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中国特大城市(上海)臭氧的长期变化趋势:特征、成因及其与前体物的相互作用。

Long-term trend of O in a mega City (Shanghai), China: Characteristics, causes, and interactions with precursors.

机构信息

Shanghai Key Laboratory of Meteorology and Health, Shanghai 200030, China; Shanghai Meteorological Service, Shanghai 200030, China.

Shanghai Key Laboratory of Meteorology and Health, Shanghai 200030, China; Key Laboratory of Aerosol Science and Technology, SKLLQG, Institute of Earth Environment, Chinese Academy of Sciences, Xi'an, China; CAS Center for Excellence in Regional Atmospheric Environment, Chinese Academy of Sciences, Xiamen 361021, China; National Center for Atmospheric Research (NCAR), Boulder 80303, USA.

出版信息

Sci Total Environ. 2017 Dec 15;603-604:425-433. doi: 10.1016/j.scitotenv.2017.06.099. Epub 2017 Jun 23.

Abstract

In recent years, ozone (O) is often the major pollutant during summertime in China. In order to better understand this problem, a long-term measurement of ozone (from 2006 to 2015) and its precursors (NO and VOCs) as well as the photochemical parameter (UV radiation) in a mega city of China (Shanghai) is analyzed. The focus of this study is to investigate the trend of O and the causes of the O trend in large cities in China. In order to understand the relationship between the O precursors and O formation, two distinguished different sites of measurements are selected in the study, including an urbanization site (XJH-Xujiahui) and a remote site (DT-Dongtan). At the XJH site, there are high local emissions of ozone precursors (such as VOCs and NO), which is suitable to study the effect of O precursors on O formation. In contrast, at the DT site, where there are low local emissions, the measured result can be used to analyze the background conditions nearby the city of Shanghai. The analysis shows that there were long-term trends of O and NO concentrations at the urban site (XJH) from 2006 to 2015 (O increasing 67% and NO decreasing 38%), while there were very small trends of O and NO concentrations at the background site (DT). The analysis for causing the O trend suggests that (1) the large O increase at the urban area (XJH) was not due to the regional transport of O; (2) the measurement of solar radiation had not significant trend during the period, and was not the major cause for the long-term O trend; (3) the measurement of VOCs had small change during the same period, suggesting that the trend in NO concentrations at the urban site (XJH) was a major factor for causing the long-term change of O at the urban area of Shanghai. As a result, the O and NO concentrations from 2006 to 2015 at the urban area of Shanghai were strongly anti-correlated, suggesting that the extremely high NO concentration in the urban area depressed the O concentrations. It is interesting to note that the anti-correlation between O and NO was in an un-linearly relationship. Under high O concentration condition, the ratio of Δ[O]/Δ[NO] was as large as -1.5. In contrast, under low O concentrations, the ratio of Δ[O]/Δ[NO] was only -0.2. This result suggested that when O concentration was high, it was more sensitive to NO concentration, while when O concentration was low, it was less sensitive to NO concentration. This study provides useful insights for better understanding the causes of the long-term-trend of regional O pollution nearby Shanghai, and has important implication for air pollution control in large cities in China. Due to the fact that NO and VOCs are not only precursors for O, but also are important precursors for particular matter (PM). If reduction of NO leads to decrease in PM, but increase in O, the NO emission control become a very complicated issue and need to carefully design a comprehensive control method.

摘要

近年来,臭氧(O)在中国夏季通常是主要污染物。为了更好地了解这个问题,我们对中国一个特大城市(上海)的臭氧(从 2006 年到 2015 年)及其前体物(NO 和 VOCs)以及光化学反应参数(UV 辐射)进行了长期测量。本研究的重点是研究 O 的趋势以及中国大城市 O 趋势的原因。为了了解 O 前体物与 O 形成之间的关系,我们在研究中选择了两个具有不同特征的测量地点,包括一个城市化地区(XJH-徐家汇)和一个偏远地区(DT-东滩)。在 XJH 站点,臭氧前体物(如 VOCs 和 NO)的本地排放很高,适合研究 O 前体物对 O 形成的影响。相比之下,在 DT 站点,本地排放很低,测量结果可用于分析上海市区附近的背景条件。分析表明,2006 年至 2015 年,城市化地区(XJH)的 O 和 NO 浓度存在长期趋势(O 增加 67%,NO 减少 38%),而背景地区(DT)的 O 和 NO 浓度几乎没有变化。造成 O 趋势的原因分析表明:(1)城市地区(XJH)的 O 大量增加并非是由于 O 的区域输送造成的;(2)测量期间太阳辐射没有明显的趋势,也不是造成长期 O 趋势的主要原因;(3)同一时期 VOCs 的测量值变化很小,这表明城市化地区(XJH)NO 浓度的变化是造成上海市区 O 长期变化的主要因素。因此,2006 年至 2015 年上海市区的 O 和 NO 浓度呈强烈的负相关关系,表明城市地区极高的 NO 浓度抑制了 O 的浓度。有趣的是,O 和 NO 的相关性呈非线性关系。在高 O 浓度条件下,Δ[O]/Δ[NO]的比值高达-1.5。相比之下,在低 O 浓度下,Δ[O]/Δ[NO]的比值仅为-0.2。这一结果表明,当 O 浓度较高时,它对 NO 浓度更敏感,而当 O 浓度较低时,它对 NO 浓度的敏感度较低。本研究为更好地了解上海地区 O 污染长期趋势的原因提供了有用的见解,并对中国大城市的空气污染控制具有重要意义。由于 NO 和 VOCs 不仅是 O 的前体物,也是细颗粒物(PM)的重要前体物。如果减少 NO 会导致 PM 减少,而 O 增加,那么 NO 排放控制就会成为一个非常复杂的问题,需要仔细设计一种综合的控制方法。

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