成，其化学组分十分复杂。人体短期或长期暴露于高浓度PM2.5环境下可能对呼吸系统造成不利的健康效应，从而增加相关疾病的发病率和死亡率。研究表明，大气中PM2.5浓度水平的升高可以诱发人体产生不利的健康效应，并导致能见度降低、气候变化及其他空气质量问题。通常，PM2.5的主要来源包括机动车尾气排放、生物质燃烧以及光化学反应二次生成等自然或人为来源。内蒙古鄂尔多斯地区的空气质量易受污染物长距离传输的影响，污染物来源有其独特的规律，因而对其空气质量的表征及其变化规律的探究具有十分重要的意义。为获得行之有效的大气污染控制对策，需要对研究区域大气中PM2.5的化学成分进行详细的表征，以及定量识别对空气质量影响较大的污染物来源并量化其影响程度。本研究采集了鄂尔多斯地区具有代表性的PM2.5样品并进行了相应的化学组分分析，利用优化后的受体模型解析出PM2.5的主要来源及其源贡献。鉴于有关内蒙古自治区大气PM2.5来源的研究较少，本研究利用CMB和PMF模型得到的结果正好为该领域提供了强有力的数据支持，能够为区域污染控制或本地源控制为主的环境管理模式探索新的道路。 近年来，有关中国大气污染的研究主要集中于大城市；然而，小城市的空气污染问题同样需要重视，特别是对于工业快速发展的地区，急需弄清其污染物的主要来源及时空变化。鄂尔多斯地区目前正处于经济和工业高速发展的过程中，面临着空气质量差，细颗粒物浓度水平超标等环境问题，污染物长距离传输对该地区的空气质量具有重要影响。初步分析表明, 鄂尔多斯地区PM2.5年平均浓度超过75 μg/m3，但本地源只占18 μg/m3 （23%）, 约60 μg/m3（77%）由区域传输贡献，仅本地源还不足以导致空气污染程度达到现有水平。本研究的目的主要在于对PM2.5的来源进行量化，并评估本地源的贡献以及区域传输对当地空气质量的影响。通过空间相关分析、双变量极坐标图表征以及后向轨迹模拟表明鄂尔多斯地区的PM2.5浓度主要受自治区外的远距离传输以及内蒙古西部沙漠地区沙尘的影响。总的来说，减少内蒙古自治区南部地区的污染输入可以在很大程度上改善鄂尔多斯地区的空气质量。 为判断污染过程中的主要污染来源及影响因子，我们将污染天和非污染天主要污染源的贡献进行比较分析，辨析出重要污染事件中的关键污染源，从而摸清主要污染月份中需要重点控制的污染来源。OC的源解析结果表明，污染事件发生时，工业/煤炭燃烧排放和机动车尾气排放对空气污染的贡献明显高于非污染天，而SOC、生物质燃烧和生物排放的贡献在污染天和非污染天之间并没有显著的差异。此外，双变量极坐标图和CWT图表征结果揭示出：工业燃煤排放和机动车尾气排放主要是长距离传输导致的，然而在污染事件发生时，这些源则大多来自本地。SOC、生物质燃烧和生物排放在污染天和非污染天的来源地相同，均来自远距离传输。 作为创新性尝试，我们研发出一种基于光学彩色空间传感方法而建立的新型颗粒物OC/EC测量方法。该方法结合了气溶胶光学特性、独立CIE-Lab色彩空间传感应用及多参数校准系统，并考虑了颗粒物中不同化学组分（水溶性离子和金属元素）对方法准确性的影响。和传统方法相比，该方法不仅可以测定石英膜上颗粒物OC/EC的含量，还可以应用于Teflon膜上OC/EC的测定。同时，我们初步证实了虽然有机物来源对光的吸收和散射有一定的影响，但对本研究中的OC/EC的测定结果影响不大。因此，该方法具有无损、低成本、高效率以及对Teflon独特的实用性等特点，可以广泛应用于大气环境化学和环境健康研究等领域。 |
| 英文摘要 | Fine particulate matter (PM2.5) is a complex mixture of chemical species originating from primary emission sources and secondary formation via photochemical reactions in the atmosphere. Acute and chronic human exposure to high-level PM2.5 can cause adverse respiratory health outcomes leading to increased morbidity and mortality rates. Increased airborne fine particulate matter (PM2.5) has been linked to adverse human health effects, reduced visibility, climate change, and other air quality concerns. Typically, the major contributors of PM2.5 include mobile source emissions, biomass burning, and secondary sources with anthropogenic and biogenic nature in origin. The Ordos region of the Inner Mongolia is of particular interest for air quality studies due to its unique characteristics in the regional long-range transport of air pollution. Effective control strategies for air pollutants require a detailed investigation of chemical composition of airborne PM2.5 in this area as well as quantitative identification of specific source impacts on ambient air quality. In this research, various airborne PM2.5 samples were collected and analyzed. Receptor models have been developed and applied to ambient PM2.5 chemical composition data in order to identify emission sources and quantify their contributions to ambient concentrations. However, little information is available to provide regional perspectives of PM2.5 sources in the Inner Mongolia Autonomous region. PM2.5 source apportionment conducted using hybrid receptor modeling provided such information. This can provide new insights about whether regionally or more locally targeted control strategies should be developed and applied for PM2.5 emission sources in the region. Recently, there have been several research studies on air pollution situation in China but mainly focused on metropolitan cities; however, comprehensive studies of the source identification as well as spatial and temporal variations of the air pollution situation in smaller cities, especially those recognized for their rapid industrial development need to be emphasized. The Ordos region of Inner Mongolia is rapidly developing and suffers from poor air quality and unhealthy levels of fine particulate matter. The area is a very unique site in case of the regional long-range transport of air pollution. Our preliminary analysis showed that the PM2.5 concentrations in the Ordos region