Iron (Fe) speciation in size-fractionated aerosol particles in the Pacific Ocean: The role of organic complexation of Fe with humic-like substances in controlling Fe solubility
<p<Atmospheric deposition is one of the main sources of dissolved iron (Fe) in the ocean surfaces. Atmospheric processes are recognized as controlling fractional Fe solubility (Fe<span class="inline-formula"<<sub<sol</sub<</span<%) in marine aerosol particles....
Ausführliche Beschreibung
Gespeichert in:
| Autor*in: |
K. Sakata [verfasserIn] M. Kurisu [verfasserIn] Y. Takeichi [verfasserIn] A. Sakaguchi [verfasserIn] H. Tanimoto [verfasserIn] Y. Tamenori [verfasserIn] A. Matsuki [verfasserIn] Y. Takahashi [verfasserIn] |
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| Format: |
E-Artikel |
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| Sprache: |
Englisch |
| Erschienen: |
2022 |
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| Übergeordnetes Werk: |
In: Atmospheric Chemistry and Physics - Copernicus Publications, 2003, 22(2022), Seite 9461-9482 |
|---|---|
| Übergeordnetes Werk: |
volume:22 ; year:2022 ; pages:9461-9482 |
| Links: |
Link aufrufen |
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| DOI / URN: |
10.5194/acp-22-9461-2022 |
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| Katalog-ID: |
DOAJ024616931 |
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| 245 | 1 | 0 | |a Iron (Fe) speciation in size-fractionated aerosol particles in the Pacific Ocean: The role of organic complexation of Fe with humic-like substances in controlling Fe solubility |
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| 520 | |a <p<Atmospheric deposition is one of the main sources of dissolved iron (Fe) in the ocean surfaces. Atmospheric processes are recognized as controlling fractional Fe solubility (Fe<span class="inline-formula"<<sub<sol</sub<</span<%) in marine aerosol particles. However, the impact of these processes on Fe<span class="inline-formula"<<sub<sol</sub<</span<% remains unclear. One of the reasons for this is the lack of field observations focusing on the relationship between Fe<span class="inline-formula"<<sub<sol</sub<</span<% and Fe species in marine aerosol particles. In particular, the effects of organic ligands on Fe<span class="inline-formula"<<sub<sol</sub<</span<% have not been thoroughly investigated in observational studies. In this study, Fe species in size-fractionated aerosol particles in the Pacific Ocean were determined using X-ray absorption fine structure (XAFS) spectroscopy. The internal mixing states of Fe and organic carbon were investigated using scanning transmission X-ray microscopy (STXM). The effects of atmospheric processes on Fe<span class="inline-formula"<<sub<sol</sub<</span<% in marine aerosol particles were investigated based on the speciation results. Iron in size-fractionated aerosol particles was mainly derived from mineral dust, regardless of aerosol diameter, because the enrichment factor of Fe was almost 1 in both coarse (PM<span class="inline-formula"<<sub<>1.3</sub<</span<) and fine aerosol particles (PM<span class="inline-formula"<<sub<1.3</sub<</span<). Approximately 80 % of the total Fe (insoluble <span class="inline-formula"<+</span< labile Fe) was present in PM<span class="inline-formula"<<sub<>1.3</sub<</span<, whereas labile Fe was mainly present in PM<span class="inline-formula"<<sub<1.3</sub<</span<. The Fe<span class="inline-formula"<<sub<sol</sub<</span<% in PM<span class="inline-formula"<<sub<>1.3</sub<</span< was not significantly increased (<span class="inline-formula"<2.56±2.53</span< %, 0.00 %–8.50 %, <span class="inline-formula"<<i<n</i<=20</span<) by the atmospheric processes because mineral dust was not acidified beyond the buffer capacity of calcite. In contrast, mineral dust in PM<span class="inline-formula"<<sub<1.3</sub<</span< was acidified beyond the buffer capacity of calcite. As a result, Fe<span class="inline-formula"<<sub<sol</sub<</span<% in PM<span class="inline-formula"<<sub<1.3</sub<</span< (0.202 %–64.7 %, <span class="inline-formula"<<i<n</i<=10</span<) was an order of magnitude higher than that in PM<span class="inline-formula"<<sub<>1.3</sub<</span<. The PM<span class="inline-formula"<<sub<1.3</sub<</span< contained ferric organic complexes with humic-like substances (Fe(III)-HULIS, but not Fe-oxalate complexes), and the abundance correlated with Fe<span class="inline-formula"<<sub<sol</sub<</span<%. Iron(III)-HULIS was formed during transport in the Pacific Ocean because Fe(III)-HULIS was not found in aerosol particles in Beijing and Japan. The pH estimations of mineral dust in PM<span class="inline-formula"<<sub<1.3</sub<</span< established that Fe was solubilized by proton-promoted dissolution under highly acidic conditions (pH <span class="inline-formula"<<</span< 3.0), whereas Fe(III)-HULIS was stabilized under moderately acidic conditions (pH 3.0–6.0). Since the observed labile Fe concentration could not be reproduced by proton-promoted dissolution under moderately acidic conditions, the pH of mineral dust increased after proton-promoted dissolution. The cloud process in the marine atmosphere increases the mineral dust pH because the dust particles are covered with organic carbon and Na. The precipitation of ferrihydrite was suppressed by Fe(III)-HULIS owing to its high water solubility. Thus, the organic complexation of Fe with HULIS plays a significant role in the stabilization of Fe that was initially solubilized by proton-promoted dissolution.</p< | ||
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| 700 | 0 | |a A. Matsuki |e verfasserin |4 aut | |
| 700 | 0 | |a Y. Takahashi |e verfasserin |4 aut | |
