scholarly journals Investigation of secondary formation of formic acid: urban environment vs. oil and gas producing region

2014 ◽  
Vol 14 (17) ◽  
pp. 24863-24914
Author(s):  
B. Yuan ◽  
P. R. Veres ◽  
C. Warneke ◽  
J. M. Roberts ◽  
J. B. Gilman ◽  
...  
Keyword(s):  
Formic Acid ◽  
Oil And Gas ◽  
Model Performance ◽  
Receptor Site ◽  
Heterogeneous Reactions ◽  
Box Model ◽  
Chemical Mechanism ◽  
Secondary Formation ◽  
June July ◽  
A Site

Abstract. Formic acid (HCOOH) is one of the most abundant carboxylic acids in the atmosphere. However, current photochemical models cannot fully explain observed concentrations and in particular secondary formation of formic acid across various environments. In this work, formic acid measurements made at an urban receptor site in June–July of 2010 during CalNex and a site in an oil and gas producing region in January–February of 2013 during UBWOS 2013 will be discussed. Although the VOC compositions differed dramatically at the two sites, measured formic acid concentrations were comparable: 2.3 ± 1.3 ppb in UBWOS 2013 and 2.0 ± 1.0 ppb in CalNex. We determine that concentrations of formic acid at both sites were dominated by secondary formation (> 8%). A constrained box model using the Master Chemical Mechanism (MCM v3.2) underestimates the measured formic acid concentrations drastically at both sites (by a factor of > 10). Inclusion of recent findings on additional precursors and formation pathways of formic acid in the box model increases modeled formic acid concentrations for UBWOS 2013 and CalNex by a factor of 6.4 and 4.5, respectively. A comparison of measured and modeled HCOOH/acetone ratios is used to evaluate the model performance for formic acid. We conclude that the modified chemical mechanism can explain 21 and 47% of secondary formation of formic acid in UBWOS 2013 and CalNex, respectively. The contributions from aqueous reactions in aerosol and heterogeneous reactions on aerosol surface to formic acid are estimated to be −7 and 0–6% in UBWOS 2013 and CalNex, respectively. We observe that air-snow exchange processes and morning fog events may also contribute to ambient formic acid concentrations during UBWOS 2013 (∼20% in total). In total, 50–57% in UBWOS 2013 and 48–53% in CalNex of secondary formation of formic acid remains unexplained. More work on formic acid formation pathways is needed to reduce the uncertainties in the sources and budget of formic acid and to narrow the gaps between measurements and model results.

scholarly journals Investigation of secondary formation of formic acid: urban environment vs. oil and gas producing region

2015 ◽  
Vol 15 (4) ◽  
pp. 1975-1993 ◽  
Author(s):  
B. Yuan ◽  
P. R. Veres ◽  
C. Warneke ◽  
J. M. Roberts ◽  
J. B. Gilman ◽  
...  
Keyword(s):  
Formic Acid ◽  
Organic Compounds ◽  
Oil And Gas ◽  
Model Performance ◽  
Receptor Site ◽  
Heterogeneous Reactions ◽  
Chemical Mechanism ◽  
Secondary Formation ◽  
June July ◽  
Uintah Basin

Abstract. Formic acid (HCOOH) is one of the most abundant carboxylic acids in the atmosphere. However, current photochemical models cannot fully explain observed concentrations and in particular secondary formation of formic acid across various environments. In this work, formic acid measurements made at an urban receptor site (Pasadena) in June–July 2010 during CalNex (California Research at the Nexus of Air Quality and Climate Change) and a site in an oil and gas producing region (Uintah Basin) in January–February 2013 during UBWOS 2013 (Uintah Basin Winter Ozone Studies) will be discussed. Although the VOC (volatile organic compounds) compositions differed dramatically at the two sites, measured formic acid concentrations were comparable: 2.3 ± 1.3 in UBWOS 2013 and 2.0 ± 1.0 ppb in CalNex. We determine that concentrations of formic acid at both sites were dominated by secondary formation (> 99%). A constrained box model using the Master Chemical Mechanism (MCM v3.2) underestimates the measured formic acid concentrations drastically at both sites (by a factor of > 10). Compared to the original MCM model that includes only ozonolysis of unsaturated organic compounds and OH oxidation of acetylene, when we updated yields of ozonolysis of alkenes and included OH oxidation of isoprene, vinyl alcohol chemistry, reaction of formaldehyde with HO2, oxidation of aromatics, and reaction of CH3O2 with OH, the model predictions for formic acid were improved by a factor of 6.4 in UBWOS 2013 and 4.5 in CalNex, respectively. A comparison of measured and modeled HCOOH/acetone ratios is used to evaluate the model performance for formic acid. We conclude that the modified chemical mechanism can explain 19 and 45% of secondary formation of formic acid in UBWOS 2013 and CalNex, respectively. The contributions from aqueous reactions in aerosol and heterogeneous reactions on aerosol surface to formic acid are estimated to be 0–6 and 0–5% in UBWOS 2013 and CalNex, respectively. We observe that air–snow exchange processes and morning fog events may also contribute to ambient formic acid concentrations during UBWOS 2013 (~ 20% in total). In total, 53–59 in UBWOS 2013 and 50–55% in CalNex of secondary formation of formic acid remains unexplained. More work on formic acid formation pathways is needed to reduce the uncertainties in the sources and budget of formic acid and to narrow the gaps between measurements and model results.