exceeded 75 μg/m3 on the annual average, however, the local air pollution emissions from surrounding sources only accounted for 18 μg/m3 (23%) on average annual PM2.5 mass in the study area which seems not sufficient to drive pollution levels to its current concentrations. The analysis approved that approximately 77% of PM2.5 mass is transported long-range from the sites exterior to the study area and contributes approximately 60 μg/m3 on average annual PM2.5 mass. The present analysis was designed to quantify sources of PM2.5 and assess the local source contributions and the impact of regional transport on local pollution. The Spatial correlation analysis, bivariate polar plots and hybrid trajectory models illustrated that the Ordos region is mainly impacted by regional long-range transport from the sources located outside of the Inner Mongolia autonomous region, and the regional dust transported from the deserts located in western Inner Mongolia. Overall, the results suggested that the improvements in air quality in the Ordos region can be largely achieved by reducing emissions in the external sources located in the southern regions of the Inner Mongolia, China.In order to determine the key sources of PM2.5 contributing to the pollution episodes in the study area, the main sources of PM2.5 OC during elevated PM episodes were analyzed and compared with non-polluted days. This will provide significant insight to the main sources of particulate matter pollution during the high pollution episodes and the effective seasonal strategies to control sources of particulate matter during months and with the highest PM concentrations that need to be controlled. The source contributions to OC demonstrated that the Industrial/coal combustion and mobile source factors showed greater contributions to the elevated concentrations during the episode. The spatial analysis of SOC factors, biomass burning and biogenic sources did not show significant difference in the pollution episodes and the non-polluted months. In addition, the bivariate polar plots and CWT maps the Industrial coal combustion and mobile illustrated regional long-range transport patterns from the sources external to the study area, however, local adjacent areas were mostly controlling the contributions of these factors during the PM elevated episodes. The SOC sources, biomass burning and biogenic sources illustrated a regional long-range transport with similar locations found during the elevated pollution episodes compared to the normal situations.As an initial attempt, we also developed a new optical color space sensing method and a multi-parameter reference calibration system to estimate the OC and EC loadings collected on Teflon and quartz filters with the measurement of the aerosols optical properties and the independent CIE-Lab color space sensing of the quartz and Teflon filter loadings. We also explore the effects of the mixing state of PM composition in OC/EC model uncertainty. In addition, our analysis begins to illustrate that the sources of OC may also contribute and impact the absorption and scattering of light, which may be exploited in future method developments but is not a large impact in the current analysis of OC and EC. Finally, the non-destructive nature, low analytical cost, and specific coefficients of our new method in estimating OC/EC on Teflon filters will provide significant opportunities, in developing regions and large scale monitoring programs in occupational exposure testing and health studies. |
| 中文关键词 | “PMF模型” ; “CMB模型” ; “鄂尔多斯地区” ; “长距离传输” |
| 英文关键词 | \PMF\ \CMB\ \Ordos region\ \Long-range transport\ |
| 语种 | 中文 |
| 国家 | 中国 |
| 来源学科分类 | 环境科学 |
| 来源机构 | 中国科学院大学 |
| 资源类型 | 学位论文 |
| 条目标识符 | http://119.78.100.177/qdio/handle/2XILL650/288223 |
| 推荐引用方式 GB/T 7714 | REZA BASHIRI KHUZESTANI. 大气颗粒物长距离传输源的定量研究[D]. 中国科学院大学,2018. |
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