Estimate of biogenic VOC emissions in Japan and their effects on photochemical formation of ambient ozone and secondary organic aerosol

2015 ◽  
Vol 120 ◽  
pp. 38-50 ◽  
Author(s):  
Satoru Chatani ◽  
Sou N. Matsunaga ◽  
Seiji Nakatsuka
Keyword(s):  
Secondary Organic Aerosol ◽  
Organic Aerosol ◽  
Voc Emissions ◽  
Ambient Ozone ◽  
Photochemical Formation ◽  
Biogenic Voc

scholarly journals Naturally driven variability in the global secondary organic aerosol over a decade

2005 ◽  
Vol 5 (7) ◽  
pp. 1891-1904 ◽  
Author(s):  
K. Tsigaridis ◽  
J. Lathière ◽  
M. Kanakidou ◽  
D. A. Hauglustaine
Keyword(s):  
Secondary Organic Aerosol ◽  
Hydrological Cycle ◽  
Transport Model ◽  
Organic Aerosol ◽  
Voc Emissions ◽  
3 Dimensional ◽  
Voc Oxidation ◽  
Biogenic Voc ◽  
On Line ◽  
Emission Changes

Abstract. In order to investigate the variability of the secondary organic aerosol (SOA) distributions and budget and provide a measure for the robustness of the conclusions on human induced changes of SOA, a global 3-dimensional chemistry transport model describing both the gas and the particulate phase chemistry of the troposphere has been applied. The response of the global budget of SOA to temperature and moisture changes as well as to biogenic emission changes over a decade (1984-1993) has been evaluated. The considered emissions of biogenic non-methane volatile organic compounds (VOC) are driven by temperature, light and vegetation. They vary between 756 and 810 Tg Cy-1 and are therefore about 5.5 times higher than the anthropogenic VOC emissions. All secondary aerosols (sulphuric, nitrates and organics) are computed on-line together with the aerosol associated water. Over the studied decade, the computed natural variations (8%) in the chemical SOA production from biogenic VOC oxidation equal the chemical SOA production from anthropogenic VOC oxidation. Maximum values are calculated for 1990 (warmer and drier) and minimum values for 1986 (colder and wetter). The SOA computed variability results from a 7% increase in biogenic VOC emissions from 1986 to 1990 combined with 8.5% and 6% increases in the wet and dry deposition of SOA and leads to about 11.5% increase in the SOA burden of biogenic origin. The present study also demonstrates the importance of the hydrological cycle in determining the built up and fate of SOA in the atmosphere. It also reveals the existence of significant positive and negative feedback mechanisms in the atmosphere responsible for the non linear relationship between emissions of biogenic VOC and SOA burden.

scholarly journals Naturally driven variability in the global secondary organic aerosol over a decade

2005 ◽  
Vol 5 (2) ◽  
pp. 1255-1283
Author(s):  
K. Tsigaridis ◽  
J. Lathière ◽  
M. Kanakidou ◽  
D. A. Hauglustaine
Keyword(s):  
Secondary Organic Aerosol ◽  
Hydrological Cycle ◽  
Transport Model ◽  
Organic Aerosol ◽  
Voc Emissions ◽  
3 Dimensional ◽  
Voc Oxidation ◽  
Biogenic Voc ◽  
On Line ◽  
Emission Changes

Abstract. In order to investigate the variability of the secondary organic aerosol (SOA) distributions and budget and provide a measure for the robustness of the conclusions on human induced changes of SOA, a global 3-dimensional chemistry transport model describing both the gas and the particulate phase chemistry of the troposphere has been applied. The response of the global budget of SOA to temperature and moisture changes as well as to biogenic emission changes over a decade (1984–1993) has been evaluated. The considered emissions of biogenic non-methane volatile organic compounds (VOC) are driven by temperature, light and vegetation. They vary between 756 and 810 TgC y-1 and are therefore about 5.5 times higher than the anthropogenic VOC emissions. All secondary aerosols (sulphuric, nitrates and organics) are computed on-line together with the aerosol associated water. Over the studied decade, the computed natural variations (8%) in the chemical SOA production from biogenic VOC oxidation equal the chemical SOA production from anthropogenic VOC oxidation. This computed variability results from a 7% increase in biogenic VOC emissions combined with 8.5% and 6% increases in the wet and dry deposition of SOA and leads to about 11.5% increase in the SOA burden of biogenic origin. The present study also demonstrates the importance of the hydrological cycle in determining the built up and fate of SOA in the atmosphere. It also reveals the existence of significant positive and negative feedback mechanisms in the atmosphere responsible for the non linear relationship between emissions of biogenic VOC and SOA burden.

