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Secondary Inorganic Aerosol in the Yangtze River Delta of China
Roeland Cornelis JANSEN
12110740001
PhD defense presentation
Fudan University Handan Road 220, 200433, Shanghai China
November 30, 2014
Professor Jianmin CHEN
Outline:
1. Introduction:
• Introduction in Secondary Inorganic Aerosol and the Yangtze River Delta of China and objectives of this study
2. Experimental part:
• Results from 2 campaigns: Shanghai and Hangzhou
3. Conclusions and suggestions for further work
4. Acknowledgment
5. Q&A
Introduction: The Yangtze River Delta of China
Millions of people
Millions of cars
Thousands of factories
Tons of emission
A lot of agriculture
…
NOx SO2 NH3
Tropospheric NO2 concentrations in east China mapped with the
ERS-2 research satellite during the Global Ozone Monitoring
Experiment (GOME). Reprinted from Huang et al., 2011.
Introduction: Emissions in Yangtze River Delta of China
Point sources in the Yangtze River Delta: left
power plants and right: industrial point sources
Reprinted from Li et al.,2011
Reprinted from Aneja et al., 2001
Formation, growth and removal of atmospheric aerosol
Samples are all sub-micrometer aerosol. Reprinted from
Jimenez et al., 2009.
Introduction: Secondary Inorganic Aerosol (SIA)
Precursor gasses NH3, SO2 , NOx and HCl react
(SO2 and NOx after oxidation) to form SIA:
2 NH3(g) + H2SO4(l) (NH4)2SO4(l)
NH3(g) + HNO3(g) NH4NO3(s or l)
NH3(g) + HCl(g) NH4Cl(s or l)
SIA makes up 30-70% of the total mass of
submicron aerosol (PM1)
Reprinted from Malm, 1999
Studies on SIA role and behavior
Hygroscopic properties
Reprinted from Tang, 1979
Scattering of radiation
Effects of hygroscopicity:
• Increase in water content
• Increase of particle size
• More effective scattering
• Cloud formation
Effects of scattering:
• Decrease of visibility
• Global cooling effect
Reprinted from Malm, 1999.
Reprinted from NOAA
Introduction: Atmospheric aerosol behavior
Hygroscopic properties
Scattering of radiation
What is the behavior and role of SIA in the YRD?
Experimental part: 2 campaigns
Hangzhou, Zhejiang University Shanghai, Fudan University
December 2012April-May 2012
Instrument: Time Resolution:
Aerosol inorganic composition: MARGA 1 hour
PM mass: R&P TEOM 1400a 1 hour
Thermo SHARP 5030 1 hour
Acidic trace gas + ammonia MARGA 1 hour
O3 Thermo 49i continuous
NOx Thermo 42i continuous
Visibility Belfort 5000/6000 continuous
RH, temperature, pressure, wind speed Metone continuous
Vaisala (Hydromet) continuous
Aerosol
Gas
Meteorological
Experimental part: Instruments
MARGA at site in Hangzhou.
Experimental part: MARGA worldwide ~50 publications since 2010
Aerosol: Gas:
Na+ NH3
K+ SO2
NH4
+ HNO2
Mg2+ HNO3
Ca2+ HCl
NO3
-
Cl-
SO4
2-
hourly results, recovery ~90%
Validation of data:
Winiwarter, 1989
Wyers et al., 1993
Khlystov et al, 1995
Slanina et al, 2001
Trebs et al., 2004
Antkowiak et al., 2009
Hahlbusch et al., 2011
Makkonen et al., 2012
TOC
TN
VA
MS
Experimental part: Time series of RH and Visibility in Shanghai
Experimental part: Time series of SIA and precursor gasses
Experimental part: Correlations Visibility versus PM1 mass
Correlation of visibility vs. PM1 mass.
Correlations of visibility vs. PM1 mass for different
RH values
Conclusion: The correlation between visibility and mass concentration of PM1 depends strongly
on the relative humidity
Fudannonmov
Experimental part: Rel. mass contribution of SIA to PM
Shanghai PM1; December 2012; N=660
SO4
2- NO3
-
Sun et al., 2013; PM1 in Beijing
Classifying periods of air pollution
Visibility > 10 km.
Du et al., 2011; Xiao et al., 2011; Wu et al., 2005
Clear FogHaze
Visibility < 10 km.
RH < 90%
Time > 4 hr.
Visibility < 10 km.
RH > 90%
Time > 4 hr.