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10.5194/acp-22-9461-2022 doi (DE-627)DOAJ024616931 (DE-599)DOAJ60c21047b1d346f197d745a315a34076 DE-627 ger DE-627 rakwb eng QC1-999 QD1-999 K. Sakata verfasserin aut Iron (Fe) speciation in size-fractionated aerosol particles in the Pacific Ocean: The role of organic complexation of Fe with humic-like substances in controlling Fe solubility 2022 Text txt rdacontent Computermedien c rdamedia Online-Ressource cr rdacarrier <p<Atmospheric deposition is one of the main sources of dissolved iron (Fe) in the ocean surfaces. Atmospheric processes are recognized as controlling fractional Fe solubility (Fe<span class="inline-formula"<<sub<sol</sub<</span<%) in marine aerosol particles. However, the impact of these processes on Fe<span class="inline-formula"<<sub<sol</sub<</span<% remains unclear. One of the reasons for this is the lack of field observations focusing on the relationship between Fe<span class="inline-formula"<<sub<sol</sub<</span<% and Fe species in marine aerosol particles. In particular, the effects of organic ligands on Fe<span class="inline-formula"<<sub<sol</sub<</span<% have not been thoroughly investigated in observational studies. In this study, Fe species in size-fractionated aerosol particles in the Pacific Ocean were determined using X-ray absorption fine structure (XAFS) spectroscopy. The internal mixing states of Fe and organic carbon were investigated using scanning transmission X-ray microscopy (STXM). The effects of atmospheric processes on Fe<span class="inline-formula"<<sub<sol</sub<</span<% in marine aerosol particles were investigated based on the speciation results. Iron in size-fractionated aerosol particles was mainly derived from mineral dust, regardless of aerosol diameter, because the enrichment factor of Fe was almost 1 in both coarse (PM<span class="inline-formula"<<sub<>1.3</sub<</span<) and fine aerosol particles (PM<span class="inline-formula"<<sub<1.3</sub<</span<). Approximately 80 % of the total Fe (insoluble <span class="inline-formula"<+</span< labile Fe) was present in PM<span class="inline-formula"<<sub<>1.3</sub<</span<, whereas labile Fe was mainly present in PM<span class="inline-formula"<<sub<1.3</sub<</span<. The Fe<span class="inline-formula"<<sub<sol</sub<</span<% in PM<span class="inline-formula"<<sub<>1.3</sub<</span< was not significantly increased (<span class="inline-formula"<2.56±2.53</span< %, 0.00 %–8.50 %, <span class="inline-formula"<<i<n</i<=20</span<) by the atmospheric processes because mineral dust was not acidified beyond the buffer capacity of calcite. In contrast, mineral dust in PM<span class="inline-formula"<<sub<1.3</sub<</span< was acidified beyond the buffer capacity of calcite. As a result, Fe<span class="inline-formula"<<sub<sol</sub<</span<% in PM<span class="inline-formula"<<sub<1.3</sub<</span< (0.202 %–64.7 %, <span class="inline-formula"<<i<n</i<=10</span<) was an order of magnitude higher than that in PM<span class="inline-formula"<<sub<>1.3</sub<</span<. The PM<span class="inline-formula"<<sub<1.3</sub<</span< contained ferric organic complexes with humic-like substances (Fe(III)-HULIS, but not Fe-oxalate complexes), and the abundance correlated with Fe<span class="inline-formula"<<sub<sol</sub<</span<%. Iron(III)-HULIS was formed during transport in the Pacific Ocean because Fe(III)-HULIS was not found in aerosol particles in Beijing and Japan. The pH estimations of mineral dust in PM<span class="inline-formula"<<sub<1.3</sub<</span< established that Fe was solubilized by proton-promoted dissolution under highly acidic conditions (pH <span class="inline-formula"<<</span< 3.0), whereas Fe(III)-HULIS was stabilized under moderately acidic conditions (pH 3.0–6.0). Since the observed labile Fe concentration could not be reproduced by proton-promoted dissolution under moderately acidic conditions, the pH of mineral dust increased after proton-promoted dissolution. The cloud process in the marine atmosphere increases the mineral dust pH because the dust particles are covered with organic carbon and Na. The precipitation of ferrihydrite was suppressed by Fe(III)-HULIS owing to its high water solubility. Thus, the organic complexation of Fe with HULIS plays a significant role in the stabilization of Fe that was initially solubilized by proton-promoted dissolution.</p< Physics Chemistry M. Kurisu verfasserin aut M. Kurisu verfasserin aut Y. Takeichi verfasserin aut A. Sakaguchi verfasserin aut H. Tanimoto verfasserin aut H. Tanimoto verfasserin aut Y. Tamenori verfasserin aut A. Matsuki verfasserin aut Y. Takahashi verfasserin aut Y. Takahashi verfasserin aut In Atmospheric Chemistry and Physics Copernicus Publications, 2003 22(2022), Seite 9461-9482 (DE-627)092499996 16807324 nnns volume:22 year:2022 pages:9461-9482 https://doi.org/10.5194/acp-22-9461-2022 kostenfrei https://doaj.org/article/60c21047b1d346f197d745a315a34076 kostenfrei https://acp.copernicus.org/articles/22/9461/2022/acp-22-9461-2022.pdf kostenfrei https://doaj.org/toc/1680-7316 Journal toc kostenfrei https://doaj.org/toc/1680-7324 Journal toc kostenfrei GBV_USEFLAG_A SYSFLAG_A GBV_DOAJ SSG-OLC-PHA GBV_ILN_381 AR 22 2022 9461-9482 |
| spelling |
