the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
| 22 Jan 2024
Source-resolved atmospheric metal emissions, concentrations, and their deposition fluxes into the East Asian Seas
Abstract. Atmospheric deposition is an important source of marine metallic elements, which have a non-negligible impact on marine ecology. Atmospheric trace metals come from different sources, undergo their respective transport processes, and are deposited into seas finally. This study aims to provide gridded data on sea-wide concentrations, deposition fluxes, and soluble deposition fluxes with detailed source categories of metals by the modified Community Multiscale Air Quality (CMAQ) model. A monthly emission inventory of six metals – Fe, Al, V, Ni, Zn, and Cu – from land anthropogenic, ship, and dust sources in East Asia (0–55° N, 85–150° E) in 2017 was developed. Most metals came mainly from land-based sources, contributing over 80 %. The annual marine atmospheric deposition fluxes of Fe, Al, V, Ni, Zn, and Cu were 9614, 15000, 102, 84, 171, 88 μg·m-2, and soluble deposition fluxes were 646.8, 1799.6, 43.3, 36.3, 118.4, 42.9 μg·m-2, respectively. Contributions of each source for trace metals varied in emissions, atmospheric concentrations, and depositions. Dust source, as a main contributor of Fe and Al, accounted for a higher proportion of emissions (~90 %) than marine deposition fluxes (~20 %). However, anthropogenic sources have larger shares of marine deposition flux compared with emissions. The deposition of Zn, Cu, and soluble Fe in East Asian seas was dominated by land anthropogenic sources, while V and Ni were dominated by shipping. The seasonal gridded data and the identification of the dominant source of metal deposition offer a foundation for dynamic assessments of the marine ecological effects of atmospheric trace metals. This study also implies the importance of potential co-synthesis and complementation effects of multiple trace elements deposited into marine ecosystems.
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Notice on discussion status
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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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
(944 KB) - BibTeX
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- Final revised paper
Journal article(s) based on this preprint
Interactive discussion
Status: closed
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RC1: 'Comment on egusphere-2024-155', Anonymous Referee #1, 23 Feb 2024
General comments:
The manuscript of egusphere-2024-155 entitled “Source-resolved atmospheric metal emissions, concentrations, and their deposition fluxes into the East Asian Seas” presented the development of source-specific emission inventory for metals (Fe, Al, Cu, V, Ni, and Zn) and further conducted the model simulations to estimate ambient concentrations and depositions over East Asia. The importance of this kind of study is understandable, and I generally agree with the possible publication. However, I have one major concern as follows, and relevant discussions are required to be fully amended.
Major concern:
- Development of emission inventory (Sections 2.2 and 3.1): I can follow the methodology itself; however, we should recognize that dust emission can largely varied year-to-year. From the simulation, only four months (January, April, July, and October) were conducted, but annual emissions were presented in Fig. 1. How did the authors estimate annual total emissions? Or, the covering spring time is enough to calculate the annual total emissions as stated? Moreover, this study targeted the year of 2017, but why? The estimated dust emissions were possible maxima/minima or average situation for Asia dust? These details explanations are required to follow this study.
Specific comments:
- Line 30: The component of trace metals should be first defined in the first appearance (not in the second sentence).
- Line 49: A high temperature of aerosol itself? Please clarify.
- Line 58-63: But this study was conducted over East Asia. This paragraph seems to be mainly focused on the Southern Ocean. The motivation for East Asia is also required to understand the introduction of this study.
- Line 78 or Line 84: The relevant information (e.g., doi of zenodo) for the original CMAQ modeling system itself is needed here.
- Line 84-90: Because this study analyzed deposition, a description of the deposition scheme in the CMAQ should be presented.
- Line 121: I guess the inline dust module in the CMAQ for Foroutan et al. (2017) (doi:10.1002/2016MS000823) is required, or did the authors develop their models?
- Line 131-133: I do not fully understand this sentence.
- Line 185: Before starting this section 3.1.2, it would be better to mention Fig. 2 at first (not in Line 201).
- Line 215-218: In addition to the targeted seas such as ECS explained here, further discussion focusing on the springtime would clarify the importance of dust emissions.