scholarly journals Secondary formation of nitrated phenols: insights from observations during the Uintah Basin Winter Ozone Study (UBWOS) 2014

2015 ◽  
Vol 15 (20) ◽  
pp. 28659-28697 ◽  
Author(s):  
B. Yuan ◽  
J. Liggio ◽  
J. Wentzell ◽  
S.-M. Li ◽  
H. Stark ◽  
...  
Keyword(s):  
Gas Phase ◽  
Oil And Gas ◽  
Gas Production ◽  
Heterogeneous Reactions ◽  
Box Model ◽  
Ionization Mass ◽  
Oil And Gas Production ◽  
Production Region ◽  
Secondary Formation ◽  
Online Measurements

Abstract. We describe the results from online measurements of nitrated phenols using a time of flight chemical ionization mass spectrometer (ToF-CIMS) with acetate as reagent ion in an oil and gas production region in January and February of 2014. Strong diurnal profiles were observed for nitrated phenols, with concentration maxima at night. Based on known markers (CH4, NOx, CO2), primary emissions of nitrated phenols were not important in this study. A box model was used to simulate secondary formation of phenol, nitrophenol (NP) and dinitrophenols (DNP). The box model results indicate that oxidation of aromatics in the gas phase can explain the observed concentrations of NP and DNP in this study. Photolysis was the most efficient loss pathway for NP in the gas phase. We show that aqueous-phase reactions and heterogeneous reactions were minor sources of nitrated phenols in our study. This study demonstrates that the emergence of new ToF-CIMS (including PTR-TOF) techniques allows for the measurement of intermediate oxygenates at low levels and these measurements improve our understanding of the evolution of primary VOCs in the atmosphere.

scholarly journals Secondary formation of nitrated phenols: insights from observations during the Uintah Basin Winter Ozone Study (UBWOS) 2014

2016 ◽  
Vol 16 (4) ◽  
pp. 2139-2153 ◽  
Author(s):  
Bin Yuan ◽  
John Liggio ◽  
Jeremy Wentzell ◽  
Shao-Meng Li ◽  
Harald Stark ◽  
...  
Keyword(s):  
Gas Phase ◽  
Oil And Gas ◽  
Gas Production ◽  
Heterogeneous Reactions ◽  
Box Model ◽  
Ionization Mass ◽  
Oil And Gas Production ◽  
Production Region ◽  
Secondary Formation ◽  
Online Measurements

Abstract. We describe the results from online measurements of nitrated phenols using a time-of-flight chemical ionization mass spectrometer (ToF-CIMS) with acetate as reagent ion in an oil and gas production region in January and February of 2014. Strong diurnal profiles were observed for nitrated phenols, with concentration maxima at night. Based on known markers (CH4, NOx, CO2), primary emissions of nitrated phenols were not important in this study. A box model was used to simulate secondary formation of phenol, nitrophenol (NP), and dinitrophenols (DNP). The box model results indicate that oxidation of aromatics in the gas phase can explain the observed concentrations of NP and DNP in this study. Photolysis was the most efficient loss pathway for NP in the gas phase. We show that aqueous-phase reactions and heterogeneous reactions were minor sources of nitrated phenols in our study. This study demonstrates that the emergence of new ToF-CIMS (including PTR-TOF) techniques allows for the measurement of intermediate oxygenates at low levels and these measurements improve our understanding on the evolution of primary VOCs in the atmosphere.