10.5194/acp-22-9461-2022 doi (DE-627)DOAJ024616931 (DE-599)DOAJ60c21047b1d346f197d745a315a34076 DE-627 ger DE-627 rakwb eng QC1-999 QD1-999 K. Sakata verfasserin aut Iron (Fe) speciation in size-fractionated aerosol particles in the Pacific Ocean: The role of organic complexation of Fe with humic-like substances in controlling Fe solubility 2022 Text txt rdacontent Computermedien c rdamedia Online-Ressource cr rdacarrier <p<Atmospheric deposition is one of the main sources of dissolved iron (Fe) in the ocean surfaces. Atmospheric processes are recognized as controlling fractional Fe solubility (Fe<span class="inline-formula"<<sub<sol</sub<</span<%) in marine aerosol particles. However, the impact of these processes on Fe<span class="inline-formula"<<sub<sol</sub<</span<% remains unclear. One of the reasons for this is the lack of field observations focusing on the relationship between Fe<span class="inline-formula"<<sub<sol</sub<</span<% and Fe species in marine aerosol particles. In particular, the effects of organic ligands on Fe<span class="inline-formula"<<sub<sol</sub<</span<% have not been thoroughly investigated in observational studies. In this study, Fe species in size-fractionated aerosol particles in the Pacific Ocean were determined using X-ray absorption fine structure (XAFS) spectroscopy. The internal mixing states of Fe and organic carbon were investigated using scanning transmission X-ray microscopy (STXM). The effects of atmospheric processes on Fe<span class="inline-formula"<<sub<sol</sub<</span<% in marine aerosol particles were investigated based on the speciation results. Iron in size-fractionated aerosol particles was mainly derived from mineral dust, regardless of aerosol diameter, because the enrichment factor of Fe was almost 1 in both coarse (PM<span class="inline-formula"<<sub<>1.3</sub<</span<) and fine aerosol particles (PM<span class="inline-formula"<<sub<1.3</sub<</span<). Approximately 80 % of the total Fe (insoluble <span class="inline-formula"<+</span< labile Fe) was present in PM<span class="inline-formula"<<sub<>1.3</sub<</span<, whereas labile Fe was mainly present in PM<span class="inline-formula"<<sub<1.3</sub<</span<. The Fe<span class="inline-formula"<<sub<sol</sub<</span<% in PM<span class="inline-formula"<<sub<>1.3</sub<</span< was not significantly increased (<span class="inline-formula"<2.56±2.53</span< %, 0.00 %–8.50 %, <span class="inline-formula"<<i<n</i<=20</span<) by the atmospheric processes because mineral dust was not acidified beyond the buffer capacity of calcite. In contrast, mineral dust in PM<span class="inline-formula"<<sub<1.3</sub<</span< was acidified beyond the buffer capacity of calcite. As a result, Fe<span class="inline-formula"<<sub<sol</sub<</span<% in PM<span class="inline-formula"<<sub<1.3</sub<</span< (0.202 %–64.7 %, <span class="inline-formula"<<i<n</i<=10</span<) was an order of magnitude higher than that in PM<span class="inline-formula"<<sub<>1.3</sub<</span<. The PM<span class="inline-formula"<<sub<1.3</sub<</span< contained ferric organic complexes with humic-like substances (Fe(III)-HULIS, but not Fe-oxalate complexes), and the abundance correlated with Fe<span class="inline-formula"<<sub<sol</sub<</span<%. Iron(III)-HULIS was formed during transport in the Pacific Ocean because Fe(III)-HULIS was not found in aerosol particles in Beijing and Japan. The pH estimations of mineral dust in PM<span class="inline-formula"<<sub<1.3</sub<</span< established that Fe was solubilized by proton-promoted dissolution under highly acidic conditions (pH <span class="inline-formula"<<</span< 3.0), whereas Fe(III)-HULIS was stabilized under moderately acidic conditions (pH 3.0–6.0). Since the observed labile Fe concentration could not be reproduced by proton-promoted dissolution under moderately acidic conditions, the pH of mineral dust increased after proton-promoted dissolution. The cloud process in the marine atmosphere increases the mineral dust pH because the dust particles are covered with organic carbon and Na. The precipitation of ferrihydrite was suppressed by Fe(III)-HULIS owing to its high water solubility. Thus, the organic complexation of Fe with HULIS plays a significant role in the stabilization of Fe that was initially solubilized by proton-promoted dissolution.</p< Physics Chemistry M. Kurisu verfasserin aut M. Kurisu verfasserin aut Y. Takeichi verfasserin aut A. Sakaguchi verfasserin aut H. Tanimoto verfasserin aut H. Tanimoto verfasserin aut Y. Tamenori verfasserin aut A. Matsuki verfasserin aut Y. Takahashi verfasserin aut Y. Takahashi verfasserin aut In Atmospheric Chemistry and Physics Copernicus Publications, 2003 22(2022), Seite 9461-9482 (DE-627)092499996 16807324 nnns volume:22 year:2022 pages:9461-9482 https://doi.org/10.5194/acp-22-9461-2022 kostenfrei https://doaj.org/article/60c21047b1d346f197d745a315a34076 kostenfrei https://acp.copernicus.org/articles/22/9461/2022/acp-22-9461-2022.pdf kostenfrei https://doaj.org/toc/1680-7316 Journal toc kostenfrei https://doaj.org/toc/1680-7324 Journal toc kostenfrei GBV_USEFLAG_A SYSFLAG_A GBV_DOAJ SSG-OLC-PHA GBV_ILN_381 AR 22 2022 9461-9482 |
| allfields_unstemmed |
10.5194/acp-22-9461-2022 doi (DE-627)DOAJ024616931 (DE-599)DOAJ60c21047b1d346f197d745a315a34076 DE-627 ger DE-627 rakwb eng QC1-999 QD1-999 K. Sakata verfasserin aut Iron (Fe) speciation in size-fractionated aerosol particles in the Pacific Ocean: The role of organic complexation of Fe with humic-like substances in controlling Fe solubility 2022 Text txt rdacontent Computermedien c rdamedia Online-Ressource cr rdacarrier <p<Atmospheric deposition is one of the main sources of dissolved iron (Fe) in the ocean surfaces. Atmospheric processes are recognized as controlling fractional Fe solubility (Fe<span class="inline-formula"<<sub<sol</sub<</span<%) in marine aerosol particles. However, the impact of these processes on Fe<span class="inline-formula"<<sub<sol</sub<</span<% remains unclear. One of the reasons for this is the lack of field observations focusing on the relationship between Fe<span class="inline-formula"<<sub<sol</sub<</span<% and Fe species in marine aerosol particles. In particular, the effects of organic ligands on Fe<span class="inline-formula"<<sub<sol</sub<</span<% have not been thoroughly investigated in observational studies. In this study, Fe species in size-fractionated aerosol particles in the Pacific Ocean were determined using X-ray absorption fine structure (XAFS) spectroscopy. The internal mixing states of Fe and organic carbon were investigated using scanning transmission X-ray microscopy (STXM). The effects of atmospheric processes on Fe<span