scholarly journals Simulation of the interannual variations of aerosols in China: role of variations in meteorological parameters

2014 ◽  
Vol 14 (18) ◽  
pp. 9597-9612 ◽  
Author(s):  
Q. Mu ◽  
H. Liao
Keyword(s):  
Organic Carbon ◽  
Meteorological Parameters ◽  
Transport Model ◽  
Southern China ◽  
Control Strategies ◽  
Specific Humidity ◽  
Anthropogenic Emissions ◽  
Interannual Variations ◽  
Chemical Transport Model

Abstract. We used the nested grid version of the global three-dimensional Goddard Earth Observing System chemical transport model (GEOS-Chem) to examine the interannual variations (IAVs) of aerosols over heavily polluted regions in China for years 2004–2012. The role of variations in meteorological parameters was quantified by a simulation with fixed anthropogenic emissions at year 2006 levels and changes in meteorological parameters over 2004–2012. Simulated PM2.5 (particles with a diameter of 2.5 μm or less) aerosol concentrations exhibited large IAVs in North China (NC; 32–42° N, 110–120° E), with regionally averaged absolute percent departure from the mean (APDM) values of 17, 14, 14, and 11% in December-January-February (DJF), March-April-May (MAM), June-July-August (JJA), and September-October-November (SON), respectively. Over South China (SC; 22–32° N, 110–120° E), the IAVs in PM2.5 were found to be the largest in JJA, with the regional mean APDM values of 14% in JJA and of about 9% in other seasons. The concentrations of PM2.5 over the Sichuan Basin (SCB; 27–33° N, 102–110° E) were simulated to have the smallest IAVs among the polluted regions examined in this work, with APDM values of 8–9% in all seasons. All aerosol species (sulfate, nitrate, ammonium, black carbon, and organic carbon) were simulated to have the largest IAVs over NC in DJF, corresponding to the large variations in meteorological parameters over NC in this season. Process analyses were performed to identify the key meteorological parameters that determined the IAVs of different aerosol species in different regions. While the variations in temperature and specific humidity, which influenced the gas-phase formation of sulfate, jointly determined the IAVs of sulfate over NC in both DJF and JJA, wind (or convergence of wind) in DJF and precipitation in JJA were the dominant meteorological factors to influence IAVs of sulfate over SC and the SCB. The IAVs in temperature and specific humidity influenced gas-to-aerosol partitioning, which were the major factors that led to the IAVs of nitrate aerosol in China. The IAVs in wind and precipitation were found to drive the IAVs of organic carbon aerosol. We also compared the IAVs of aerosols simulated with variations in meteorological parameters alone with those simulated with variations in anthropogenic emissions alone; the variations in meteorological fields were found to dominate the IAVs of aerosols in northern and southern China over 2004–2012. Considering that the IAVs in meteorological fields are mainly associated with natural variability in the climate system, the IAVs in aerosol concentrations driven by meteorological parameters have important implications for the effectiveness of short-term air quality control strategies in China.

scholarly journals Simulation of the interannual variations of aerosols in China: role of variations in meteorological parameters

2014 ◽  
Vol 14 (8) ◽  
pp. 11177-11219 ◽  
Author(s):  
Q. Mu ◽  
H. Liao
Keyword(s):  
Organic Carbon ◽  
Meteorological Parameters ◽  
Transport Model ◽  
Three Dimensional ◽  
Specific Humidity ◽  
Anthropogenic Emissions ◽  
Interannual Variations ◽  
Chemical Transport Model ◽  
June July

