the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
| 26 Jan 2023
Coarse particulate matter air quality in East Asia: implications for fine particulate nitrate
Daniel J. Jacob
Drew C. Pendergrass
Nadia K. Colombi
Viral Shah
Laura Hyesung Yang
Qiang Zhang
Shuxiao Wang
Hwajin Kim
Jin-Soo Choi
Jin-Soo Park
Fangqun Yu
Jung-Hun Woo
Younha Kim
Jack E. Dibb
Taehyoung Lee
Jin-Seok Han
Bruce E. Anderson
Hong Liao
Abstract. Air quality network data in China and South Korea show very high year-round mass concentrations of coarse particulate matter (PM), as inferred by difference between PM10 and PM2.5. Coarse PM concentrations in 2015 averaged 52 μg m-3 in the North China Plain (NCP) and 23 μg m-3 in the Seoul Metropolitan Area (SMA), contributing nearly half of PM10. Strong daily correlations between coarse PM and carbon monoxide imply a dominant source from anthropogenic fugitive dust. Coarse PM concentrations in the NCP and the SMA decreased by 21 % from 2015 to 2019 and further dropped abruptly in 2020 due to COVID-19 reductions in construction and vehicle traffic. Anthropogenic coarse PM is generally not included in air quality models but scavenges nitric acid to suppress the formation of fine particulate nitrate, a major contributor to PM2.5 pollution. GEOS-Chem model simulation of surface and aircraft observations from the KORUS-AQ campaign over the SMA in May–June 2016 shows that consideration of anthropogenic coarse PM largely resolves the previous model overestimate of fine particulate nitrate. The effect is smaller in the NCP which has a larger excess of ammonia. Model sensitivity simulations show that decreasing anthropogenic coarse PM over 2015–2019 directly increases PM2.5 nitrate in summer, offsetting half the effect of other emission controls, while in winter it increases the sensitivity of PM2.5 nitrate to ammonia and sulfur dioxide emissions. Decreasing coarse PM helps to explain the flat wintertime PM2.5 nitrate trends observed in the NCP and the SMA despite decreases in nitrogen oxides and ammonia emissions. The continuing decrease of coarse PM from abating fugitive dust pollution will require more stringent nitrogen oxides and ammonia emission controls to successfully decrease PM2.5 nitrate.
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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
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Supplement
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- Final revised paper
Journal article(s) based on this preprint
Shixian Zhai et al.
Interactive discussion
Status: closed
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RC1: 'Comment on egusphere-2022-1485', Anonymous Referee #2, 18 Feb 2023
Zhai et al. present a novel perspective on the impact of coarse particulate matter (PM) on the formation of fine PM nitrate in the North China Plain and the Seoul Metropolitan Area. The authors report that anthropogenic coarse PM, particularly fugitive dust from construction, which has not been considered in atmospheric chemical transport models, is capable of more efficiently absorbing gas-phase nitrate acid during the summer, resulting in a suppression of fine PM nitrate formation. Consequently, reducing emissions of coarse PM could lead to an unanticipated increase in fine PM nitrate levels, despite the decrease in NOx and NH3 emissions. The findings suggest the need for more extraordinary efforts to control NOx and NH3 emissions as fugitive dust pollution is controlled. The manuscript is well-organized, and the conclusions drawn are solid and well-supported by the data and simulation results. Therefore, I recommend the manuscript for acceptance with minimal revisions.
1. While the manuscript clearly outlines the relationships between coarse PM, fine PM, and gas-phase NOx and NH3, it would be helpful for readers if the authors could provide a diagram illustrating the tradeoffs associated with reducing emissions of coarse PM and NOx/NH3.
2. Line 160 suggests that the absorption of HNO3 by coarse PM is three times more efficient than dry deposition, with alkalinity not being a limiting factor. However, it is not clear what the limiting factor is. Given that the available surface area typically restricts reactive uptake, the authors could provide clarification on how the surface area of coarse PM compares to that of fine PM, and which factor (e.g., surface area, chemical composition, relative humidity/temperature, etc.) limits the simulation.
Citation: https://doi.org/10.5194/egusphere-2022-1485-RC1 -
RC2: 'Comment on egusphere-2022-1485', Anonymous Referee #1, 19 Feb 2023
This paper presents an interesting analysis of the influence of coarse mode aerosol on the distribution of nitrate in the East Asian atmosphere. They use detailed aircraft and ground measurements during KORUS-AQ to show that a significant amount of nitrate appears to be associated with coarse mode particles and that including a more realistic representation of coarse mode particles reduces the GEOS-Chem model’s high bias in fine mode nitrate. The analysis is also extended to simulations over the North China Plain. Overall the data and interpretation are clearly presented and I think the paper should be published following some clarifications, as requested below.
I found it difficult to follow the description of the approach for including coarse mode particles in the model on lines 142-147. Were the network observations applied as emissions or concentrations? How did the inclusion of the coarse mode in the lowest model level influence higher altitudes in the model domain? Was the linear interpolation in time, space?
The authors should clarify the definition of PM1-4 nitrate from the DC-8 observations. The AMS only measures submicron semi-volatile nitrate whereas the SAGA measures all PM4 nitrate. It appears, though is not stated, that the difference between the SAGA and AMS nitrate measurements is used to define PM1-4 nitrate. What if there is refractory PM1 nitrate? Figure S2 does not rule out this possibility because the AMS would likely not be sensitive to nitrate associated with refractory minerals in dust. What if there is semi-volatile supermicron nitrate? Would this impact the measurement model comparisons (it’s unclear from line 151 if the model nitrate is PM1 or any ammonium nitrate)? These details are unlikely to impact the qualitative outcomes of the analysis, but it would be useful to have more precision in the definitions.