class="inline-formula"<<sub<sol</sub<</span<% in marine aerosol particles were investigated based on the speciation results. Iron in size-fractionated aerosol particles was mainly derived from mineral dust, regardless of aerosol diameter, because the enrichment factor of Fe was almost 1 in both coarse (PM<span class="inline-formula"<<sub<>1.3</sub<</span<) and fine aerosol particles (PM<span class="inline-formula"<<sub<1.3</sub<</span<). Approximately 80 % of the total Fe (insoluble <span class="inline-formula"<+</span< labile Fe) was present in PM<span class="inline-formula"<<sub<>1.3</sub<</span<, whereas labile Fe was mainly present in PM<span class="inline-formula"<<sub<1.3</sub<</span<. The Fe<span class="inline-formula"<<sub<sol</sub<</span<% in PM<span class="inline-formula"<<sub<>1.3</sub<</span< was not significantly increased (<span class="inline-formula"<2.56±2.53</span< %, 0.00 %–8.50 %, <span class="inline-formula"<<i<n</i<=20</span<) by the atmospheric processes because mineral dust was not acidified beyond the buffer capacity of calcite. In contrast, mineral dust in PM<span class="inline-formula"<<sub<1.3</sub<</span< was acidified beyond the buffer capacity of calcite. As a result, Fe<span class="inline-formula"<<sub<sol</sub<</span<% in PM<span class="inline-formula"<<sub<1.3</sub<</span< (0.202 %–64.7 %, <span class="inline-formula"<<i<n</i<=10</span<) was an order of magnitude higher than that in PM<span class="inline-formula"<<sub<>1.3</sub<</span<. The PM<span class="inline-formula"<<sub<1.3</sub<</span< contained ferric organic complexes with humic-like substances (Fe(III)-HULIS, but not Fe-oxalate complexes), and the abundance correlated with Fe<span class="inline-formula"<<sub<sol</sub<</span<%. Iron(III)-HULIS was formed during transport in the Pacific Ocean because Fe(III)-HULIS was not found in aerosol particles in Beijing and Japan. The pH estimations of mineral dust in PM<span class="inline-formula"<<sub<1.3</sub<</span< established that Fe was solubilized by proton-promoted dissolution under highly acidic conditions (pH <span class="inline-formula"<<</span< 3.0), whereas Fe(III)-HULIS was stabilized under moderately acidic conditions (pH 3.0–6.0). Since the observed labile Fe concentration could not be reproduced by proton-promoted dissolution under moderately acidic conditions, the pH of mineral dust increased after proton-promoted dissolution. The cloud process in the marine atmosphere increases the mineral dust pH because the dust particles are covered with organic carbon and Na. The precipitation of ferrihydrite was suppressed by Fe(III)-HULIS owing to its high water solubility. Thus, the organic complexation of Fe with HULIS plays a significant role in the stabilization of Fe that was initially solubilized by proton-promoted dissolution.</p< Physics Chemistry M. Kurisu verfasserin aut M. Kurisu verfasserin aut Y. Takeichi verfasserin aut A. Sakaguchi verfasserin aut H. Tanimoto verfasserin aut H. Tanimoto verfasserin aut Y. Tamenori verfasserin aut A. Matsuki verfasserin aut Y. Takahashi verfasserin aut Y. Takahashi verfasserin aut In Atmospheric Chemistry and Physics Copernicus Publications, 2003 22(2022), Seite 9461-9482 (DE-627)092499996 16807324 nnns volume:22 year:2022 pages:9461-9482 https://doi.org/10.5194/acp-22-9461-2022 kostenfrei https://doaj.org/article/60c21047b1d346f197d745a315a34076 kostenfrei https://acp.copernicus.org/articles/22/9461/2022/acp-22-9461-2022.pdf kostenfrei https://doaj.org/toc/1680-7316 Journal toc kostenfrei https://doaj.org/toc/1680-7324 Journal toc kostenfrei GBV_USEFLAG_A SYSFLAG_A GBV_DOAJ SSG-OLC-PHA GBV_ILN_381 AR 22 2022 9461-9482 |
| allfieldsGer |
10.5194/acp-22-9461-2022 doi (DE-627)DOAJ024616931 (DE-599)DOAJ60c21047b1d346f197d745a315a34076 DE-627 ger DE-627 rakwb eng QC1-999 QD1-999 K. Sakata verfasserin aut Iron (Fe) speciation in size-fractionated aerosol particles in the Pacific Ocean: The role of organic complexation of Fe with humic-like substances in controlling Fe solubility 2022 Text txt rdacontent Computermedien c rdamedia Online-Ressource cr rdacarrier <p<Atmospheric deposition is one of the main sources of dissolved iron (Fe) in the ocean surfaces. Atmospheric processes are recognized as controlling fractional Fe solubility (Fe<span class="inline-formula"<<sub<sol</sub<</span<%) in marine aerosol particles. However, the impact of these processes on Fe<span class="inline-formula"<<sub<sol</sub<</span<% remains unclear. One of the reasons for this is the lack of field observations focusing on the relationship between Fe<span class="inline-formula"<<sub<sol</sub<</span<% and Fe species in marine aerosol particles. In particular, the effects of organic ligands on Fe<span class="inline-formula"<<sub<sol</sub<</span<% have not been thoroughly investigated in observational studies. In this study, Fe species in size-fractionated aerosol particles in the Pacific Ocean were determined using X-ray absorption fine structure (XAFS) spectroscopy. The internal mixing states of Fe and organic carbon were investigated using scanning transmission X-ray microscopy (STXM). The effects of atmospheric processes on Fe<span class="inline-formula"<<sub<sol</sub<</span<% in marine aerosol particles were investigated based on the speciation results. Iron in size-fractionated aerosol particles was mainly derived from mineral dust, regardless of aerosol diameter, because the enrichment factor of Fe was almost 1 in both coarse (PM<span class="inline-formula"<<sub<>1.3</sub<</span<) and fine aerosol particles (PM<span class="inline-formula"<<sub<1.3</sub<</span<). Approximately 80 % of the total Fe (insoluble <span class="inline-formula"<+</span< labile Fe) was present in PM<span class="inline-formula"<<sub<>1.3</sub<</span<, whereas labile Fe was mainly present in PM<span class="inline-formula"<<sub<1.3</sub<</span<. The Fe<span