- Line 228-230 (the caption of Figure 3) and the relevant discussion: I do not follow why this estimation is expressed as the total annual mean concentration. Because this study was only conducted for four months, even though these are representative months of each season, the wording “annual mean” will be overstated. In addition to this question, what is the meaning of “total”? If this is the total concentration, the concentration for the “ALL” region should be the sum of all ocean areas. Please clarify these expressions and the actual analyzed contents.
- Line 257-260 (the caption of Figure 4) and the relevant discussion: Same comment to the above comment on Line 228-230.
- Line 288-313: Again, why these estimations can be explained as annual amounts? Taking into consideration the important role of Asian dust in spring, how about the additional analyses for soluble Fe deposition flux focusing on springtime?
- Line 289-292: I do not follow where the targeted seas to this estimation. Please specify.
- Line 293: What is the meaning of “final”, and how to evaluate again the solubility?
- Line 323: It might be better to reconsider this subsection title.
- Line 332-343: This kind of analysis is interesting, but it is still hard to understand the result. I am a little bit confused because the deposition over land should be considered in Figure 6. So, how about to show the concentration over land and ocean, and the deposition over land and ocean separately (not as “All”)?
- Line 425: “emissions“ of what?
- Line 432-434: The final remark was ambiguous. How to enhance the accuracy of soluble metal deposition flux? What is the contribution of this study to the future study?
Citation: https://doi.org/10.5194/egusphere-2024-155-RC1 - AC2: 'Reply on RC1', Yan Zhang, 09 May 2024
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RC2: 'Comment on egusphere-2024-155', Anonymous Referee #2, 17 Mar 2024
This study provides gridded data on sea-wide concentrations, deposition fluxes, and soluble deposition fluxes with detailed source categories of metals by the modified Community Multiscale Air Quality (CMAQ) model. In general, this paper is well-written and organized, and I only have minor comments.
First, the validation of the modeling results should be further discussed, which I think is very important for modeling work. Tables S9-10 were not discussed sufficiently. If there are measurements on surface concentrations of metals over lands and oceans, some detailed comparisons are needed (site/region/total average). You can refer to some similar works on N emissions, in which the validation works were made between modeling and measurements on land and oceans (see the supporting materials of papers: https://doi.org/10.1073/pnas.2121998119; https://doi.org/10.1073/pnas.2221459120).
Second, are there any social-economic drivers for seasonal changes in metal emissions? For instance, when we talked about NH3, it’s usually controlled by increasing population and food production (N fertilizer, livestock). NH3 seasonal changes are mainly affected by temperature and fertilizer applications. I hope to see some additional discussions on metal seasonal changes. How the urbanization affect metal emissions and pollution? (see refs on social-economic drivers on agricultural N emissions: L. Liu. 2023 Nature, https://doi.org/10.1038/d41586-023-02753-9; Deng et al. 2024 Nature communications, https://doi.org/10.1038/s41467-023-44685-y).
Citation: https://doi.org/10.5194/egusphere-2024-155-RC2 - AC1: 'Reply on RC2', Yan Zhang, 09 May 2024
Interactive discussion
Status: closed
-
RC1: 'Comment on egusphere-2024-155', Anonymous Referee #1, 23 Feb 2024
General comments:
The manuscript of egusphere-2024-155 entitled “Source-resolved atmospheric metal emissions, concentrations, and their deposition fluxes into the East Asian Seas” presented the development of source-specific emission inventory for metals (Fe, Al, Cu, V, Ni, and Zn) and further conducted the model simulations to estimate ambient concentrations and depositions over East Asia. The importance of this kind of study is understandable, and I generally agree with the possible publication. However, I have one major concern as follows, and relevant discussions are required to be fully amended.
Major concern:
- Development of emission inventory (Sections 2.2 and 3.1): I can follow the methodology itself; however, we should recognize that dust emission can largely varied year-to-year. From the simulation, only four months (January, April, July, and October) were conducted, but annual emissions were presented in Fig. 1. How did the authors estimate annual total emissions? Or, the covering spring time is enough to calculate the annual total emissions as stated? Moreover, this study targeted the year of 2017, but why? The estimated dust emissions were possible maxima/minima or average situation for Asia dust? These details explanations are required to follow this study.
Specific comments:
- Line 30: The component of trace metals should be first defined in the first appearance (not in the second sentence).
- Line 49: A high temperature of aerosol itself? Please clarify.
