Harvard-NUIST Joint Laboratory for Air Quality and Climate, Nanjing University of Information Science and Technology, 210044 Nanjing, China.
John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA 02138.
Proc Natl Acad Sci U S A. 2019 Jan 8;116(2):422-427. doi: 10.1073/pnas.1812168116. Epub 2018 Dec 31.
Observations of surface ozone available from ∼1,000 sites across China for the past 5 years (2013-2017) show severe summertime pollution and regionally variable trends. We resolve the effect of meteorological variability on the ozone trends by using a multiple linear regression model. The residual of this regression shows increasing ozone trends of 1-3 ppbv a in megacity clusters of eastern China that we attribute to changes in anthropogenic emissions. By contrast, ozone decreased in some areas of southern China. Anthropogenic NO emissions in China are estimated to have decreased by 21% during 2013-2017, whereas volatile organic compounds (VOCs) emissions changed little. Decreasing NO would increase ozone under the VOC-limited conditions thought to prevail in urban China while decreasing ozone under rural NO-limited conditions. However, simulations with the Goddard Earth Observing System Chemical Transport Model (GEOS-Chem) indicate that a more important factor for ozone trends in the North China Plain is the ∼40% decrease of fine particulate matter (PM) over the 2013-2017 period, slowing down the aerosol sink of hydroperoxy (HO) radicals and thus stimulating ozone production.
过去 5 年(2013-2017 年)在中国约 1000 个站点获得的近地面臭氧观测结果表明,夏季污染严重且存在区域性变化趋势。我们通过使用多元线性回归模型解决了气象变化对臭氧趋势的影响。该回归的残差表明,中国东部大城市群的臭氧呈 1-3 ppbv/a 的上升趋势,我们认为这归因于人为排放的变化。相比之下,中国南方的一些地区的臭氧呈下降趋势。据估计,2013-2017 年期间中国的人为氮排放减少了 21%,而挥发性有机化合物(VOCs)的排放变化不大。在认为中国城市普遍存在 VOC 限制条件下,减少 NO 将增加臭氧,而在农村 NO 限制条件下,减少臭氧。然而,使用戈达德地球观测系统化学输送模型(GEOS-Chem)的模拟表明,对华北平原臭氧趋势更为重要的因素是 2013-2017 年间细颗粒物(PM)减少了约 40%,这减缓了过氧(HO)自由基的气溶胶清除作用,从而刺激了臭氧的产生。