scholarly journals A fast stratospheric chemistry solver: the E4CHEM submodel for the atmospheric chemistry global circulation model EMAC

2010 ◽  
Vol 3 (1) ◽  
pp. 321-328 ◽  
Author(s):  
A. J. G. Baumgaertner ◽  
P. Jöckel ◽  
B. Steil ◽  
H. Tost ◽  
R. Sander
Keyword(s):  
Atmospheric Chemistry ◽  
General Circulation ◽  
Circulation Model ◽  
Reaction Rates ◽  
Heterogeneous Reactions ◽  
Tropospheric Chemistry ◽  
Box Model ◽  
Chemical Mechanism ◽  
Global Circulation Model ◽  
Stratospheric Chemistry

Abstract. The atmospheric chemistry general circulation model ECHAM5/MESSy (EMAC) and the atmospheric chemistry box model CAABA are extended by a computationally very efficient submodel for atmospheric chemistry, E4CHEM. It focuses on stratospheric chemistry but also includes background tropospheric chemistry. It is based on the chemistry of MAECHAM4-CHEM and is intended to serve as a simple and fast alternative to the flexible but also computationally more demanding submodel MECCA. In a model setup with E4CHEM, EMAC is now also suitable for simulations of longer time scales. The reaction mechanism contains basic O3, CH4, CO, HOx, NOx, and ClOx gas phase chemistry. In addition, E4CHEM includes optional fast routines for heterogeneous reactions on sulphate aerosols and polar stratospheric clouds (substituting the existing submodels PSC and HETCHEM), and scavenging (substituting the existing submodel SCAV). We describe the implementation of E4CHEM into the MESSy structure of CAABA and EMAC. For some species the steady state in the box model differs by up to 100% when compared to results from CAABA/MECCA due to different reaction rates. After an update of the reaction rates in E4CHEM the mixing ratios in both boxmodel and 3-D model simulations are in satisfactory agreement with the results from a simulation where MECCA with a similar chemistry scheme was employed. Finally, a comparison against a simulation with a more complex and already evaluated chemical mechanism is presented in order to discuss shortcomings associated with the simplification of the chemical mechanism.

scholarly journals Understanding the primary emissions and secondary formation of gaseous organic acids in the oil sands region of Alberta, Canada

2017 ◽  
Vol 17 (13) ◽  
pp. 8411-8427 ◽  
Author(s):  
John Liggio ◽  
Samar G. Moussa ◽  
Jeremy Wentzell ◽  
Andrea Darlington ◽  
Peter Liu ◽  
...  
Keyword(s):  
Molecular Weight ◽  
Organic Acids ◽  
Organic Acid ◽  
Oil Sands ◽  
Box Model ◽  
Chemical Mechanism ◽  
Formation Mechanisms ◽  
Low Molecular Weight ◽  
Airborne Measurements ◽  
Secondary Formation

Abstract. Organic acids are known to be emitted from combustion processes and are key photochemical products of biogenic and anthropogenic precursors. Despite their multiple environmental impacts, such as on acid deposition and human–ecosystem health, little is known regarding their emission magnitudes or detailed chemical formation mechanisms. In the current work, airborne measurements of 18 gas-phase low-molecular-weight organic acids were made in the summer of 2013 over the oil sands region of Alberta, Canada, an area of intense unconventional oil extraction. The data from these measurements were used in conjunction with emission retrieval algorithms to derive the total and speciated primary organic acid emission rates, as well as secondary formation rates downwind of oil sands operations. The results of the analysis indicate that approximately 12 t day−1 of low-molecular-weight organic acids, dominated by C1–C5 acids, were emitted directly from off-road diesel vehicles within open pit mines. Although there are no specific reporting requirements for primary organic acids, the measured emissions were similar in magnitude to primary oxygenated hydrocarbon emissions, for which there are reporting thresholds, measured previously ( ≈  20 t day−1). Conversely, photochemical production of gaseous organic acids significantly exceeded the primary sources, with formation rates of up to  ≈  184 t day−1 downwind of the oil sands facilities. The formation and evolution of organic acids from a Lagrangian flight were modelled with a box model, incorporating a detailed hydrocarbon reaction mechanism extracted from the Master Chemical Mechanism (v3.3). Despite evidence of significant secondary organic acid formation, the explicit chemical box model largely underestimated their formation in the oil sands plumes, accounting for 39, 46, 26, and 23 % of the measured formic, acetic, acrylic, and propionic acids respectively and with little contributions from biogenic VOC precursors. The model results, together with an examination of the carbon mass balance between the organic acids formed and the primary VOCs emitted from oil sands operations, suggest the existence of significant missing secondary sources and precursor emissions related to oil sands and/or an incomplete mechanistic and quantitative understanding of how they are processed in the atmosphere.