Abstract. We used the nested grid version of the global three-dimensional Goddard Earth Observing System chemical transport model (GEOS-Chem) to examine the interannual variations (IAVs) of aerosols over heavily polluted regions in China for years 2004–2012. The role of variations in meteorological parameters was quantified by a simulation with fixed anthropogenic emissions at year 2006 levels and changes in meteorological parameters over 2004–2012. Simulated PM2.5 (particles with a diameter of 2.5 μm or less) aerosol concentrations exhibited large IAVs in North China (NC, 32–42° N, 110–120° E), with regionally averaged absolute percent departure from the mean (APDM) values of 17, 14, 14, and 11% in December-January-February (DJF), March-April-May (MAM), June-July-August (JJA), and September-October-November (SON), respectively. Over South China (SC, 22–32° N, 110–120° E), the IAVs in PM2.5 were found to be the largest in JJA, with the regional mean APDM values of 14% in JJA and of about 9% in other seasons. Concentrations of PM2.5 over the Sichuan Basin (SCB, 27–33° N, 102–110° E) were simulated to have the smallest IAVs among the polluted regions examined in this work, with the APDM values of 8–9% in all seasons. All aerosol species (sulfate, nitrate, ammonium, black carbon, and organic carbon) were simulated to have the largest IAVs over NC in DJF, corresponding to the large variations in meteorological parameters over NC in this season. Process analyses were performed to identify the key meteorological parameters that determined the IAVs of different aerosol species in different regions. While the variations in temperature and specific humidity, which influenced the gas-phase formation of sulfate, jointly determined the IAVs of sulfate over NC in both DJF and JJA, wind (or convergence of wind) in DJF and precipitation in JJA were the dominant meteorological factors to influence IAVs of sulfate over SC and the SCB. The IAVs in temperature and specific humidity influenced gas-to-aerosol partitioning, which were the major factors that led to the IAVs of nitrate aerosol in China. The IAVs in wind and precipitation were found to drive the IAVs of organic carbon aerosol. We also compared the IAVs of aerosols simulated with variations in meteorological parameters alone with those simulated with variations in both meteorological parameters and anthropogenic emissions; the variations in meteorological fields were found to dominate the IAVs of aerosols in China.

scholarly journals Severe winter haze days in the Beijing–Tianjin–Hebei region from 1985 to 2017 and the roles of anthropogenic emissions and meteorology

2019 ◽  
Vol 19 (16) ◽  
pp. 10801-10816 ◽  
Author(s):  
Ruijun Dang ◽  
Hong Liao
Keyword(s):  
Meteorological Parameters ◽  
Transport Model ◽  
Process Analysis ◽  
Dominant Role ◽  
Anthropogenic Emissions ◽  
Steady Increase ◽  
Severe Winter ◽  
Chemical Transport Model ◽  
Haze Days ◽  
Pm2.5 Concentration

Abstract. We applied a global 3-D chemical transport model (GEOS-Chem) to examine the variations in the frequency and intensity in severe winter haze days (SWHDs) in Beijing–Tianjin–Hebei (BTH) from 1985 to 2017 and quantified the roles of changes in anthropogenic emissions and/or meteorological parameters. Observed SWHDs were defined as the days with daily mean PM2.5 concentration exceeding 150 µg m−3, and simulated SWHDs were identified by using the same threshold but with adjustment on the basis of simulation biases. Comparisons between the simulated SWHDs and those obtained from the observed PM2.5 concentrations and atmospheric visibility showed that the model can capture the spatial and temporal variations in SWHDs in China; the correlation coefficient between the simulated and observed SWHDs is 0.98 at 161 grids in China. From 1985 to 2017, with changes in both anthropogenic emissions and meteorological parameters, the simulated frequency (total severe haze days in winter) and intensity (PM2.5 concentration averaged over severe haze days in winter) of SWHDs in BTH showed increasing trends of 4.5 d per decade and 13.5 µg m−3 per decade, respectively. The simulated frequency exhibited fluctuations from 1985 to 2017, with a sudden decrease from 1992 to 2001 (29 to 10 d) and a rapid growth from 2003 to 2012 (16 to 47 d). The sensitivity simulations indicated that variations in meteorological parameters played a dominant role during 1992–2001, while variations in both emissions and meteorological parameters were important for the simulated frequency trend during 2003–2012 (simulated trends were 27.3 and 12.5 d per decade owing to changes in emissions alone and changes in meteorology alone, respectively). The simulated intensity showed a steady increase from 1985 to 2017, which was driven by changes in both emissions and meteorology. Process analysis on all SWHDs during 1985–2017 indicated that transport was the most important process for the formation of SWHDs in BTH with a relative contribution of 65.3 %, followed by chemistry (17.6 %), cloud processes (−7.5 %), dry deposition (−6.4 %), and planetary boundary layer (PBL) mixing (3.2 %). Further examination showed that SWHDs exhibited large interannual variations in frequency and intensity, which were mainly driven by changes in meteorology. The results of this study have important implications for the control of SWHDs in BTH.

scholarly journals Severe winter haze days in the Beijing-Tianjin-Hebei region from 1985–2017 and the roles of anthropogenic emissions and meteorological parameters

2019 ◽  
Author(s):  
Ruijun Dang ◽  
Hong Liao
Keyword(s):  
Meteorological Parameters ◽  
Transport Model ◽  
Dominant Role ◽  
Temporal Variations ◽  
Anthropogenic Emissions ◽  
Steady Increase ◽  
Severe Winter ◽  
Chemical Transport Model ◽  
Sudden Decrease ◽  
Haze Days