class="inline-formula"<<sub<sol</sub<</span<% in PM<span class="inline-formula"<<sub<>1.3</sub<</span< was not significantly increased (<span class="inline-formula"<2.56±2.53</span< %, 0.00 %–8.50 %, <span class="inline-formula"<<i<n</i<=20</span<) by the atmospheric processes because mineral dust was not acidified beyond the buffer capacity of calcite. In contrast, mineral dust in PM<span class="inline-formula"<<sub<1.3</sub<</span< was acidified beyond the buffer capacity of calcite. As a result, Fe<span class="inline-formula"<<sub<sol</sub<</span<% in PM<span class="inline-formula"<<sub<1.3</sub<</span< (0.202 %–64.7 %, <span class="inline-formula"<<i<n</i<=10</span<) was an order of magnitude higher than that in PM<span class="inline-formula"<<sub<>1.3</sub<</span<. The PM<span class="inline-formula"<<sub<1.3</sub<</span< contained ferric organic complexes with humic-like substances (Fe(III)-HULIS, but not Fe-oxalate complexes), and the abundance correlated with Fe<span class="inline-formula"<<sub<sol</sub<</span<%. Iron(III)-HULIS was formed during transport in the Pacific Ocean because Fe(III)-HULIS was not found in aerosol particles in Beijing and Japan. The pH estimations of mineral dust in PM<span class="inline-formula"<<sub<1.3</sub<</span< established that Fe was solubilized by proton-promoted dissolution under highly acidic conditions (pH <span class="inline-formula"<<</span< 3.0), whereas Fe(III)-HULIS was stabilized under moderately acidic conditions (pH 3.0–6.0). Since the observed labile Fe concentration could not be reproduced by proton-promoted dissolution under moderately acidic conditions, the pH of mineral dust increased after proton-promoted dissolution. The cloud process in the marine atmosphere increases the mineral dust pH because the dust particles are covered with organic carbon and Na. The precipitation of ferrihydrite was suppressed by Fe(III)-HULIS owing to its high water solubility. Thus, the organic complexation of Fe with HULIS plays a significant role in the stabilization of Fe that was initially solubilized by proton-promoted dissolution.</p< Physics Chemistry M. Kurisu verfasserin aut M. Kurisu verfasserin aut Y. Takeichi verfasserin aut A. Sakaguchi verfasserin aut H. Tanimoto verfasserin aut H. Tanimoto verfasserin aut Y. Tamenori verfasserin aut A. Matsuki verfasserin aut Y. Takahashi verfasserin aut Y. Takahashi verfasserin aut In Atmospheric Chemistry and Physics Copernicus Publications, 2003 22(2022), Seite 9461-9482 (DE-627)092499996 16807324 nnns volume:22 year:2022 pages:9461-9482 https://doi.org/10.5194/acp-22-9461-2022 kostenfrei https://doaj.org/article/60c21047b1d346f197d745a315a34076 kostenfrei https://acp.copernicus.org/articles/22/9461/2022/acp-22-9461-2022.pdf kostenfrei https://doaj.org/toc/1680-7316 Journal toc kostenfrei https://doaj.org/toc/1680-7324 Journal toc kostenfrei GBV_USEFLAG_A SYSFLAG_A GBV_DOAJ SSG-OLC-PHA GBV_ILN_381 AR 22 2022 9461-9482 |
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10.5194/acp-22-9461-2022 doi (DE-627)DOAJ024616931 (DE-599)DOAJ60c21047b1d346f197d745a315a34076 DE-627 ger DE-627 rakwb eng QC1-999 QD1-999 K. Sakata verfasserin aut Iron (Fe) speciation in size-fractionated aerosol particles in the Pacific Ocean: The role of organic complexation of Fe with humic-like substances in controlling Fe solubility 2022 Text txt rdacontent Computermedien c rdamedia Online-Ressource cr rdacarrier <p<Atmospheric deposition is one of the main sources of dissolved iron (Fe) in the ocean surfaces. Atmospheric processes are recognized as controlling fractional Fe solubility (Fe<span class="inline-formula"<<sub<sol</sub<</span<%) in marine aerosol particles. However, the impact of these processes on Fe<span class="inline-formula"<<sub<sol</sub<</span<% remains unclear. One of the reasons for this is the lack of field observations focusing on the relationship between Fe<span class="inline-formula"<<sub<sol</sub<</span<% and Fe species in marine aerosol particles. In particular, the effects of organic ligands on Fe<span class="inline-formula"<<sub<sol</sub<</span<% have not been thoroughly investigated in observational studies. In this study, Fe species in size-fractionated aerosol particles in the Pacific Ocean were determined using X-ray absorption fine structure (XAFS) spectroscopy. The internal mixing states of Fe and organic carbon were investigated using scanning transmission X-ray microscopy (STXM). The effects of atmospheric processes on Fe<span class="inline-formula"<<sub<sol</sub<</span<% in marine aerosol particles were investigated based on the speciation results. Iron in size-fractionated aerosol particles was mainly derived from mineral dust, regardless of aerosol diameter, because the enrichment factor of Fe was almost 1 in both coarse (PM<span class="inline-formula"<<sub<>1.3</sub<</span<) and fine aerosol particles (PM<span class="inline-formula"<<sub<1.3</sub<</span<). Approximately 80 % of the total Fe (insoluble <span class="inline-formula"<+</span< labile Fe) was present in PM<span class="inline-formula"<<sub<>1.3</sub<</span<, whereas labile Fe was mainly present in PM<span class="inline-formula"<<sub<1.3</sub<</span<. The Fe<span class="inline-formula"<<sub<sol</sub<</span<% in PM<span class="inline-formula"<<sub<>1.3</sub<</span< was not significantly increased (<span class="inline-formula"<2.56±2.53</span< %, 0.00 %–8.50 %, <span class="inline-formula"<<i<n</i<=20</span<) by the atmospheric processes because mineral dust was not acidified beyond the buffer capacity of calcite. In contrast, mineral dust in PM<span class="inline-formula"<<sub<1.3</sub<</span< was acidified beyond the buffer capacity of calcite. As a result, Fe<span class="inline-formula"<<sub<sol</sub<</span<% in PM<span class="inline-formula"<<sub<1.3</sub<</span< (0.202 %–64.7 %, <span class="inline-formula"<<i<n</i<=10</span<) was