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© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.

Submitted as: research article 06 May 2019

Submitted as: research article | 06 May 2019

Review status
This discussion paper is a preprint. It is a manuscript under review for the journal Atmospheric Chemistry and Physics (ACP).

Evaluation and uncertainty investigation of the NO2, CO and NH3 modeling over China under the framework of MICS-Asia III

Lei Kong1,3, Xiao Tang2,3, Jiang Zhu1,3, Zifa Wang2,3, Joshua S. Fu4, Xuemei Wang5, Syuichi Itahashi6,7, Kazuyo Yamaji8, Tatsuya Nagashima9, Hyo-Jung Lee10, Cheol-Hee Kim10, Chuan-Yao Lin11, Lei Chen2,3, Meigen Zhang2,3, Zhining Tao12,13, Jie Li2,3, Mizuo Kajino14,15, Hong Liao16, Kengo Sudo17, Yuesi Wang2,3, Yuepeng Pan2,3, Guiqian Tang2,3, Meng Li18,19, Qizhong Wu20,21, Baozhu Ge2,3, and Gregory R. Carmichael22 Lei Kong et al.
  • 1ICCES,Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing, 100029, China
  • 2LAPC, Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing, 100029, China
  • 3University of Chinese Academy of Sciences, Beijing, 100049, China
  • 4Department of Civil and Environmental Engineering, University of Tennessee, Knoxville, TN, 37996, USA
  • 5Institite for Environment and Climate Research, Jinan University, Guangzhou, 510632, China
  • 6Central Research Institute of Electric Power Industry, Abiko, Chiba, 270-1194, Japan
  • 7Department of Marine, Earth, and Atmospheric Sciences, North Carolina State University, Raleigh, NC 27607, USA
  • 8Graduate School of Maritime Sciences, Kobe University, Kobe, Hyogo 658-0022, Japan
  • 9National Institute for Environmental Studies, Onogawa, Tsukuba 305-8506, Japan
  • 10Department of Atmospheric Sciences, Pusan National University, Busan, 46241, South Korea
  • 11Research Center for Environmental Changes, Academia Sinica, Taipei, 115, Taiwan
  • 12Universities Space Research Association, Columbia, MD, USA
  • 13NASA Goddard Space Flight Center, Greenbelt, MD, 130, USA
  • 14Meteorological Research Institute, Japan Meteorological Agency, Tsukuba, Ibaraki, 305-0052, Japan
  • 15Faculty of Life and Environmental Sciences, University of Tsukuba, Tsukuba, Ibaraki, 305-8577, Japan
  • 16School of Environmental Science and Engineering, Nanjing University of Information Science & Technology, Nanjing 210044, China
  • 17Graduate School of Environmental Studies, Nagoya University, Nagoya, Japan
  • 18Ministry of Education Key laboratory for Earth System Modeling, Department of Earth System Science, Tsinghua University, Beijing, 100084, China
  • 19Multiphase Chemistry Department, Max Planck Institute for Chemistry, Mainz, 55128, Germany
  • 20College of Global Change and Earth System Science, Beijing Normal University, Beijing 100875, China
  • 21Joint Centre for Global Changes Studies, Beijing Normal University, Beijing 100875, China
  • 22Center for Global and Regional Environmental Research, University of Iowa, Iowa City, IA, 52242, USA

Abstract. Despite significant progress in improving chemical transport models (CTMs), applications of these modeling endeavours are still subject to the large and complex model uncertainty. Model Inter-Comparison Study for Asia III (MICS-Asia III) provides the opportunity to assess the capability and uncertainty of current CTMs in East Asia applications. In this study, we evaluated the multi-model simulations of nitrogen dioxide (NO2), carbon monoxide (CO) and ammonia (NH3) over China under the framework of MICS-Asia III. Compared with MICS-Asia II, modeling results were provided by a larger number of independent groups from different countries/regions and covered a longer period of time (one-full year). Furthermore, most of these groups used a common emission inventory, common meteorological inputs, and the same modeling domain and horizontal resolutions. New observations over North China Plain (NCP) and Peral River Delta (PRD) were also available in MICS-Asia III, allowing model evaluations over highly industrialized regions. The results show that most models well captured the monthly and spatial patterns of NO2 in NCP though NO2 levels were slightly underestimated. Relatively poor performance in NO2 simulations was found in PRD with larger root mean square error and lower spatial correlation coefficients, possibly due to the relative coarse model resolutions. All models significantly underpredicted CO concentrations both in NCP and PRD, with annual mean concentrations 65.4 % and 61.4 % underestimated by the ensemble mean respectively. Such large underestimations suggest that CO emissions might be underestimated in current emission inventory. In contrast to the good skills in simulating the monthly variations of NO2 and CO concentrations, all models failed to reproduce the observed monthly variations of NH3 concentrations in NCP. Most models mismatched the observed peak in July and showed negative correlation coefficients with observations, which may be closely related to the uncertainty in the monthly variations of NH3 emissions and the NH3 gas-aerosol partitioning. Finally, inter-comparisons of these model results were conducted to quantify the impacts of model uncertainty on the simulations of these gases, which are shown increase with the reactivity of species. Models contained more uncertainty in the NH3 simulations. This suggests that for some highly active and/or short-lived primary pollutants, like NH3, model uncertainty can also take a great part in the forecast uncertainty in addition to the emission uncertainty. Based on these results, some recommendations are made for future studies.

Lei Kong et al.
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Short summary
Evaluation and uncertainty investigation of NO2, CO and NH3 modeling over China were conducted in this study using 14 CTM results from MICS-Asia III. All models largely underestimated CO concentrations and showed very poor performance in reproducing the observed monthly variations of NH3 concentrations. Potential factors related to such deficiencies were investigated and discussed in this manuscript.
Evaluation and uncertainty investigation of NO2, CO and NH3 modeling over China were conducted...