Abstract. We applied a global 3-D chemical transport model (GEOS-Chem) to examine the variations in the frequency and intensity in severe winter haze days (SWHDs) in BTH from 1985–2017 and quantified the roles of changes in anthropogenic emissions and/or meteorological parameters. Comparisons between the simulated SWHDs and those obtained from the observed PM2.5 concentrations and atmospheric visibility showed that the model can capture the spatial and temporal variations of SWHDs in China; the correlation coefficient between the simulated and observed SWHDs is 0.98 at 161 grids in China. From 1985–2017, with changes in both anthropogenic emissions and meteorological parameters, the simulated frequency (total severe haze days in winter) and intensity (PM2.5 concentration averaged over severe haze days in winter) of SWHDs in BTH showed increasing trends of 4.5 days decade−1 and 13.7 μg m−3 decade−1, respectively. The simulated frequency exhibited fluctuations from 1985–2017, with a sudden decrease from 1992–2001 (29 days to 10 days) and a rapid growth from 2003–2012 (16 days to 47 days). The sensitivity simulations indicated that variations in meteorological parameters played a dominant role during 1992–2001, while variations in both emissions and meteorological parameters were important for the simulated frequency trend during 2003–2012 (simulated trends were 27.3 days decade−1 and 12.5 days decade−1 owing to changes in emissions alone and changes in meteorology alone, respectively). The simulated intensity showed a steady increase from 1985–2017, which was driven by changes in both emissions and meteorology. The results of this study have important implications for the control of SWHDs in BTH.

scholarly journals A new diagnostic for tropospheric ozone production

2017 ◽  
Author(s):  
Peter M. Edwards ◽  
Mathew J. Evans
Keyword(s):  
Air Quality ◽  
Tropospheric Ozone ◽  
Transport Model ◽  
Chemical Transport ◽  
Ozone Production ◽  
Chemical Transport Model ◽  
Organic Species ◽  
Earth’S Climate ◽  
Oxidation Of Organics

Abstract. Tropospheric ozone is important for the Earth’s climate and air quality. It is produced during the oxidation of organics in the presence of nitrogen oxides. Due to the range of organic species emitted and the chain like nature of their oxidation, this chemistry is complex and understanding the role of different processes (emission, deposition, chemistry) is difficult. We demonstrate a new methodology for diagnosing ozone production based on the processing of bonds contained within emitted molecules, the fate of which is determined by the conservation of spin of the bonding electrons. Using this methodology to diagnose ozone production in the GEOS-Chem chemical transport model, we demonstrate its advantages over the standard diagnostic. We show that the number of bonds emitted, their chemistry and lifetime, and feedbacks on OH are all important in determining the ozone production within the model and its sensitivity to changes. This insight may allow future model-model comparisons to better identify the root causes of model differences.

scholarly journals Regional and intercontinental pollution signatures on modeled and measured PAN at northern mid-latitude mountain sites

2018 ◽  
Author(s):  
Arlene M. Fiore ◽  
Emily V. Fischer ◽  
Shubha Pandey Deolal ◽  
Oliver Wild ◽  
Dan Jaffe ◽  
...  
Keyword(s):  
Transport Model ◽  
Ozone Production ◽  
Anthropogenic Emissions ◽  
Chemical Transport Model ◽  
Reservoir Species ◽  
Remote Troposphere ◽  
Global Chemical Transport Model ◽  
Peroxy Acetyl Nitrate ◽  
Source Receptor Relationships

Abstract. Peroxy acetyl nitrate (PAN) is the most important reservoir species for nitrogen oxides (NOx) in the remote troposphere. Upon decomposition in remote regions, PAN promotes efficient ozone production. We evaluate monthly mean PAN abundances from global chemical transport model simulations (HTAP1) for 2001 with measurements from five northern mid-latitude mountain sites (four European and one North American). The multi-model mean generally captures the observed monthly mean PAN but individual models simulate a factor of ~ 4–8 range in monthly abundances. We quantify PAN source-receptor relationships at the measurement sites with sensitivity simulations that decrease regional anthropogenic emissions of PAN (and ozone) precursors by 20 % from North America (NA), Europe (EU), and East Asia (EA). The HTAP1 models attribute more of the observed PAN at Jungfraujoch (Switzerland) to emissions in NA and EA, and less to EU, than a prior trajectory-based estimate. The trajectory-based and modeling approaches agree that EU emissions play a role in the observed springtime PAN maximum at Jungfraujoch. The signal from anthropogenic emissions on PAN is strongest at Jungfraujoch and Mount Bachelor (Oregon, U.S.A.) during April. In this month, PAN source-receptor relationships correlate both with model differences in regional anthropogenic volatile organic compound (AVOC) emissions and with ozone source-receptor relationships. PAN observations at mountaintop sites can thus provide key information for evaluating models, including links between PAN and ozone production and source-receptor relationships. Establishing routine, long-term, mountaintop measurements is essential given the large observed interannual variability in PAN.