Experimental part: Identifying haze periods
Experimental part: Meteorological conditions
Clear Haze Fog
Number of hours 354 114 48
T (°C) 20.9±6.1 20.8±3.8 18.4±3.2
RH (%) 61.3±16.9 73.9±11.4 93.1±1.9
Pressure (hPa) 1005±5.6 1002.7±3.6 1001.7±4.7
Wind Speed (m/s) 1.4±0.8 1.3±0.7 0.8±0.5
Visibility (km) 21.2±10.4 6.6±2.0 3.3±0.8
PM2.5 (μg/m3) 67±38 118±41 105±27
Clear Haze Fog
Number of hours 483 94 40
T (°C) 5.9±3.9 7.0±3.9 7.4±1.5
RH (%) 58.9±14.7 69.8±15.1 93.6±3.3
Pressure (hPa) 1024±3.7 1022±4.5 1019±1.7
Wind Speed (m/s) 2.4±1.1 2.6±1.1 2.2±0.9
Visibility (km) 25.6±11.2 7.2±1.9 5.4±2.1
PM1 (μg/m3) 31±17 62±26 24±9
Shanghai PM1; December 2012, n=617Hangzhou PM2.5; April-May 2012, n=516
69
22
9
clear
haze
fog
78
15
7
clear
haze
fog
%
% %%%
%
Conclusion: The visibility during fog is lowest while the mass concentration on PM is not, this
shows the importance of the RH value on visibility
246231
67
118 105
Experimental part: SIA mass contribution to PM
Shanghai
PM1
Hangzhou
PM2.5
Conclusion: The SIA in aerosol changes slightly between clear, haze and fog
with nitrate being the most obvious change.
Clear Haze Fog
Experimental part: Molar equivalent ratio SIA
Equi-molar balance: ([NH4
+]/18) / ((2[SO4
2-]/96) + ([NO3
-]/62))2 NH3 + H2SO4 (NH4)2SO4
NH3 + HNO3 NH4NO3
Conclusion: PM1 particles in Shanghai (in Dec. ‘12) are slightly alkaline. In the balance there is
no significant difference between clear, haze and fog weather periods.
Experimental part: Molar equivalent SIA with Cl-
NH4
+ / (NO3
- + 2SO4
2- ) NH4
+ / (NO3
- + 2SO4
2- + Cl- )
All data (N=660) Y = 1.12x – 0.18; R2 = 0.97 Y = 0.99x – 0.42; R2 = 0.99
Clear weather (N=425) Y = 1.08x – 0.08; R2 = 0.95 Y = 0.98x – 0.42; R2 = 0.99
Haze weather (N=90) Y = 1.18x – 0.54; R2 = 0.95 Y = 1.03x – 0.74; R2 = 0.99
Fog weather (N=30) Y = 1.13x – 0.14; R2 = 0.96 Y = 0.89x – 0.14; R2 = 0.97
Y = actual measured NH4
+ concentration in μg/m3
X = predicted NH4
+ concentration in μg/m3 (sum of NO3
- and SO4
2- and NO3
- SO4
2- and Cl-)
What binds to NH4
+ at high RH values?? Lack of HSO4
- data.
Sun et al., 2013; PM1 in Beijing
Nitrate to sulfate molar ratio
[NO3
-]/[SO4
2-] as function of
ammonium to sulfate ratio
[NH4
+]/[SO4
2-].
Relation between molar
concentrations of [NO3
-] and
[NH4
+] – [SO4
2-].
Hangzhou PM2.5 Shanghai PM 1
Experimental part: Molar ratios of SIA
Reprinted from Pathak et al., 2009 (PM2.5)
Conclusion: Nitrate formation starts after sulfate formation and there is no significant
difference between clear, haze and fog weather periods.
Conclusion: Nitrate formation happens mainly by SIA formation
Beside sulfate and nitrate, ammonium is bound to species like chloride and bisulfate
Experimental part: NOAA HYSPLIT 4
500 and 1000 meter were used,
which represent the average
mixed layer height in Shanghai
(Huang et al., 2012a; Yang et al.,
2006; Kong et al., 2014).
NH3 emission sources are
Yangzhou (NW of Shanghai),
Nantong (NNW of Shanghai) and
Jiaxing (SW of Shanghai)
Huang et al., 2011.