scholarly journals Ozone photochemistry in an oil and natural gas extraction region during winter: simulations of a snow-free season in the Uintah Basin, Utah

2013 ◽  
Vol 13 (17) ◽  
pp. 8955-8971 ◽  
Author(s):  
P. M. Edwards ◽  
C. J. Young ◽  
K. Aikin ◽  
J. deGouw ◽  
W. P. Dubé ◽  
...  
Keyword(s):  
Oil And Gas ◽  
Box Model ◽  
Chemical Mechanism ◽  
Gas Extraction ◽  
Nox Emissions ◽  
Oil And Gas Development ◽  
Model Simulations ◽  
Primary Radical ◽  
Radical Production ◽  
Uintah Basin

Abstract. The Uintah Basin in northeastern Utah, a region of intense oil and gas extraction, experienced ozone (O3) concentrations above levels harmful to human health for multiple days during the winters of 2009–2010 and 2010–2011. These wintertime O3 pollution episodes occur during cold, stable periods when the ground is snow-covered, and have been linked to emissions from the oil and gas extraction process. The Uintah Basin Winter Ozone Study (UBWOS) was a field intensive in early 2012, whose goal was to address current uncertainties in the chemical and physical processes that drive wintertime O3 production in regions of oil and gas development. Although elevated O3 concentrations were not observed during the winter of 2011–2012, the comprehensive set of observations tests our understanding of O3 photochemistry in this unusual emissions environment. A box model, constrained to the observations and using the near-explicit Master Chemical Mechanism (MCM) v3.2 chemistry scheme, has been used to investigate the sensitivities of O3 production during UBWOS 2012. Simulations identify the O3 production photochemistry to be highly radical limited (with a radical production rate significantly smaller than the NOx emission rate). Production of OH from O3 photolysis (through reaction of O(1D) with water vapor) contributed only 170 pptv day−1, 8% of the total primary radical source on average (primary radicals being those produced from non-radical precursors). Other radical sources, including the photolysis of formaldehyde (HCHO, 52%), nitrous acid (HONO, 26%), and nitryl chloride (ClNO2, 13%) were larger. O3 production was also found to be highly sensitive to aromatic volatile organic compound (VOC) concentrations, due to radical amplification reactions in the oxidation scheme of these species. Radical production was shown to be small in comparison to the emissions of nitrogen oxides (NOx), such that NOx acted as the primary radical sink. Consequently, the system was highly VOC sensitive, despite the much larger mixing ratio of total non-methane hydrocarbons (230 ppbv (2080 ppbC), 6 week average) relative to NOx (5.6 ppbv average). However, the importance of radical sources which are themselves derived from NOx emissions and chemistry, such as ClNO2 and HONO, make the response of the system to changes in NOx emissions uncertain. Model simulations attempting to reproduce conditions expected during snow-covered cold-pool conditions show a significant increase in O3 production, although calculated concentrations do not achieve the highest seen during the 2010–2011 O3 pollution events in the Uintah Basin. These box model simulations provide useful insight into the chemistry controlling winter O3 production in regions of oil and gas extraction.

scholarly journals A fast stratospheric chemistry solver: the E4CHEM submodel for the atmospheric chemistry global circulation model EMAC

2010 ◽  
Vol 3 (1) ◽  
pp. 181-200
Author(s):  
A. J. G. Baumgaertner ◽  
P. Jöckel ◽  
B. Steil ◽  
H. Tost ◽  
R. Sander
Keyword(s):  
Atmospheric Chemistry ◽  
General Circulation ◽  
Circulation Model ◽  
Reaction Rates ◽  
Heterogeneous Reactions ◽  
Tropospheric Chemistry ◽  
Box Model ◽  
Chemical Mechanism ◽  
Global Circulation Model ◽  
Stratospheric Chemistry