Related to the points above, the authors note that the impact of including coarse mode aerosol that can uptake HNO3 is less impactful in the NCP, but in this example they compare PM2.5 nitrate rather than PM1 nitrate. Very little is said about the observations from China, but are these measurements limited to semi-volatile nitrate, or would they also include dust nitrate in the fine mode?
In the analysis of the overall sensitivity of fine mode nitrate to recent emissions trends, the authors explain the more modest sensitivity of nitrate to dust by the abundance of NH3 and kinetic arguments about mass transfer (lines 207-212). I find this surprising as I would assume that in the model the ammonium nitrate remains semi-volatile, whereas the coarse nitrate formation is irreversible. In that case, it doesn’t matter how quickly the ammonium nitrate forms, given sufficient time the presence of a reactive coarse mode would still siphon off fine mode nitrate, unless there are other competing sinks?
Citation: https://doi.org/10.5194/egusphere-2022-1485-RC2 - AC1: 'Comment on egusphere-2022-1485', Shixian Zhai, 16 Mar 2023
Interactive discussion
Status: closed
-
RC1: 'Comment on egusphere-2022-1485', Anonymous Referee #2, 18 Feb 2023
Zhai et al. present a novel perspective on the impact of coarse particulate matter (PM) on the formation of fine PM nitrate in the North China Plain and the Seoul Metropolitan Area. The authors report that anthropogenic coarse PM, particularly fugitive dust from construction, which has not been considered in atmospheric chemical transport models, is capable of more efficiently absorbing gas-phase nitrate acid during the summer, resulting in a suppression of fine PM nitrate formation. Consequently, reducing emissions of coarse PM could lead to an unanticipated increase in fine PM nitrate levels, despite the decrease in NOx and NH3 emissions. The findings suggest the need for more extraordinary efforts to control NOx and NH3 emissions as fugitive dust pollution is controlled. The manuscript is well-organized, and the conclusions drawn are solid and well-supported by the data and simulation results. Therefore, I recommend the manuscript for acceptance with minimal revisions.
1. While the manuscript clearly outlines the relationships between coarse PM, fine PM, and gas-phase NOx and NH3, it would be helpful for readers if the authors could provide a diagram illustrating the tradeoffs associated with reducing emissions of coarse PM and NOx/NH3.
2. Line 160 suggests that the absorption of HNO3 by coarse PM is three times more efficient than dry deposition, with alkalinity not being a limiting factor. However, it is not clear what the limiting factor is. Given that the available surface area typically restricts reactive uptake, the authors could provide clarification on how the surface area of coarse PM compares to that of fine PM, and which factor (e.g., surface area, chemical composition, relative humidity/temperature, etc.) limits the simulation.
Citation: https://doi.org/10.5194/egusphere-2022-1485-RC1 -
RC2: 'Comment on egusphere-2022-1485', Anonymous Referee #1, 19 Feb 2023
This paper presents an interesting analysis of the influence of coarse mode aerosol on the distribution of nitrate in the East Asian atmosphere. They use detailed aircraft and ground measurements during KORUS-AQ to show that a significant amount of nitrate appears to be associated with coarse mode particles and that including a more realistic representation of coarse mode particles reduces the GEOS-Chem model’s high bias in fine mode nitrate. The analysis is also extended to simulations over the North China Plain. Overall the data and interpretation are clearly presented and I think the paper should be published following some clarifications, as requested below.
I found it difficult to follow the description of the approach for including coarse mode particles in the model on lines 142-147. Were the network observations applied as emissions or concentrations? How did the inclusion of the coarse mode in the lowest model level influence higher altitudes in the model domain? Was the linear interpolation in time, space?
The authors should clarify the definition of PM1-4 nitrate from the DC-8 observations. The AMS only measures submicron semi-volatile nitrate whereas the SAGA measures all PM4 nitrate. It appears, though is not stated, that the difference between the SAGA and AMS nitrate measurements is used to define PM1-4 nitrate. What if there is refractory PM1 nitrate? Figure S2 does not rule out this possibility because the AMS would likely not be sensitive to nitrate associated with refractory minerals in dust. What if there is semi-volatile supermicron nitrate? Would this impact the measurement model comparisons (it’s unclear from line 151 if the model nitrate is PM1 or any ammonium nitrate)? These details are unlikely to impact the qualitative outcomes of the analysis, but it would be useful to have more precision in the definitions.
Related to the points above, the authors note that the impact of including coarse mode aerosol that can uptake HNO3 is less impactful in the NCP, but in this example they compare PM2.5 nitrate rather than PM1 nitrate. Very little is said about the observations from China, but are these measurements limited to semi-volatile nitrate, or would they also include dust nitrate in the fine mode?
In the analysis of the overall sensitivity of fine mode nitrate to recent emissions trends, the authors explain the more modest sensitivity of nitrate to dust by the abundance of NH3 and kinetic arguments about mass transfer (lines 207-212). I find this surprising as I would assume that in the model the ammonium nitrate remains semi-volatile, whereas the coarse nitrate formation is irreversible. In that case, it doesn’t matter how quickly the ammonium nitrate forms, given sufficient time the presence of a reactive coarse mode would still siphon off fine mode nitrate, unless there are other competing sinks?
Citation: https://doi.org/10.5194/egusphere-2022-1485-RC2 - AC1: 'Comment on egusphere-2022-1485', Shixian Zhai, 16 Mar 2023
Peer review completion
Journal article(s) based on this preprint
Shixian Zhai et al.
Shixian Zhai et al.
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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
(1533 KB) - Metadata XML
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Supplement
(661 KB) - BibTeX
- EndNote
- Final revised paper