the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Reactive Organic Carbon Air Emissions from Mobile Sources in the United States
Abstract. Mobile sources are responsible for a substantial controllable portion of the reactive organic carbon (ROC) emitted to the atmosphere, especially in urban environments of the United States (U.S.). We update existing methods for calculating mobile source organic particle and vapor emissions in the U.S. with over a decade of laboratory data that parameterize the volatility and organic aerosol (OA) potential of emissions from onroad vehicles, nonroad engines, aircraft, marine vessels, and locomotives. We find that existing emission factor information from teflon filters combined with quartz filters collapses into simple relationships and can be used to reconstruct the complete volatility distribution of ROC emissions. This new approach consists of source-specific filter artifact corrections and state-of-the-science speciation including explicit intermediate volatility organic compounds (IVOCs), yielding the first bottom-up volatility-resolved inventory of U.S. mobile source emissions. Using the Community Multiscale Air Quality model, we estimate mobile sources account for 20–25 % of the IVOC concentrations and 4.4–21.4 % of ambient OA. The updated emissions and air quality model reduce biases in predicting fine-particle organic carbon in winter, spring, and autumn throughout the U.S. (4.3–11.3 % reduction in normalized bias). We identify key uncertain parameters that align with current state-of-the-art research measurement challenges.
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The requested preprint has a corresponding peer-reviewed final revised paper. You are encouraged to refer to the final revised version.
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Preprint
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The requested preprint has a corresponding peer-reviewed final revised paper. You are encouraged to refer to the final revised version.
- Preprint
(1622 KB) - Metadata XML
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Supplement
(3390 KB) - BibTeX
- EndNote
- Final revised paper
Journal article(s) based on this preprint
Interactive discussion
Status: closed
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RC1: 'Comment on egusphere-2023-855', Anonymous Referee #1, 13 Jun 2023
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The authors have constructed comprehensive emission data of organic compounds from mobile sources by utilizing conventional emission data of nonmethane organic gas (NMOG) and particulate organic matter (OM). The developed emission data include information about volatility and detailed chemical composition of organic compounds, and are important basis for accurate simulation of atmospheric PM and O3. This manuscript is well written, and clearly organized.
I recommend this manuscript for publication after the following minor comments are addressed.
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Line 168: I could not follow the procedure for converting OM emissions to CROC emissions. I guess that gas-particle partitioning during filter sampling is critical in this conversion and that sampling temperature and OM concentrations are key parameters. However, you calculate EF_CROC as a function of EF_OM, and you did not consider sampling temperature and OM concentrations in this conversion. Did you assume that EF_OM is proportional to OM concentrations at sources, and that effect of sampling temperature is negligible? I would like this point to be clearly stated.
Line 220: daily-averaged measurements?
Numbering of Figures and Tables should be carefully checked. (e.g., CROC/OM ratio in Line 284 is in Table S6 (not Table S5). Fig. S41 (Line 351) and Fig. S42 (Section S10) are not shown in the Supplementary Material.
Citation: https://doi.org/10.5194/egusphere-2023-855-RC1 -
RC2: 'Comment on egusphere-2023-855', Anonymous Referee #2, 11 Jul 2023
This article aims at detailing the speciation of reactive organic compounds in OM and NMOG emissions. This article provides many details on the specification, which may be very useful for other modellers. However, many papers already estimate reactive organic compound specifications from OM and NMOG emissions, and the introduction does not sufficiently explain what is done in the other papers. Also, for clarity, the measurement biases that this article aims to correct should be introduced and explained in a paragraph in the introduction.
Minor comments :
- Line 60 : Is IVOC more impacted than SVOC for filter artefacts ? Please explain why.
- In the introduction line 64 and thereafter, please detail the main assumption currently used in the litterature to estimate IVOC and SVOC. Although IVOC may be specified from NMVOC or GROC, it may also be directly speciated in the measurements (see for example Sarica et al. Env. Pollution, doi:10.1016/j.envpol.2023.121955)
- What is the advantage to define GROC ? In the methodology defined here, GROC/NMOG ratio and IVOC/GROC ratio with speciation for each of them need to be specified. Why is it better than what is usually done, i.e. simply define a speciation for VOC and determe a IVOC/NMVOC ratio ?