2 SCI publications in 2014
Jansen et al., 2014. Advances in Atmospheric
Sciences Nov. 2014, Vol. 31, Issue 6, pp 1427-1434
IF: 1.459
Roeland Cornelis Jansen, Jianmin Chen, and
Yunjie Hu. Advances in Meteorology, Vol. 2014,
Article ID 534675. IF: 1.348

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Fudannonmov

  • 1. Secondary Inorganic Aerosol in the Yangtze River Delta of China Roeland Cornelis JANSEN 12110740001 PhD defense presentation Fudan University Handan Road 220, 200433, Shanghai China November 30, 2014 Professor Jianmin CHEN
  • 2. Outline: 1. Introduction: • Introduction in Secondary Inorganic Aerosol and the Yangtze River Delta of China and objectives of this study 2. Experimental part: • Results from 2 campaigns: Shanghai and Hangzhou 3. Conclusions and suggestions for further work 4. Acknowledgment 5. Q&A
  • 3. Introduction: The Yangtze River Delta of China Millions of people Millions of cars Thousands of factories Tons of emission A lot of agriculture … NOx SO2 NH3
  • 4. Tropospheric NO2 concentrations in east China mapped with the ERS-2 research satellite during the Global Ozone Monitoring Experiment (GOME). Reprinted from Huang et al., 2011. Introduction: Emissions in Yangtze River Delta of China Point sources in the Yangtze River Delta: left power plants and right: industrial point sources Reprinted from Li et al.,2011
  • 5. Reprinted from Aneja et al., 2001 Formation, growth and removal of atmospheric aerosol
  • 6. Samples are all sub-micrometer aerosol. Reprinted from Jimenez et al., 2009. Introduction: Secondary Inorganic Aerosol (SIA) Precursor gasses NH3, SO2 , NOx and HCl react (SO2 and NOx after oxidation) to form SIA: 2 NH3(g) + H2SO4(l) (NH4)2SO4(l) NH3(g) + HNO3(g) NH4NO3(s or l) NH3(g) + HCl(g) NH4Cl(s or l) SIA makes up 30-70% of the total mass of submicron aerosol (PM1)
  • 7. Reprinted from Malm, 1999 Studies on SIA role and behavior Hygroscopic properties Reprinted from Tang, 1979 Scattering of radiation Effects of hygroscopicity: • Increase in water content • Increase of particle size • More effective scattering • Cloud formation Effects of scattering: • Decrease of visibility • Global cooling effect Reprinted from Malm, 1999.
  • 8. Reprinted from NOAA Introduction: Atmospheric aerosol behavior Hygroscopic properties Scattering of radiation
  • 9. What is the behavior and role of SIA in the YRD?
  • 10. Experimental part: 2 campaigns Hangzhou, Zhejiang University Shanghai, Fudan University December 2012April-May 2012
  • 11. Instrument: Time Resolution: Aerosol inorganic composition: MARGA 1 hour PM mass: R&P TEOM 1400a 1 hour Thermo SHARP 5030 1 hour Acidic trace gas + ammonia MARGA 1 hour O3 Thermo 49i continuous NOx Thermo 42i continuous Visibility Belfort 5000/6000 continuous RH, temperature, pressure, wind speed Metone continuous Vaisala (Hydromet) continuous Aerosol Gas Meteorological Experimental part: Instruments
  • 12. MARGA at site in Hangzhou. Experimental part: MARGA worldwide ~50 publications since 2010 Aerosol: Gas: Na+ NH3 K+ SO2 NH4 + HNO2 Mg2+ HNO3 Ca2+ HCl NO3 - Cl- SO4 2- hourly results, recovery ~90% Validation of data: Winiwarter, 1989 Wyers et al., 1993 Khlystov et al, 1995 Slanina et al, 2001 Trebs et al., 2004 Antkowiak et al., 2009 Hahlbusch et al., 2011 Makkonen et al., 2012 TOC TN VA MS
  • 13. Experimental part: Time series of RH and Visibility in Shanghai
  • 14. Experimental part: Time series of SIA and precursor gasses
  • 15. Experimental part: Correlations Visibility versus PM1 mass Correlation of visibility vs. PM1 mass. Correlations of visibility vs. PM1 mass for different RH values Conclusion: The correlation between visibility and mass concentration of PM1 depends strongly on the relative humidity
  • 17. Experimental part: Rel. mass contribution of SIA to PM Shanghai PM1; December 2012; N=660 SO4 2- NO3 - Sun et al., 2013; PM1 in Beijing
  • 18. Classifying periods of air pollution Visibility > 10 km. Du et al., 2011; Xiao et al., 2011; Wu et al., 2005 Clear FogHaze Visibility < 10 km. RH < 90% Time > 4 hr. Visibility < 10 km. RH > 90% Time > 4 hr.