scholarly journals On the implications of aerosol liquid water and phase separation for organic aerosol mass

2017 ◽  
Vol 17 (1) ◽  
pp. 343-369 ◽  
Author(s):  
Havala O. T. Pye ◽  
Benjamin N. Murphy ◽  
Lu Xu ◽  
Nga L. Ng ◽  
Annmarie G. Carlton ◽  
...  
Keyword(s):  
Organic Carbon ◽  
Organic Compounds ◽  
Water Uptake ◽  
Liquid Water ◽  
Transport Model ◽  
Organic Aerosol ◽  
Water Soluble ◽  
Organic Nitrates ◽  
Monitoring Networks ◽  
Chemical Transport Model

Abstract. Organic compounds and liquid water are major aerosol constituents in the southeast United States (SE US). Water associated with inorganic constituents (inorganic water) can contribute to the partitioning medium for organic aerosol when relative humidities or organic matter to organic carbon (OM ∕ OC) ratios are high such that separation relative humidities (SRH) are below the ambient relative humidity (RH). As OM ∕ OC ratios in the SE US are often between 1.8 and 2.2, organic aerosol experiences both mixing with inorganic water and separation from it. Regional chemical transport model simulations including inorganic water (but excluding water uptake by organic compounds) in the partitioning medium for secondary organic aerosol (SOA) when RH  >  SRH led to increased SOA concentrations, particularly at night. Water uptake to the organic phase resulted in even greater SOA concentrations as a result of a positive feedback in which water uptake increased SOA, which further increased aerosol water and organic aerosol. Aerosol properties, such as the OM ∕ OC and hygroscopicity parameter (κorg), were captured well by the model compared with measurements during the Southern Oxidant and Aerosol Study (SOAS) 2013. Organic nitrates from monoterpene oxidation were predicted to be the least water-soluble semivolatile species in the model, but most biogenically derived semivolatile species in the Community Multiscale Air Quality (CMAQ) model were highly water soluble and expected to contribute to water-soluble organic carbon (WSOC). Organic aerosol and SOA precursors were abundant at night, but additional improvements in daytime organic aerosol are needed to close the model–measurement gap. When taking into account deviations from ideality, including both inorganic (when RH  >  SRH) and organic water in the organic partitioning medium reduced the mean bias in SOA for routine monitoring networks and improved model performance compared to observations from SOAS. Property updates from this work will be released in CMAQ v5.2.

scholarly journals Sensitivity of chemical tracers to meteorological parameters in the MOZART-3 chemical transport model

2007 ◽  
Vol 112 (D20) ◽  
Author(s):  
D. E. Kinnison ◽  
G. P. Brasseur ◽  
S. Walters ◽  
R. R. Garcia ◽  
D. R. Marsh ◽  
...  
Keyword(s):  
Meteorological Parameters ◽  
Transport Model ◽  
Chemical Transport ◽  
Chemical Transport Model ◽  
Chemical Tracers

scholarly journals Sulfate-nitrate-ammonium aerosols over China: response to 2000–2015 emission changes of sulfur dioxide, nitrogen oxides, and ammonia

2013 ◽  
Vol 13 (5) ◽  
pp. 2635-2652 ◽  
Author(s):  
Y. Wang ◽  
Q. Q. Zhang ◽  
K. He ◽  
Q. Zhang ◽  
L. Chai
Keyword(s):  
Emission Reduction ◽  
Transport Model ◽  
Critical Role ◽  
Sufficient Information ◽  
Nox Emissions ◽  
Chemical Transport Model ◽  
Dominant Component ◽  
Emission Changes ◽  
Emission Reduction Target