Abstract. The atmospheric chemistry general circulation model ECHAM5/MESSy (EMAC) and the atmospheric chemistry box model CAABA are extended by a computationally very efficient submodel for atmospheric chemistry, E4CHEM. It focuses on stratospheric chemistry but also includes background tropospheric chemistry. It is based on the chemistry of MAECHAM4-CHEM and is intended to serve as a simple and fast alternative to the flexible but also computationally more demanding submodel MECCA. In a model setup with E4CHEM, EMAC is now also suitable for simulations of longer time scales. The reaction mechanism contains basic O3, CH4, CO, HOx, NOx and ClOx gas phase chemistry. In addition, E4CHEM includes optional fast routines for heterogeneous reactions on sulphate aerosols and polar stratospheric clouds (substituting the existing submodels PSC and HETCHEM), and scavenging (substituting the existing submodel SCAV). We describe the implementation of E4CHEM into the MESSy structure of CAABA and EMAC. For some species the steady state in the box model differs by up to 100% when compared to results from CAABA/MECCA due to different reaction rates. After an update of the reaction rates in E4CHEM the mixing ratios in both boxmodel and 3-D model simulations are in satisfactory agreement with the results from a simulation where MECCA with a similar chemistry scheme was employed. Finally, a comparison against a simulation with a more complex and already evaluated chemical mechanism is presented in order to discuss shortcomings associated with the simplification of the chemical mechanism.

scholarly journals Understanding the Primary Emissions and Secondary Formation of Gaseous Organic Acids in the Oil Sands Region of Alberta, Canada

2017 ◽  
Author(s):  
John Liggio ◽  
Samar G. Moussa ◽  
Jeremy Wentzell ◽  
Andrea Darlington ◽  
Peter Liu ◽  
...  
Keyword(s):  
Molecular Weight ◽  
Organic Acids ◽  
Organic Acid ◽  
Oil Sands ◽  
Box Model ◽  
Chemical Mechanism ◽  
Formation Mechanisms ◽  
Low Molecular Weight ◽  
Airborne Measurements ◽  
Secondary Formation

Abstract. Organic acids are known to be emitted from combustion processes and are key photochemical products of biogenic and anthropogenic precursors. Despite their multiple environmental impacts, such as on acid deposition and human/ecosystem health, little is known regarding their emission magnitudes or detailed chemical formation mechanisms. In the current work, airborne measurements of 18 gas-phase low molecular weight organic acids were made in the summer of 2013 over the oil sands region of Alberta, Canada, an area of intense unconventional oil extraction. The data from these measurements were used in conjunction with emission retrieval algorithms to derive the total and speciated primary organic acid emission rates, as well as secondary formation rates downwind of oil sands operations. The results of the analysis indicate that approximately 12 tonnes day−1 of low molecular weight organic acids, dominated by C1–C5 acids, were emitted directly from off-road diesel vehicles within open pit mines. Although there are no specific reporting requirements for primary organic acids, the measured emissions were similar in magnitude to primary oxygenated hydrocarbon emissions measured previously (≈ 20 tonnes day−1), for which there are reporting thresholds. Conversely, photochemical production of gaseous organic acids significantly exceeded the primary sources, with formation rates up to ≈ 184 tonnes day−1 downwind of the oil sands facilities. The formation and evolution of organic acids from a Lagrangian flight were modeled with a box model, incorporating a detailed hydrocarbon reaction mechanism extracted from the Master Chemical Mechanism (v 3.3). Despite evidence of significant secondary organic acid formation, the explicit chemical box model largely underestimated their formation in the oil sands plumes, accounting for 39 %, 46 %, 26 % and 23 % of the measured formic, acetic, acrylic and propionic acids respectively, and with little contributions from biogenic VOC precursors. The model results, together with an examination of the carbon mass balance between the organic acids formed and the primary VOCs emitted from oils sands operations, suggest the existence of significant missing oil sands related secondary sources/precursor emissions and/or an incomplete mechanistic and quantitative understanding of how they are processed in the atmosphere.

scholarly journals Ozone photochemistry in an oil and natural gas extraction region during winter: simulations of a snow-free season in the Uintah Basin, Utah

