Measurement and model analyses of the ozone variation during 2006 to 2015 and its response to emission change in megacity Shanghai, China

Abstract

The fine particles (PM 2.5) in China have decreased significantly in recent years as a result of the implementation of Chinese Clean Air Action Plan since 2013, while the O3 pollution is getting worse, especially in megacities such as Beijing and Shanghai. Better understanding of the elevated O3 pollution in Chinese megacities and its response to emission change is important for developing an effective emission control strategy in the future. In this study, we analyze the significant increasing trend of daily maximum O3 concentration from 2006 to 2015 in the megacity Shanghai with the variability of 0.8-1.3 ppbv yr -1. It could likely be attributed to the notable reduction in NO x concentrations with the decreasing rate of 1.86-2.15 ppbv yr -1 accompanied by the small change in VOCs during the same period by excluding the weak trends of meteorological impacts on local dispersion (wind speed), regional transport (wind direction), and O3 photolysis (solar radiation). It is further illustrated by using a state-of-the-art regional chemical and dynamical model (WRF-Chem) to explore the O3 variation response to the reduction in NO x emissions in Shanghai. The control experiment conducted for September of 2009 shows excellent performance for O3 and NO x simulations, including both the spatial distribution pattern and the day-by-day variation through comparison with six in situ measurements from the MIRAGE-Shanghai field campaign. Sensitivity experiments with 30 % reduction in NO x emissions from 2009 to 2015 in Shanghai estimated by Shanghai Environmental Monitoring Center shows that the calculated O3 concentrations exhibit obvious enhancement by 4-7 ppbv in urban zones with increasing variability of 0.96-1.06 ppbv yr -1, which is consistent with the observed O3 trend as a result of the strong VOC-limited condition for O3 production. The large reduction in NO x combined with less change in VOCs in the past 10 years promotes the O3 production in Shanghai to move towards an NO x -limited regime. Further analysis of the WRF-Chem experiments and O3 isopleth diagram suggests that the O3 production downtown is still under a VOC-limited regime after 2015 despite the remarkable NO x reduction, while it moves to the transition regime between NO x -limited and VOC-limited in sub-urban zones. Supposing the insignificant VOC variation persists, the O3 concentration downtown would keep increasing until 2020 with the further 20 % reduction in NO x emission after 2015 estimated by Shanghai Clean Air Action Plan. The O3 production in Shanghai will switch from a VOC-limited to an NO x -limited regime after 2020 except for downtown area, which is likely close to the transition regime. As a result the O3 concentration will decrease by 2-3 ppbv in sub-urban zones and by more than 4 ppbv in rural areas as a response to a 20 % reduction in NO x emission after 2020, whereas it is not sensitive to both NO x and VOC changes downtown. This result reveals that the control strategy of O3 pollution is a very complex process and needs to be carefully studied.