Abstract

Abstract. China is facing a severe ozone problem, but the origin of its ozone remains unclear. Here we use a GEOS-Chem based global–regional two-way coupled model system to quantify the individual contributions of eight emission source regions worldwide to springtime ozone in 2008 over China. The model reproduces the observed ozone from 31 ground sites and various aircraft and ozonesonde measurements in China and nearby countries, with a mean bias of 10 %–15 % both near the surface and in the troposphere. We then combine zero-out simulations, tagged ozone simulations, and a linear weighting approach to account for the effect of nonlinear chemistry on ozone source attribution. We find considerable contributions of total foreign anthropogenic emissions to surface ozone over China (2–11 ppb). For ozone of anthropogenic origin averaged over China, foreign regions together contribute 40 %–60 % below the height of 2 km and 85 % in the upper troposphere. For total ozone contributed by foreign anthropogenic emissions over China at various heights, the portion of transboundary ozone produced within foreign emission source regions is less than 50 %, with the rest produced by precursors transported out of those source regions. Japan and Korea contribute 0.6–2.1 ppb of surface ozone over the east coastal regions. Southeast Asia contributes 1–5 ppb over much of southern China and South Asia contributes up to 5–10 ppb of surface ozone over the border of southwestern China; and their contributions increase with height due to strong upwelling over the source regions. The European contribution reaches 2.1–3.0 ppb for surface ozone over the northern border of China and 1.5 ppb in the lower troposphere averaged over China. North America contributes 0.9–2.7 ppb of surface ozone over most of China (1.5–2.1 ppb over the North China Plain), with a China average at 1.5–2.5 ppb at different heights below 8 km, due to its large anthropogenic emissions and the transport-favorable midlatitude westerly wind. In addition to domestic emission control, global emission reduction is critical for China's ozone mitigation.

Highlights

  • Ozone is an important atmospheric oxidant and the primary source of the hydroxyl radical (OH)

  • The severe ozone problem is largely associated with growth in anthropogenic emissions of nitrogen oxides (NOx) and non-methane volatile organic compounds (NMVOCs)

  • Chinese anthropogenic NOx emissions increased at a rate of 7.9 % yr−1 from 2000 to 2010 (Zhao et al, 2013), and Chinese anthropogenic NMVOC emissions increased from 22.45 Tg in 2008 to 29.85 Tg in 2012 (Wu et al, 2016)

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Summary

Introduction

Ozone is an important atmospheric oxidant and the primary source of the hydroxyl radical (OH). Wang et al (2011) used tagged ozone simulations with GEOS-Chem to study the global production of surface ozone over China for 2006. They showed that in spring 2006, tropospheric ozone produced over India contributed up to 6 ppb to surface ozone over western China and that ozone produced over Europe and North America each contributed 2–5 ppb of ozone over northeastern China and North China.

Two-way coupled GEOS-Chem modeling system
Surface measurements
Measurements of vertical profiles
Model evaluation
Surface ozone and CO over China and nearby countries
Vertical profiles of ozone and CO
Summarizing remark on model evaluation
Source attribution modeling for surface ozone over China
Domestic versus foreign anthropogenic contributions to ozone
Vertical distributions of domestic and foreign anthropogenic contributions
Findings
Conclusions

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