scholarly journals Numerical Sensitivity Tests of Volatile Organic Compounds Emission to PM2.5 Formation during Heat Wave Period in 2018 in Two Southeast Korean Cities

Atmosphere ◽  
2020 ◽  
Vol 11 (4) ◽  
pp. 331 ◽  
Author(s):  
Geum-Hee Yang ◽  
Yu-Jin Jo ◽  
Hyo-Jung Lee ◽  
Chang-Keun Song ◽  
Cheol-Hee Kim
Keyword(s):  
Heat Wave ◽  
Metropolitan Areas ◽  
Secondary Organic Aerosol ◽  
Atmospheric Transport ◽  
Wrf Model ◽  
Organic Aerosol ◽  
Photochemical Reactions ◽  
Wave Period ◽  
Voc Emissions ◽  
Volatile Organic

A record-breaking severe heat wave was recorded in southeast Korea from 11 July to 15 August 2018, and the numerical sensitivity simulations of volatile organic compound (VOC) to secondarily generated particulate matter with diameter of less than 2.5 µm (PM2.5) concentrations were studied in the Busan and Ulsan metropolitan areas in southeast Korea. A weather research and forecasting (WRF) model coupled with chemistry (WRF-Chem) was employed, and we carried out VOC emission sensitivity simulations to investigate variations in PM2.5 concentrations during the heat wave period that occurred from 11 July to 15 August 2018. In our study, when anthropogenic VOC emissions from the Comprehensive Regional Emissions Inventory for Atmospheric Transport Experiment-2015 (CREATE-2015) inventory were increased by approximately a factor of five in southeast Korea, a better agreement with observations of PM2.5 mass concentrations was simulated, implying an underestimation of anthropogenic VOC emissions over southeast Korea. The simulated secondary organic aerosol (SOA) fraction, in particular, showed greater dominance during high temperature periods such as 19–21 July, 2018, with the SOA fractions of 42.3% (in Busan) and 34.3% (in Ulsan) among a sub-total of seven inorganic and organic components. This is considerably higher than observed annual mean organic carbon (OC) fraction (28.4 ± 4%) among seven components, indicating the enhancement of secondary organic aerosols induced by photochemical reactions during the heat wave period in both metropolitan areas. The PM2.5 to PM10 ratios were 0.69 and 0.74, on average, during the study period in the two cities. These were also significantly higher than the typical range in those cities, which was 0.5–0.6 in 2018. Our simulations implied that extremely high temperatures with no precipitation are significantly important to the secondary generation of PM2.5 with higher secondary organic aerosol fraction via photochemical reactions in southeastern Korean cities. Other possible relationships between anthropogenic VOC emissions and temperature during the heat wave episode are also discussed in this study.

Photochemical Formation of Nitrite and Nitrous Acid (HONO) upon Irradiation of Nitrophenols in Aqueous Solution and in Viscous Secondary Organic Aerosol Proxy

2017 ◽  
Vol 51 (13) ◽  
pp. 7486-7495 ◽  
Author(s):  
Francesco Barsotti ◽  
Thorsten Bartels-Rausch ◽  
Elisa De Laurentiis ◽  
Markus Ammann ◽  
Marcello Brigante ◽  
...  
Keyword(s):  
Aqueous Solution ◽  
Nitrous Acid ◽  
Secondary Organic Aerosol ◽  
Organic Aerosol ◽  
Photochemical Formation

scholarly journals Simulating the detailed chemical composition of secondary organic aerosol formed on a regional scale during the TORCH 2003 campaign in the southern UK

2006 ◽  
Vol 6 (2) ◽  
pp. 419-431 ◽  
Author(s):  
D. Johnson ◽  
S. R. Utembe ◽  
M. E. Jenkin
Keyword(s):  
Chemical Composition ◽  
Secondary Organic Aerosol ◽  
Regional Scale ◽  
Equilibrium Phase ◽  
Organic Aerosol ◽  
Oxidation Products ◽  
Chemical Mechanism ◽  
Phase Partitioning ◽  
Biogenic Voc ◽  
Detailed Chemical