Abstract. We use a chemical transport model to examine the change of sulfate-nitrate-ammonium (SNA) aerosols over China due to anthropogenic emission changes of their precursors (SO2, NOx and NH3) from 2000 to 2015. From 2000 to 2006, annual mean SNA concentrations increased by about 60% over China as a result of the 60% and 80% increases in SO2 and NOx emissions. During this period, sulfate is the dominant component of SNA over South China (SC) and Sichuan Basin (SCB), while nitrate and sulfate contribute equally over North China (NC). Based on emission reduction targets in the 12th (2011–2015) Five-Year Plan (FYP), China's total SO2 and NOx emissions are projected to change by −16% and +16% from 2006 to 2015, respectively. The amount of NH3 emissions in 2015 is uncertain, given the lack of sufficient information on the past and present levels of NH3 emissions in China. With no change in NH3 emissions, SNA mass concentrations in 2015 will decrease over SCB and SC compared to their 2006 levels, but increase over NC where the magnitude of nitrate increase exceeds that of sulfate reduction. This suggests that the SO2 emission reduction target set by the 12th FYP, although effective in reducing SNA over SC and SCB, will not be successful over NC, for which NOx emission control needs to be strengthened. If NH3 emissions are allowed to keep their recent growth rate and increase by +16% from 2006 to 2015, the benefit of SO2 reduction will be completely offset over all of China due to the significant increase of nitrate, demonstrating the critical role of NH3 in regulating nitrate. The effective strategy to control SNA and hence PM2.5 pollution over China should thus be based on improving understanding of current NH3 emissions and putting more emphasis on controlling NH3 emissions in the future.

scholarly journals Source attribution of Arctic black carbon constrained by aircraft and surface measurements

2017 ◽  
Vol 17 (19) ◽  
pp. 11971-11989 ◽  
Author(s):  
Jun-Wei Xu ◽  
Randall V. Martin ◽  
Andrew Morrow ◽  
Sangeeta Sharma ◽  
Lin Huang ◽  
...  
Keyword(s):  
North America ◽  
Biomass Burning ◽  
Western Siberia ◽  
Transport Model ◽  
Chemical Transport ◽  
The Arctic ◽  
Anthropogenic Emissions ◽  
Chemical Transport Model ◽  
Northern Asia ◽  
Airborne Measurements

Abstract. Black carbon (BC) contributes to Arctic warming, yet sources of Arctic BC and their geographic contributions remain uncertain. We interpret a series of recent airborne (NETCARE 2015; PAMARCMiP 2009 and 2011 campaigns) and ground-based measurements (at Alert, Barrow and Ny-Ålesund) from multiple methods (thermal, laser incandescence and light absorption) with the GEOS-Chem global chemical transport model and its adjoint to attribute the sources of Arctic BC. This is the first comparison with a chemical transport model of refractory BC (rBC) measurements at Alert. The springtime airborne measurements performed by the NETCARE campaign in 2015 and the PAMARCMiP campaigns in 2009 and 2011 offer BC vertical profiles extending to above 6 km across the Arctic and include profiles above Arctic ground monitoring stations. Our simulations with the addition of seasonally varying domestic heating and of gas flaring emissions are consistent with ground-based measurements of BC concentrations at Alert and Barrow in winter and spring (rRMSE  < 13 %) and with airborne measurements of the BC vertical profile across the Arctic (rRMSE  = 17 %) except for an underestimation in the middle troposphere (500–700 hPa).Sensitivity simulations suggest that anthropogenic emissions in eastern and southern Asia have the largest effect on the Arctic BC column burden both in spring (56 %) and annually (37 %), with the largest contribution in the middle troposphere (400–700 hPa). Anthropogenic emissions from northern Asia contribute considerable BC (27 % in spring and 43 % annually) to the lower troposphere (below 900 hPa). Biomass burning contributes 20 % to the Arctic BC column annually.At the Arctic surface, anthropogenic emissions from northern Asia (40–45 %) and eastern and southern Asia (20–40 %) are the largest BC contributors in winter and spring, followed by Europe (16–36 %). Biomass burning from North America is the most important contributor to all stations in summer, especially at Barrow.Our adjoint simulations indicate pronounced spatial heterogeneity in the contribution of emissions to the Arctic BC column concentrations, with noteworthy contributions from emissions in eastern China (15 %) and western Siberia (6.5 %). Although uncertain, gas flaring emissions from oilfields in western Siberia could have a striking impact (13 %) on Arctic BC loadings in January, comparable to the total influence of continental Europe and North America (6.5 % each in January). Emissions from as far as the Indo-Gangetic Plain could have a substantial influence (6.3 % annually) on Arctic BC as well.

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