an order of magnitude higher than that in PM<span class="inline-formula"<<sub<>1.3</sub<</span<. The PM<span class="inline-formula"<<sub<1.3</sub<</span< contained ferric organic complexes with humic-like substances (Fe(III)-HULIS, but not Fe-oxalate complexes), and the abundance correlated with Fe<span class="inline-formula"<<sub<sol</sub<</span<%. Iron(III)-HULIS was formed during transport in the Pacific Ocean because Fe(III)-HULIS was not found in aerosol particles in Beijing and Japan. The pH estimations of mineral dust in PM<span class="inline-formula"<<sub<1.3</sub<</span< established that Fe was solubilized by proton-promoted dissolution under highly acidic conditions (pH <span class="inline-formula"<<</span< 3.0), whereas Fe(III)-HULIS was stabilized under moderately acidic conditions (pH 3.0–6.0). Since the observed labile Fe concentration could not be reproduced by proton-promoted dissolution under moderately acidic conditions, the pH of mineral dust increased after proton-promoted dissolution. The cloud process in the marine atmosphere increases the mineral dust pH because the dust particles are covered with organic carbon and Na. The precipitation of ferrihydrite was suppressed by Fe(III)-HULIS owing to its high water solubility. Thus, the organic complexation of Fe with HULIS plays a significant role in the stabilization of Fe that was initially solubilized by proton-promoted dissolution.</p< Physics Chemistry M. Kurisu verfasserin aut M. Kurisu verfasserin aut Y. Takeichi verfasserin aut A. Sakaguchi verfasserin aut H. Tanimoto verfasserin aut H. Tanimoto verfasserin aut Y. Tamenori verfasserin aut A. Matsuki verfasserin aut Y. Takahashi verfasserin aut Y. Takahashi verfasserin aut In Atmospheric Chemistry and Physics Copernicus Publications, 2003 22(2022), Seite 9461-9482 (DE-627)092499996 16807324 nnns volume:22 year:2022 pages:9461-9482 https://doi.org/10.5194/acp-22-9461-2022 kostenfrei https://doaj.org/article/60c21047b1d346f197d745a315a34076 kostenfrei https://acp.copernicus.org/articles/22/9461/2022/acp-22-9461-2022.pdf kostenfrei https://doaj.org/toc/1680-7316 Journal toc kostenfrei https://doaj.org/toc/1680-7324 Journal toc kostenfrei GBV_USEFLAG_A SYSFLAG_A GBV_DOAJ SSG-OLC-PHA GBV_ILN_381 AR 22 2022 9461-9482 |
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Sakata</subfield><subfield code="e">verfasserin</subfield><subfield code="4">aut</subfield></datafield><datafield tag="245" ind1="1" ind2="0"><subfield code="a">Iron (Fe) speciation in size-fractionated aerosol particles in the Pacific Ocean: The role of organic complexation of Fe with humic-like substances in controlling Fe solubility</subfield></datafield><datafield tag="264" ind1=" " ind2="1"><subfield code="c">2022</subfield></datafield><datafield tag="336" ind1=" " ind2=" "><subfield code="a">Text</subfield><subfield code="b">txt</subfield><subfield code="2">rdacontent</subfield></datafield><datafield tag="337" ind1=" " ind2=" "><subfield code="a">Computermedien</subfield><subfield code="b">c</subfield><subfield code="2">rdamedia</subfield></datafield><datafield tag="338" ind1=" " ind2=" "><subfield code="a">Online-Ressource</subfield><subfield code="b">cr</subfield><subfield code="2">rdacarrier</subfield></datafield><datafield tag="520" ind1=" " ind2=" "><subfield code="a"><p<Atmospheric deposition is one of the main sources of dissolved iron (Fe) in the ocean surfaces. 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The effects of atmospheric processes on Fe<span class="inline-formula"<<sub<sol</sub<</span<% in marine aerosol particles were investigated based on the speciation results. Iron in size-fractionated aerosol particles was mainly derived from mineral dust, regardless of aerosol diameter, because the enrichment factor of Fe was almost 1 in both coarse (PM<span class="inline-formula"<<sub<&gt;1.3</sub<</span<) and fine aerosol particles (PM<span class="inline-formula"<<sub<1.3</sub<</span<). Approximately 80 % of the total Fe (insoluble <span class="inline-formula"<+</span< labile Fe) was present in PM<span class="inline-formula"<<sub<&gt;1.3</sub<</span<, whereas labile Fe was mainly present in PM<span class="inline-formula"<<sub<1.3</sub<</span<. The Fe<span class="inline-formula"<<sub<sol</sub<</span<% in PM<span class="inline-formula"<<sub<&gt;1.3</sub<</span< was not significantly increased (<span class="inline-formula"<2.56±2.53</span< %, 0.00 %–8.50 %, <span class="inline-formula"<<i<n</i<=20</span<) by the atmospheric processes because mineral dust was not acidified beyond the buffer capacity of calcite. In contrast, mineral dust in PM<span class="inline-formula"<<sub<1.3</sub<</span< was acidified beyond the buffer capacity of calcite. As a result, Fe<span class="inline-formula"<<sub<sol</sub<</span<% in PM<span class="inline-formula"<<sub<1.3</sub<</span< (0.202 %–64.7 %, <span class="inline-formula"<<i<n</i<=10</span<) was an order of magnitude higher than that in PM<span class="inline-formula"<<sub<&gt;1.3</sub<</span<. The PM<span class="inline-formula"<<sub<1.3</sub<</span< contained ferric organic complexes with humic-like substances (Fe(III)-HULIS, but not Fe-oxalate complexes), and the abundance correlated with Fe<span class="inline-formula"<<sub<sol</sub<</span<%. Iron(III)-HULIS was formed during transport in the Pacific Ocean because Fe(III)-HULIS was not found in aerosol particles in Beijing and Japan. The pH estimations of mineral dust in PM<span class="inline-formula"<<sub<1.3</sub<</span< established that Fe was solubilized by proton-promoted dissolution under highly acidic conditions (pH <span class="inline-formula"<&lt;</span< 3.0), whereas Fe(III)-HULIS was stabilized under moderately acidic conditions (pH 3.0–6.0). Since the observed labile Fe concentration could not be reproduced by proton-promoted dissolution under moderately acidic conditions, the pH of mineral dust increased after proton-promoted dissolution. The cloud process in the marine atmosphere increases the mineral dust pH because the dust particles are covered with organic carbon and Na. The precipitation of ferrihydrite was suppressed by Fe(III)-HULIS owing to its high water solubility. Thus, the organic complexation of Fe with HULIS plays a significant role in the stabilization of Fe that was initially solubilized by proton-promoted dissolution.