  • 20. Experimental part: Meteorological conditions Clear Haze Fog Number of hours 354 114 48 T (°C) 20.9±6.1 20.8±3.8 18.4±3.2 RH (%) 61.3±16.9 73.9±11.4 93.1±1.9 Pressure (hPa) 1005±5.6 1002.7±3.6 1001.7±4.7 Wind Speed (m/s) 1.4±0.8 1.3±0.7 0.8±0.5 Visibility (km) 21.2±10.4 6.6±2.0 3.3±0.8 PM2.5 (μg/m3) 67±38 118±41 105±27 Clear Haze Fog Number of hours 483 94 40 T (°C) 5.9±3.9 7.0±3.9 7.4±1.5 RH (%) 58.9±14.7 69.8±15.1 93.6±3.3 Pressure (hPa) 1024±3.7 1022±4.5 1019±1.7 Wind Speed (m/s) 2.4±1.1 2.6±1.1 2.2±0.9 Visibility (km) 25.6±11.2 7.2±1.9 5.4±2.1 PM1 (μg/m3) 31±17 62±26 24±9 Shanghai PM1; December 2012, n=617Hangzhou PM2.5; April-May 2012, n=516 69 22 9 clear haze fog 78 15 7 clear haze fog % % %%% % Conclusion: The visibility during fog is lowest while the mass concentration on PM is not, this shows the importance of the RH value on visibility
  • 21. 246231 67 118 105 Experimental part: SIA mass contribution to PM Shanghai PM1 Hangzhou PM2.5 Conclusion: The SIA in aerosol changes slightly between clear, haze and fog with nitrate being the most obvious change. Clear Haze Fog
  • 22. Experimental part: Molar equivalent ratio SIA Equi-molar balance: ([NH4 +]/18) / ((2[SO4 2-]/96) + ([NO3 -]/62))2 NH3 + H2SO4 (NH4)2SO4 NH3 + HNO3 NH4NO3 Conclusion: PM1 particles in Shanghai (in Dec. ‘12) are slightly alkaline. In the balance there is no significant difference between clear, haze and fog weather periods.
  • 23. Experimental part: Molar equivalent SIA with Cl- NH4 + / (NO3 - + 2SO4 2- ) NH4 + / (NO3 - + 2SO4 2- + Cl- ) All data (N=660) Y = 1.12x – 0.18; R2 = 0.97 Y = 0.99x – 0.42; R2 = 0.99 Clear weather (N=425) Y = 1.08x – 0.08; R2 = 0.95 Y = 0.98x – 0.42; R2 = 0.99 Haze weather (N=90) Y = 1.18x – 0.54; R2 = 0.95 Y = 1.03x – 0.74; R2 = 0.99 Fog weather (N=30) Y = 1.13x – 0.14; R2 = 0.96 Y = 0.89x – 0.14; R2 = 0.97 Y = actual measured NH4 + concentration in μg/m3 X = predicted NH4 + concentration in μg/m3 (sum of NO3 - and SO4 2- and NO3 - SO4 2- and Cl-) What binds to NH4 + at high RH values?? Lack of HSO4 - data. Sun et al., 2013; PM1 in Beijing
  • 24. Nitrate to sulfate molar ratio [NO3 -]/[SO4 2-] as function of ammonium to sulfate ratio [NH4 +]/[SO4 2-]. Relation between molar concentrations of [NO3 -] and [NH4 +] – [SO4 2-]. Hangzhou PM2.5 Shanghai PM 1 Experimental part: Molar ratios of SIA Reprinted from Pathak et al., 2009 (PM2.5) Conclusion: Nitrate formation starts after sulfate formation and there is no significant difference between clear, haze and fog weather periods. Conclusion: Nitrate formation happens mainly by SIA formation Beside sulfate and nitrate, ammonium is bound to species like chloride and bisulfate
  • 25. Experimental part: NOAA HYSPLIT 4 500 and 1000 meter were used, which represent the average mixed layer height in Shanghai (Huang et al., 2012a; Yang et al., 2006; Kong et al., 2014). NH3 emission sources are Yangzhou (NW of Shanghai), Nantong (NNW of Shanghai) and Jiaxing (SW of Shanghai) Huang et al., 2011.
  • 26. 2 SCI publications in 2014 Jansen et al., 2014. Advances in Atmospheric Sciences Nov. 2014, Vol. 31, Issue 6, pp 1427-1434 IF: 1.459 Roeland Cornelis Jansen, Jianmin Chen, and Yunjie Hu. Advances in Meteorology, Vol. 2014, Article ID 534675. IF: 1.348