Abstract. Following on from the companion study (Johnson et al., 2006), a photochemical trajectory model (PTM) has been used to simulate the chemical composition of organic aerosol for selected events during the 2003 TORCH (Tropospheric Organic Chemistry Experiment) field campaign. The PTM incorporates the speciated emissions of 124 non-methane anthropogenic volatile organic compounds (VOC) and three representative biogenic VOC, a highly-detailed representation of the atmospheric degradation of these VOC, the emission of primary organic aerosol (POA) material and the formation of secondary organic aerosol (SOA) material. SOA formation was represented by the transfer of semi- and non-volatile oxidation products from the gas-phase to a condensed organic aerosol-phase, according to estimated thermodynamic equilibrium phase-partitioning characteristics for around 2000 reaction products. After significantly scaling all phase-partitioning coefficients, and assuming a persistent background organic aerosol (both required in order to match the observed organic aerosol loadings), the detailed chemical composition of the simulated SOA has been investigated in terms of intermediate oxygenated species in the Master Chemical Mechanism, version 3.1 (MCM v3.1). For the various case studies considered, 90% of the simulated SOA mass comprises between ca. 70 and 100 multifunctional oxygenated species derived, in varying amounts, from the photooxidation of VOC of anthropogenic and biogenic origin. The anthropogenic contribution is dominated by aromatic hydrocarbons and the biogenic contribution by α- and β-pinene (which also constitute surrogates for other emitted monoterpene species). Sensitivity in the simulated mass of SOA to changes in the emission rates of anthropogenic and biogenic VOC has also been investigated for 11 case study events, and the results have been compared to the detailed chemical composition data. The role of accretion chemistry in SOA formation, and its implications for the results of the present investigation, is discussed.

scholarly journals Evolution of the complex refractive index in the near UV spectral region in ageing secondary organic aerosol

2014 ◽  
Vol 14 (3) ◽  
pp. 4149-4187 ◽  
Author(s):  
J. M. Flores ◽  
D. F. Zhao ◽  
L. Segev ◽  
P. Schlag ◽  
A. Kiendler-Scharr ◽  
...  
Keyword(s):  
Refractive Index ◽  
Physical Properties ◽  
Spectral Region ◽  
Secondary Organic Aerosol ◽  
Ageing Time ◽  
Complex Refractive Index ◽  
Organic Aerosol ◽  
Photochemical Degradation ◽  
Optical Extinction ◽  
Biogenic Voc

Abstract. The chemical and physical properties of secondary organic aerosol (SOA) formed by the photochemical degradation of biogenic and anthropogenic volatile organic compounds (VOC) are yet poorly constrained. The evolution of the complex refractive index (RI) of SOA, formed from purely biogenic VOC and mixtures of biogenic and anthropogenic VOC was studied over a diurnal cycle in the SAPHIR photochemical outdoor chamber in Jülich, Germany. The correlation of RI with SOA chemical and physical properties such as oxidation level and volatility was examined. The RI was retrieved by a newly developed broadband cavity enhanced spectrometer for aerosol optical extinction measurements in the near UV spectral region (360 to 420 nm). Chemical composition and volatility of the particles were monitored by a high resolution time of flight aerosol mass spectrometer, and a volatility tandem differential mobility analyzer. SOA was formed by ozonolysis of either (i) a mixture of biogenic VOC (α-pinene and limonene), (ii) biogenic VOC mixture with subsequent addition of an anthropogenic VOC (p-xylene-d10), or (iii) a mixture of biogenic and anthropogenic VOC. The SOA aged by ozone / OH reactions up to 29.5 h was found to be non-absorbing in all cases. The SOA with p-xylene-d10 showed an increase of the scattering component of the RI correlated with an increase of the O / C ratio and with an increase in the SOA density. There was a greater increase in the scattering component of the RI when the SOA was produced from the mixture of biogenic VOCs and anthropogenic VOC than from the sequential addition of the VOCs after the approximate same ageing time. The increase of the scattering component was inversely correlated with the SOA volatility. Two RI retrievals determined for the pure biogenic SOA showed a constant RI for up to 5 h of ageing. Mass spectral characterization shows the three types of the SOA formed in this study have significant amount of semivolatile components. The influence of anthropogenic VOCs on the oxygenated organic aerosol, and the atmospheric implications are discussed.

scholarly journals Evolution of the complex refractive index in the UV spectral region in ageing secondary organic aerosol

2014 ◽  
Vol 14 (11) ◽  
pp. 5793-5806 ◽  
Author(s):  
J. M. Flores ◽  
D. F. Zhao ◽  
L. Segev ◽  
P. Schlag ◽  
A. Kiendler-Scharr ◽  
...  
Keyword(s):  
Refractive Index ◽  
Physical Properties ◽  
Spectral Region ◽  
Secondary Organic Aerosol ◽  
Ageing Time ◽  
Complex Refractive Index ◽  
Organic Aerosol ◽  
Photochemical Degradation ◽  
Optical Extinction ◽  
Biogenic Voc