</p<</subfield></datafield><datafield tag="653" ind1=" " ind2="0"><subfield code="a">Physics</subfield></datafield><datafield tag="653" ind1=" " ind2="0"><subfield code="a">Chemistry</subfield></datafield><datafield tag="700" ind1="0" ind2=" "><subfield code="a">M. Kurisu</subfield><subfield code="e">verfasserin</subfield><subfield code="4">aut</subfield></datafield><datafield tag="700" ind1="0" ind2=" "><subfield code="a">M. Kurisu</subfield><subfield code="e">verfasserin</subfield><subfield code="4">aut</subfield></datafield><datafield tag="700" ind1="0" ind2=" "><subfield code="a">Y. 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iron (fe) speciation in size-fractionated aerosol particles in the pacific ocean: the role of organic complexation of fe with humic-like substances in controlling fe solubility |
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Iron (Fe) speciation in size-fractionated aerosol particles in the Pacific Ocean: The role of organic complexation of Fe with humic-like substances in controlling Fe solubility |
| abstract |
<p<Atmospheric deposition is one of the main sources of dissolved iron (Fe) in the ocean surfaces. Atmospheric processes are recognized as controlling fractional Fe solubility (Fe<span class="inline-formula"<<sub<sol</sub<</span<%) in marine aerosol particles. However, the impact of these processes on Fe<span class="inline-formula"<<sub<sol</sub<</span<% remains unclear. One of the reasons for this is the lack of field observations focusing on the relationship between Fe<span class="inline-formula"<<sub<sol</sub<</span<% and Fe species in marine aerosol particles. In particular, the effects of organic ligands on Fe<span class="inline-formula"<<sub<sol</sub<</span<% have not been thoroughly investigated in observational studies. In this study, Fe species in size-fractionated aerosol particles in the Pacific Ocean were determined using X-ray absorption fine structure (XAFS) spectroscopy. The internal mixing states of Fe and organic carbon were investigated using scanning transmission X-ray microscopy (STXM). The effects of atmospheric processes on Fe<span class="inline-formula"<<sub<sol</sub<</span<% in marine aerosol particles were investigated based on the speciation results. Iron in size-fractionated aerosol particles was mainly derived from mineral dust, regardless of aerosol diameter, because the enrichment factor of Fe was almost 1 in both coarse (PM<span class="inline-formula"<<sub<>1.3</sub<</span<) and fine aerosol particles (PM<span class="inline-formula"<<sub<1.3</sub<</span<). Approximately 80 % of the total Fe (insoluble <span class="inline-formula"<+</span< labile Fe) was present in PM<span class="inline-formula"<<sub<>1.3</sub<</span<, whereas labile Fe was mainly present in PM<span class="inline-formula"<<sub<1.3</sub<</span<. The Fe<span class="inline-formula"<<sub<sol</sub<</span<% in PM<span class="inline-formula"<<sub<>1.3</sub<</span< was not significantly increased (<span class="inline-formula"<2.56±2.53</span< %, 0.00 %–8.50 %, <span class="inline-formula"<<i<n</i<=20</span<) by the atmospheric processes because mineral dust was not acidified beyond the buffer capacity of calcite. In contrast, mineral dust in PM<span class="inline-formula"<<sub<1.3</sub<</span< was acidified beyond the buffer capacity of calcite. As a result, Fe<span class="inline-formula"<<sub<sol</sub<</span<% in PM<span class="inline-formula"<<sub<1.3</sub<</span< (0.202 %–64.7 %, <span class="inline-formula"<<i<n</i<=10</span<) was an order of magnitude higher than that in PM<span class="inline-formula"<<sub<>1.3</sub<</span<. The PM<span class="inline-formula"<<sub<1.3</sub<</span< contained ferric organic complexes with humic-like substances (Fe(III)-HULIS, but not Fe-oxalate complexes), and the abundance correlated with Fe<span class="inline-formula"<<sub<sol</sub<</span<%. Iron(III)-HULIS was formed during transport in the Pacific Ocean because Fe(III)-HULIS was not found in aerosol particles in Beijing and Japan. The pH estimations of mineral dust in PM<span class="inline-formula"<<sub<1.3</sub<</span< established that Fe was solubilized by proton-promoted dissolution under highly acidic conditions (pH <span class="inline-formula"<<</span< 3.0), whereas Fe(III)-HULIS was stabilized under moderately acidic conditions (pH 3.0–6.0). Since the observed labile Fe concentration could not be reproduced by proton-promoted dissolution under moderately acidic conditions, the pH of mineral dust increased after proton-promoted dissolution. The cloud process in the marine atmosphere increases the mineral dust pH because the dust particles are covered with organic carbon and Na. The precipitation of ferrihydrite was suppressed by Fe(III)-HULIS owing to its high water solubility. Thus, the organic complexation of Fe with HULIS plays a significant role in the stabilization of Fe that was initially solubilized by proton-promoted dissolution.</p< |
| abstractGer |
