Sensitivity of ozone to precursor emissions in urban Beijing with a Monte Carlo scheme

Abstract In order to understand the formation mechanisms of high surface ozone and identify the main contributor sources in Beijing, this study investigates the sensitivity of surface ozone to NO, NO 2 and nine types of NMVOC emissions during a photochemical smog episode. Monte Carlo sensitivity analysis scheme with fifty simulations is established based on the Nested Air Quality Prediction Model System (NAQPMS). At every simulation, each of the eleven precursor emissions is perturbed with a distinct set of perturbations. The sensitivities of ozone to emissions are identified by multiple linear regressions. The stability of sensitivity results is validated by two experiments with standard deviations of log-normal perturbations set as 30% and 50% respectively. The sensitivity results suggest that the current high surface ozone is strongly stimulated by NMVOC emissions. Among NMVOC emissions, formaldehyde, ethylene and olefins emissions present the greatest impacts on ozone. On the other hand, NOx emissions have a strong inhibitory effect on ozone formation, even after 50% NOx emission reduction. This indicates that the current ozone formation in Beijing is under NOx-saturated conditions. A transition of ozone formation is observed from NOx-saturated to NOx-limited sensitivity behavior with a 75% reduction of NOx emissions. This study gives the implication that abatement of the four NMVOC types mentioned above could be efficient on reducing the high levels of surface ozone in central urban Beijing, while inadequate abatement in NOx emissions probably induces reverse effects.

[1]  Hajime Akimoto,et al.  Modeling study of ozone seasonal cycle in lower troposphere over east Asia , 2007 .

[2]  A case study of emission changes and ozone responses , 1998 .

[3]  G. Carmichael,et al.  Asian emissions in 2006 for the NASA INTEX-B mission , 2009 .

[4]  H. Christopher Frey,et al.  Uncertainties in predicted ozone concentrations due to input uncertainties for the UAM-V photochemical grid model applied to the July 1995 OTAG domain , 2001 .

[5]  Yuanfang Liu,et al.  Distributions and Source Apportionment of Ambient Volatile Organic Compounds in Beijing City, China , 2005, Journal of environmental science and health. Part A, Toxic/hazardous substances & environmental engineering.

[6]  Min Shao,et al.  Volatile organic compounds measured in summer in Beijing and their role in ground‐level ozone formation , 2009 .

[7]  Min Shao,et al.  Source profiles of volatile organic compounds (VOCs) measured in China. Part I , 2008 .

[8]  K. Sudo,et al.  CHASER: A global chemical model of the troposphere 1. Model description , 2002 .

[9]  S. Sillman The relation between ozone, NOx and hydrocarbons in urban and polluted rural environments , 1999 .

[10]  Leonard K. Peters,et al.  A new lumped structure photochemical mechanism for large‐scale applications , 1999 .

[11]  Armistead G Russell,et al.  Nonlinear response of ozone to emissions: source apportionment and sensitivity analysis. , 2005, Environmental science & technology.

[12]  J. W. Munger,et al.  Ozone Air Quality During the 2008 Beijing Olympics: Effectiveness of Emission Restrictions , 2009 .

[13]  Zifa Wang,et al.  Why does surface ozone peak in summertime at Waliguan? , 2004 .

[14]  Li Jin-long The contribution of anthropogenic hydrocarbons to ozone formation in Beijing areas , 2002 .

[15]  Jeffrey M. Vukovich,et al.  Emission inventory development and processing for the Seasonal Model for Regional Air Quality (SMRAQ) project , 2000 .

[16]  V. Grewe,et al.  Technical Note: A diagnostic for ozone contributions of various NO x emissions in multi-decadal chemistry-climate model simulations , 2004 .

[17]  Armistead G Russell,et al.  High-order, direct sensitivity analysis of multidimensional air quality models. , 2003, Environmental science & technology.

[18]  M. Wesely Parameterization of surface resistances to gaseous dry deposition in regional-scale numerical models , 1989 .

[19]  Itsushi Uno,et al.  Neutralization of soil aerosol and its impact on the distribution of acid rain over east Asia: Observations and model results , 2002 .

[20]  L. Kleinman,et al.  Sensitivity of ozone production rate to ozone precursors , 2001 .

[21]  B. de Foy,et al.  Characterizing ozone production in the Mexico City Metropolitan Area: a case study using a chemical transport model , 2006 .

[22]  Yongtao Hu,et al.  Decoupled direct 3D sensitivity analysis for particulate matter (DDM-3D/PM) , 2006 .

[23]  Zifa Wang,et al.  Numerical Study of The Effect of Traffic Restriction on Air Quality in Beijing , 2010 .

[24]  T. Zhu,et al.  Measurement of NOy during Campaign of Air Quality Research in Beijing 2006 (CAREBeijing‐2006): Implications for the ozone production efficiency of NOx , 2009 .

[25]  Wang Xi,et al.  Development and Application of Nested Air Quality Prediction Modeling System , 2006 .

[26]  Z. Yuan,et al.  Source analysis of volatile organic compounds by positive matrix factorization in urban and rural environments in Beijing , 2009 .

[27]  Paulette Middleton,et al.  A three‐dimensional Eulerian acid deposition model: Physical concepts and formulation , 1987 .

[28]  C. Chan,et al.  Air pollution in mega cities in China , 2008 .

[29]  Binyu Wang,et al.  Air quality during the 2008 Beijing Olympic Games , 2007 .

[30]  S. Hanna,et al.  Monte carlo estimates of uncertainties in predictions by a photochemical grid model (UAM-IV) due to uncertainties in input variables , 1998 .

[31]  Chester W. Spicer,et al.  Ozone production efficiency and NOx depletion in an urban plume: Interpretation of field observations and implications for evaluating O3‐NOx‐VOC sensitivity , 2003 .

[32]  G. Grell,et al.  A description of the fifth-generation Penn State/NCAR Mesoscale Model (MM5) , 1994 .

[33]  Jiming Hao,et al.  Air quality impacts of power plant emissions in Beijing. , 2007, Environmental pollution.