- Line 58-63: But this study was conducted over East Asia. This paragraph seems to be mainly focused on the Southern Ocean. The motivation for East Asia is also required to understand the introduction of this study.
- Line 78 or Line 84: The relevant information (e.g., doi of zenodo) for the original CMAQ modeling system itself is needed here.
- Line 84-90: Because this study analyzed deposition, a description of the deposition scheme in the CMAQ should be presented.
- Line 121: I guess the inline dust module in the CMAQ for Foroutan et al. (2017) (doi:10.1002/2016MS000823) is required, or did the authors develop their models?
- Line 131-133: I do not fully understand this sentence.
- Line 185: Before starting this section 3.1.2, it would be better to mention Fig. 2 at first (not in Line 201).
- Line 215-218: In addition to the targeted seas such as ECS explained here, further discussion focusing on the springtime would clarify the importance of dust emissions.
- Line 228-230 (the caption of Figure 3) and the relevant discussion: I do not follow why this estimation is expressed as the total annual mean concentration. Because this study was only conducted for four months, even though these are representative months of each season, the wording “annual mean” will be overstated. In addition to this question, what is the meaning of “total”? If this is the total concentration, the concentration for the “ALL” region should be the sum of all ocean areas. Please clarify these expressions and the actual analyzed contents.
- Line 257-260 (the caption of Figure 4) and the relevant discussion: Same comment to the above comment on Line 228-230.
- Line 288-313: Again, why these estimations can be explained as annual amounts? Taking into consideration the important role of Asian dust in spring, how about the additional analyses for soluble Fe deposition flux focusing on springtime?
- Line 289-292: I do not follow where the targeted seas to this estimation. Please specify.
- Line 293: What is the meaning of “final”, and how to evaluate again the solubility?
- Line 323: It might be better to reconsider this subsection title.
- Line 332-343: This kind of analysis is interesting, but it is still hard to understand the result. I am a little bit confused because the deposition over land should be considered in Figure 6. So, how about to show the concentration over land and ocean, and the deposition over land and ocean separately (not as “All”)?
- Line 425: “emissions“ of what?
- Line 432-434: The final remark was ambiguous. How to enhance the accuracy of soluble metal deposition flux? What is the contribution of this study to the future study?
Citation: https://doi.org/10.5194/egusphere-2024-155-RC1 - AC2: 'Reply on RC1', Yan Zhang, 09 May 2024
-
RC2: 'Comment on egusphere-2024-155', Anonymous Referee #2, 17 Mar 2024
This study provides gridded data on sea-wide concentrations, deposition fluxes, and soluble deposition fluxes with detailed source categories of metals by the modified Community Multiscale Air Quality (CMAQ) model. In general, this paper is well-written and organized, and I only have minor comments.
First, the validation of the modeling results should be further discussed, which I think is very important for modeling work. Tables S9-10 were not discussed sufficiently. If there are measurements on surface concentrations of metals over lands and oceans, some detailed comparisons are needed (site/region/total average). You can refer to some similar works on N emissions, in which the validation works were made between modeling and measurements on land and oceans (see the supporting materials of papers: https://doi.org/10.1073/pnas.2121998119; https://doi.org/10.1073/pnas.2221459120).
Second, are there any social-economic drivers for seasonal changes in metal emissions? For instance, when we talked about NH3, it’s usually controlled by increasing population and food production (N fertilizer, livestock). NH3 seasonal changes are mainly affected by temperature and fertilizer applications. I hope to see some additional discussions on metal seasonal changes. How the urbanization affect metal emissions and pollution? (see refs on social-economic drivers on agricultural N emissions: L. Liu. 2023 Nature, https://doi.org/10.1038/d41586-023-02753-9; Deng et al. 2024 Nature communications, https://doi.org/10.1038/s41467-023-44685-y).
Citation: https://doi.org/10.5194/egusphere-2024-155-RC2 - AC1: 'Reply on RC2', Yan Zhang, 09 May 2024
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Shenglan Jiang
Yan Zhang
Guangyuan Yu
Zimin Han
Junri Zhao
Tianle Zhang
Mei Zheng
The requested preprint has a corresponding peer-reviewed final revised paper. You are encouraged to refer to the final revised version.
- Preprint
(3002 KB) - Metadata XML
-
Supplement
(944 KB) - BibTeX
- EndNote
- Final revised paper