the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Residential burning is a significant source of soluble iron to the ocean
Abstract. Understanding the physicochemical processes that supply atmospheric aerosol iron (Fe) to the ocean is crucial in our understanding of global biogeochemical cycles. Anthropogenic emissions contribute significant fluxes of aerosol Fe to the atmosphere, the soluble fraction of which can modulate marine primary productivity upon its deposition to the ocean surface. However, aerosol Fe solubility remains poorly constrained, due in part to a lack of direct measurements spanning a multitude of anthropogenic sources. We measured solubility of aerosol Fe from several distinct anthropogenic combustion processes and fuel types. The median Fe solubility varied widely by source, ranging from 0.03 % for power plant coal fly ash to 55.87 % for biofuel burning; furthermore, residential coal burning aerosol possessed much higher Fe solubility than industrial coal fly ash. Using new Fe solubilities reported herein, we updated parameters for anthropogenic aerosol Fe within the Mechanism of Intermediate complexity for Modeling Iron, an aerosol Fe module of the Community Earth System Model v2. Such updates led to significant improvement in model performance over ocean regions heavily influenced by anthropogenic emissions, and we identified residential burning as a significant source of soluble aerosol Fe to the ocean. Our work underscores the need to further refine understanding of physicochemical properties of aerosol Fe from a wide variety of anthropogenic sources. In turn, this understanding will aid in characterizing the influences of anthropogenic activities on past, present, and future atmospheric nutrient inputs to marine ecosystems.
Competing interests: At least one of the (co-)authors is a member of the editorial board of Atmospheric Chemistry and Physics.
Publisher's note: Copernicus Publications remains neutral with regard to jurisdictional claims made in the text, published maps, institutional affiliations, or any other geographical representation in this paper. While Copernicus Publications makes every effort to include appropriate place names, the final responsibility lies with the authors. Views expressed in the text are those of the authors and do not necessarily reflect the views of the publisher.- Preprint
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Status: open (until 20 Nov 2025)
- RC1: 'Comment on egusphere-2025-4058', Akinori Ito, 16 Oct 2025 reply
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General comments
There are still large uncertainties in source attribution of soluble iron (Fe) in atmospheric aerosols from different anthropogenic sources, despite substantial advancement in the source attribution between natural and anthropogenic sources. Due to low iron content in residential burning aerosols, residential burning is expected to be negligible source of Fe to the ocean. This study argues that residential burning is a significant source of soluble Fe to the ocean based on the measurements of high Fe solubility at emission for residential coal burning aerosol and residential biofuel burning than industrial coal fly ash. This hypothesis is based on the assumption on a representation of iron mineralogy for anthropogenic combustion sources, which suggests that the emissions of soluble iron from residential coal and wood combustion could be an important contributor to soluble iron production (Rathod et al. 2020). The comprehensive measurements and their application to the model simulations may help us to advance modeling anthropogenic soluble iron. However, my major concern is the inconsistency between Fe content used in the model and Fe content measured from this work with the high Fe solubility at emission measured in this work. I have some comments and questions to improve this paper.
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Major comments
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Specific comments
l.116: Please describe the information about the size of ash samples.
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l.121 and Table S5: Please specify the sources of oil fly ashes, because Fe content is substantially different between the two samples. Why is this?
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l.129: You described that the acetate buffer was used to simulate cloud water (Li et al., 2022b). Here, you applied Fe solubility from the acetate buffer to that at emission before the cloud processing. Why did you choose the sodium acetate buffer over the deionized water? Please show the comparison of Fe solubility near the source regions, for example, at Guangzhou.
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l.198: You updated Fe solubility at emission but did not Fe content. I suggest additional simulations with both updated Fe content and solubility at emission (see below more details).
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l.214: The anthropogenic coal Fe sources from residential sector can be separately estimated from industrial sector, as is described on l.383. Do you mean that you segregated 1) industrial fossil fuel (coal) in the dataset provided by Rathod et al. (2020) into industrial and residential coal burning sources? Please rephrase the sentence.
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l.216: How did you assume that the Fe-to-BC ratios were matched between sources? Iron emissions from residential wood and coal combustion is only about 2% (Table S6 in Rathod et al. 2020) of the global fine Fe emissions due to their low-Fe emission factors. Thus, the industrial-to-residential BC is higher than industrial-to-residential Fe (see Table 3 in Ito et al. 2021), as you described for carbon content on l.386 and iron content in Figure 2. If you used the same Fe-to-BC ratios between the two sources, you assigned larger Fe emissions (in other words, higher Fe content than Rathod et al., 2020) into residential sector than industrial sector by more than a factor of 10. It is straightforward to calculate the Fe-to-BC ratios for residential sector and industrial sector because the anthropogenic coal Fe sources from residential sector is separately estimated from industrial sector (Rathod et al., 2020). Please show the global emissions for Fe and BC from coal combustion for each sector and final Fe content at emission.
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l.320: Please indicate the references for the additional measurements.
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l.383: Table S2 shows negative relationship between Fe content and Fe solubility, possibly because Fe species inside the particles might not be transformed to labile form in combustion process. If you used higher Fe content (> 0.5 mg/g) for aerosols, you would apply larger Fe emissions (> 13 times) to residential coal combustion aerosols which consist of the median Fe content (0.038 mg/g) measured at higher Fe solubility. Why donât you update Fe content, too?
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l.347, Table 2: Please indicate the size information and elucidate the differences between ash and aerosol.
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l.430: If you used higher Fe content (0.58 mg/g) for aerosols, you would apply larger Fe emissions (45 times) to residential biofuel combustion aerosols which consist of the median Fe content (0.013 mg/g) measured at higher Fe solubility. Why donât you update Fe content, too?
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l.568 and Table 3: Why did you use higher Fe solubility of oil bottom ash (25%) than the measurements of Fe solubility in Table 2 for oil fly ash (12.56%)?
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l.658: Please report the statistics for soluble Fe over Southeastern Asia, the Bay of Bengal, the North Pacific, and the North Atlantic to support the improvement.
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l.678: Please report the statistics for Fe to support the improvement of dust Fe.
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l.685: Please report the statistics for Fe solubility.
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l.768: Since you increased soluble Fe from anthropogenic sources, you would estimate lighter Fe isotopes than your previous estimates. How can this be reconciled with the aerosol Fe isotope measurements? If higher Fe solubility is compensated by lower Fe content in the additional simulations, your Fe isotope might be consistent. Please show the comparison of Fe isotopes.
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Technical comments
l.57: What is Fe availability? Do you mean bioavailability?
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Fig. 5: Please rename PD-OIL.