- Line 278 : How are estimated the source-specific adjustment factors ? Where are they detailed ? Table S5 details the volatility profiles (which are key properties for SOA modelling). Where do those come from ? What are the incertainties associated to those profiles ?
Citation: https://doi.org/10.5194/egusphere-2023-855-RC2 - AC1: 'Response to Reviewers: egusphere-2023-855', Ben Murphy, 31 Jul 2023
Interactive discussion
Status: closed
-
RC1: 'Comment on egusphere-2023-855', Anonymous Referee #1, 13 Jun 2023
Â
Â
The authors have constructed comprehensive emission data of organic compounds from mobile sources by utilizing conventional emission data of nonmethane organic gas (NMOG) and particulate organic matter (OM). The developed emission data include information about volatility and detailed chemical composition of organic compounds, and are important basis for accurate simulation of atmospheric PM and O3. This manuscript is well written, and clearly organized.
I recommend this manuscript for publication after the following minor comments are addressed.
Â
Line 168: I could not follow the procedure for converting OM emissions to CROC emissions. I guess that gas-particle partitioning during filter sampling is critical in this conversion and that sampling temperature and OM concentrations are key parameters. However, you calculate EF_CROC as a function of EF_OM, and you did not consider sampling temperature and OM concentrations in this conversion. Did you assume that EF_OM is proportional to OM concentrations at sources, and that effect of sampling temperature is negligible? I would like this point to be clearly stated.
Line 220: daily-averaged measurements?
Numbering of Figures and Tables should be carefully checked. (e.g., CROC/OM ratio in Line 284 is in Table S6 (not Table S5). Fig. S41 (Line 351) and Fig. S42 (Section S10) are not shown in the Supplementary Material.
Citation: https://doi.org/10.5194/egusphere-2023-855-RC1 -
RC2: 'Comment on egusphere-2023-855', Anonymous Referee #2, 11 Jul 2023
This article aims at detailing the speciation of reactive organic compounds in OM and NMOG emissions. This article provides many details on the specification, which may be very useful for other modellers. However, many papers already estimate reactive organic compound specifications from OM and NMOG emissions, and the introduction does not sufficiently explain what is done in the other papers. Also, for clarity, the measurement biases that this article aims to correct should be introduced and explained in a paragraph in the introduction.
Minor comments :
- Line 60 : Is IVOC more impacted than SVOC for filter artefacts ? Please explain why.
- In the introduction line 64 and thereafter, please detail the main assumption currently used in the litterature to estimate IVOC and SVOC. Although IVOC may be specified from NMVOC or GROC, it may also be directly speciated in the measurements (see for example Sarica et al. Env. Pollution, doi:10.1016/j.envpol.2023.121955)
- What is the advantage to define GROC ? In the methodology defined here, GROC/NMOG ratio and IVOC/GROC ratio with speciation for each of them need to be specified. Why is it better than what is usually done, i.e. simply define a speciation for VOC and determe a IVOC/NMVOC ratio ?
- Line 278 : How are estimated the source-specific adjustment factors ? Where are they detailed ? Table S5 details the volatility profiles (which are key properties for SOA modelling). Where do those come from ? What are the incertainties associated to those profiles ?
Citation: https://doi.org/10.5194/egusphere-2023-855-RC2 - AC1: 'Response to Reviewers: egusphere-2023-855', Ben Murphy, 31 Jul 2023
Peer review completion
Journal article(s) based on this preprint
Model code and software
Model Code for Reactive Organic Carbon Air Emissions from Mobile Sources in the United States Benjamin N. Murphy, Havala O. T. Pye https://doi.org/10.5281/zenodo.7869142
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Cited
1 citations as recorded by crossref.
Benjamin N. Murphy
Darrell Sonntag
Karl M. Seltzer
Havala O. T. Pye
Christine Allen
Evan Murray
Claudia Toro
Drew R. Gentner
Cheng Huang
Shantanu H. Jathar
Li Li
Andrew A. May
Allen L. Robinson
The requested preprint has a corresponding peer-reviewed final revised paper. You are encouraged to refer to the final revised version.
- Preprint
(1622 KB) - Metadata XML
-
Supplement
(3390 KB) - BibTeX
- EndNote
- Final revised paper