Abstract. The chemical and physical properties of secondary organic aerosol (SOA) formed by the photochemical degradation of biogenic and anthropogenic volatile organic compounds (VOC) are as yet still poorly constrained. The evolution of the complex refractive index (RI) of SOA, formed from purely biogenic VOC and mixtures of biogenic and anthropogenic VOC, was studied over a diurnal cycle in the SAPHIR photochemical outdoor chamber in Jülich, Germany. The correlation of RI with SOA chemical and physical properties such as oxidation level and volatility was examined. The RI was retrieved by a newly developed broadband cavity-enhanced spectrometer for aerosol optical extinction measurements in the UV spectral region (360 to 420 nm). Chemical composition and volatility of the particles were monitored by a high-resolution time-of-flight aerosol mass spectrometer, and a volatility tandem differential mobility analyzer. SOA was formed by ozonolysis of either (i) a mixture of biogenic VOC (α-pinene and limonene), (ii) biogenic VOC mixture with subsequent addition of an anthropogenic VOC (p-xylene-d10), or (iii) a mixture of biogenic and anthropogenic VOC. The SOA aged by ozone/OH reactions up to 29.5 h was found to be non-absorbing in all cases. The SOA with p-xylene-d10 showed an increase of the scattering component of the RI correlated with an increase of the O / C ratio and with an increase in the SOA density. There was a greater increase in the scattering component of the RI when the SOA was produced from the mixture of biogenic VOCs and anthropogenic VOC than from the sequential addition of the VOCs after approximately the same ageing time. The increase of the scattering component was inversely correlated with the SOA volatility. Two RI retrievals determined for the pure biogenic SOA showed a constant RI for up to 5 h of ageing. Mass spectral characterization shows the three types of the SOA formed in this study have a significant amount of semivolatile components. The influence of anthropogenic VOCs on the oxygenated organic aerosol as well as the atmospheric implications are discussed.

scholarly journals Simulating the detailed chemical composition of secondary organic aerosol formed on a regional scale during the TORCH 2003 campaign in the southern UK

2005 ◽  
Vol 5 (4) ◽  
pp. 7875-7902
Author(s):  
D. Johnson ◽  
S. R. Utembe ◽  
M. E. Jenkin
Keyword(s):  
Chemical Composition ◽  
Secondary Organic Aerosol ◽  
Regional Scale ◽  
Equilibrium Phase ◽  
Organic Aerosol ◽  
Oxidation Products ◽  
Chemical Mechanism ◽  
Phase Partitioning ◽  
Biogenic Voc ◽  
Detailed Chemical

Abstract. Following on from the companion study (Johnson et al., 2005a), a photochemical trajectory model (PTM) has been used to simulate the chemical composition of organic aerosol for selected events during the 2003 TORCH (Tropospheric Organic Chemistry Experiment) field campaign. The PTM incorporates the speciated emissions of 124 non-methane anthropogenic volatile organic compounds (VOC) and three representative biogenic VOC, a highly-detailed representation of the atmospheric degradation of these VOC, the emission of primary organic aerosol (POA) material and the formation of secondary organic aerosol (SOA) material. SOA formation was represented by the transfer of semi- and non-volatile oxidation products from the gas-phase to a condensed organic aerosol-phase, according to estimated thermodynamic equilibrium phase-partitioning characteristics for around 2000 reaction products. After significantly scaling all phase-partitioning coefficients, and assuming a persistent background organic aerosol (both required in order to match the observed organic aerosol loadings), the detailed chemical composition of the simulated SOA has been investigated in terms of intermediate oxygenated species in the Master Chemical Mechanism, version 3.1 (MCM v3.1). For the various case studies considered, 90% of the simulated SOA mass comprises between ca. 70 and 100 multifunctional oxygenated species derived, in varying amounts, from the photooxidation of VOC of anthropogenic and biogenic origin. The anthropogenic contribution is dominated by aromatic hydrocarbons and the biogenic contribution by α- and β-pinene (which also constitute surrogates for other emitted monoterpene species). Sensitivity in the simulated mass of SOA to changes in the emission rates of anthropogenic and biogenic VOC has also been investigated for 11 case study events, and the results have been compared to the detailed chemical composition data. The role of accretion chemistry in SOA formation, and its implications for the results of the present investigation, is discussed.

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