2013 ◽  
Vol 13 (3) ◽  
pp. 7503-7552 ◽  
Author(s):  
P. M. Edwards ◽  
C. J. Young ◽  
K. Aikin ◽  
J. A. deGouw ◽  
W. P. Dubé ◽  
...  
Keyword(s):  
Oil And Gas ◽  
Extraction Process ◽  
Box Model ◽  
Chemical Mechanism ◽  
Gas Extraction ◽  
Nox Emissions ◽  
Oil And Gas Development ◽  
Primary Radical ◽  
Extraction Region ◽  
Uintah Basin

Abstract. The Uintah Basin in northeastern Utah, a region of intense oil and gas extraction, experienced ozone (O3) concentrations above levels harmful to human health for multiple days during the winters of 2009–2010 and 2010–2011. These wintertime O3 pollution episodes occur during cold, stable periods when the ground is snowcovered, and have been linked to emissions from the oil and gas extraction process. The Uintah Basin Winter Ozone Study (UBWOS) was a field intensive in early 2012, whose goal was to address current uncertainties in the chemical and physical processes that drive wintertime O3 production in regions of oil and gas development. Although elevated O3 concentrations were not observed during the winter of 2011–2012, the comprehensive set of observations tests of our understanding of O3 photochemistry in this unusual emissions environment. A box model, constrained to the observations and using the explicit Master Chemical Mechanism (MCM) V3.2 chemistry scheme, has been used to investigate the sensitivities of O3 production during UBWOS 2012. Simulations identify the O3 production photochemistry to be highly radical limited. Production of OH from O3 photolysis (through reaction of O(1D) with water vapor) contributed only 170 pptv day−1, 8% of the total primary radical source on average. Other radical sources, including the photolysis of formaldehyde (HCHO, 52%), nitrous acid (HONO, 26%), and nitryl chloride (ClNO2, 13%) were larger. O3 production was also found to be highly sensitive to aromatic volatile organic compound (VOC) concentrations, due to radical amplification reactions in the oxidation scheme of these species. Radical production was shown to be small in comparison to the emissions of nitrogen oxides (NOx), such that NOx acted as the primary radical sink. Consequently, the system was highly VOC sensitive, despite the much larger mixing ratio of total non-methane hydrocarbons (230 ppbv (2080 ppbC), 6 week average) relative to NOx (5.6 ppbv average). However, the importance of radical sources which are themselves derived from NOx emissions and chemistry, such as ClNO2 and HONO, make the response of the system to changes in NOx emissions uncertain. These box model simulations provide useful insight into the chemistry controlling winter O3 production in regions of oil and gas extraction.

scholarly journals NO<sub>x</sub> and O<sub>3</sub> above a tropical rainforest: an analysis with a global and box model

2010 ◽  
Vol 10 (21) ◽  
pp. 10607-10620 ◽  
Author(s):  
R. C. Pike ◽  
J. D. Lee ◽  
P. J. Young ◽  
G. D. Carver ◽  
X. Yang ◽  
...  
Keyword(s):  
Transport Model ◽  
Model Performance ◽  
Global Model ◽  
Box Model ◽  
Chemical Mechanism ◽  
Chemistry Transport Model ◽  
Basic Model ◽  
Surface Measurements ◽  
Cross Platform ◽  
Malaysian Borneo

Abstract. A cross-platform field campaign, OP3, was conducted in the state of Sabah in Malaysian Borneo between April and July of 2008. Among the suite of observations recorded, the campaign included measurements of NOx and O3 – crucial outputs of any model chemistry mechanism. We describe the measurements of these species made from both the ground site and aircraft. We then use the output from two resolutions of the chemistry transport model p-TOMCAT to illustrate the ability of a global model chemical mechanism to capture the chemistry at the rainforest site. The basic model performance is good for NOx and poor for ozone. A box model containing the same chemical mechanism is used to explore the results of the global model in more depth and make comparisons between the two. Without some parameterization of the nighttime boundary layer – free troposphere mixing (i.e. the use of a dilution parameter), the box model does not reproduce the observations, pointing to the importance of adequately representing physical processes for comparisons with surface measurements. We conclude with a discussion of box model budget calculations of chemical reaction fluxes, deposition and mixing, and compare these results to output from p-TOMCAT. These show the same chemical mechanism behaves similarly in both models, but that emissions and advection play particularly strong roles in influencing the comparison to surface measurements.

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