<p<Atmospheric deposition is one of the main sources of dissolved iron (Fe) in the ocean surfaces. Atmospheric processes are recognized as controlling fractional Fe solubility (Fe<span class="inline-formula"<<sub<sol</sub<</span<%) in marine aerosol particles. However, the impact of these processes on Fe<span class="inline-formula"<<sub<sol</sub<</span<% remains unclear. One of the reasons for this is the lack of field observations focusing on the relationship between Fe<span class="inline-formula"<<sub<sol</sub<</span<% and Fe species in marine aerosol particles. In particular, the effects of organic ligands on Fe<span class="inline-formula"<<sub<sol</sub<</span<% have not been thoroughly investigated in observational studies. In this study, Fe species in size-fractionated aerosol particles in the Pacific Ocean were determined using X-ray absorption fine structure (XAFS) spectroscopy. The internal mixing states of Fe and organic carbon were investigated using scanning transmission X-ray microscopy (STXM). The effects of atmospheric processes on Fe<span class="inline-formula"<<sub<sol</sub<</span<% in marine aerosol particles were investigated based on the speciation results. Iron in size-fractionated aerosol particles was mainly derived from mineral dust, regardless of aerosol diameter, because the enrichment factor of Fe was almost 1 in both coarse (PM<span class="inline-formula"<<sub<>1.3</sub<</span<) and fine aerosol particles (PM<span class="inline-formula"<<sub<1.3</sub<</span<). Approximately 80 % of the total Fe (insoluble <span class="inline-formula"<+</span< labile Fe) was present in PM<span class="inline-formula"<<sub<>1.3</sub<</span<, whereas labile Fe was mainly present in PM<span class="inline-formula"<<sub<1.3</sub<</span<. The Fe<span class="inline-formula"<<sub<sol</sub<</span<% in PM<span class="inline-formula"<<sub<>1.3</sub<</span< was not significantly increased (<span class="inline-formula"<2.56±2.53</span< %, 0.00 %–8.50 %, <span class="inline-formula"<<i<n</i<=20</span<) by the atmospheric processes because mineral dust was not acidified beyond the buffer capacity of calcite. In contrast, mineral dust in PM<span class="inline-formula"<<sub<1.3</sub<</span< was acidified beyond the buffer capacity of calcite. As a result, Fe<span class="inline-formula"<<sub<sol</sub<</span<% in PM<span class="inline-formula"<<sub<1.3</sub<</span< (0.202 %–64.7 %, <span class="inline-formula"<<i<n</i<=10</span<) was an order of magnitude higher than that in PM<span class="inline-formula"<<sub<>1.3</sub<</span<. The PM<span class="inline-formula"<<sub<1.3</sub<</span< contained ferric organic complexes with humic-like substances (Fe(III)-HULIS, but not Fe-oxalate complexes), and the abundance correlated with Fe<span class="inline-formula"<<sub<sol</sub<</span<%. Iron(III)-HULIS was formed during transport in the Pacific Ocean because Fe(III)-HULIS was not found in aerosol particles in Beijing and Japan. The pH estimations of mineral dust in PM<span class="inline-formula"<<sub<1.3</sub<</span< established that Fe was solubilized by proton-promoted dissolution under highly acidic conditions (pH <span class="inline-formula"<<</span< 3.0), whereas Fe(III)-HULIS was stabilized under moderately acidic conditions (pH 3.0–6.0). Since the observed labile Fe concentration could not be reproduced by proton-promoted dissolution under moderately acidic conditions, the pH of mineral dust increased after proton-promoted dissolution. The cloud process in the marine atmosphere increases the mineral dust pH because the dust particles are covered with organic carbon and Na. The precipitation of ferrihydrite was suppressed by Fe(III)-HULIS owing to its high water solubility. Thus, the organic complexation of Fe with HULIS plays a significant role in the stabilization of Fe that was initially solubilized by proton-promoted dissolution.</p< |
| abstract_unstemmed |
<p<Atmospheric deposition is one of the main sources of dissolved iron (Fe) in the ocean surfaces. Atmospheric processes are recognized as controlling fractional Fe solubility (Fe<span class="inline-formula"<<sub<sol</sub<</span<%) in marine aerosol particles. However, the impact of these processes on Fe<span class="inline-formula"<<sub<sol</sub<</span<% remains unclear. One of the reasons for this is the lack of field observations focusing on the relationship between Fe<span class="inline-formula"<<sub<sol</sub<</span<% and Fe species in marine aerosol particles. In particular, the effects of organic ligands on Fe<span class="inline-formula"<<sub<sol</sub<</span<% have not been thoroughly investigated in observational studies. In this study, Fe species in size-fractionated aerosol particles in the Pacific Ocean were determined using X-ray absorption fine structure (XAFS) spectroscopy. The internal mixing states of Fe and organic carbon were investigated using scanning transmission X-ray microscopy (STXM). The effects of atmospheric processes on Fe<span class="inline-formula"<<sub<sol</sub<</span<% in marine aerosol particles were investigated based on the speciation results. Iron in size-fractionated aerosol particles was mainly derived from mineral dust, regardless of aerosol diameter, because the enrichment factor of Fe was almost 1 in both coarse (PM<span class="inline-formula"<<sub<>1.3</sub<</span<) and fine aerosol particles (PM<span class="inline-formula"<<sub<1.3</sub<</span<). Approximately 80 % of the total Fe (insoluble <span class="inline-formula"<+</span< labile Fe) was present in PM<span class="inline-formula"<<sub<>1.3</sub<</span<, whereas labile Fe was mainly present in PM<span class="inline-formula"<<sub<1.3</sub<</span<. The Fe<span class="inline-formula"<<sub<sol</sub<</span<% in PM<span class="inline-formula"<<sub<>1.3</sub<</span< was not significantly increased (<span class="inline-formula"<2.56±2.53</span< %, 0.00 %–8.50 %, <span class="inline-formula"<<i<n</i<=20</span<) by the atmospheric processes because mineral dust was not acidified beyond the buffer capacity of calcite. In contrast, mineral dust in PM<span class="inline-formula"<<sub<1.3</sub<</span< was acidified beyond the buffer capacity of calcite. As a result, Fe<span class="inline-formula"<<sub<sol</sub<</span<% in PM<span class="inline-formula"<<sub<1.3</sub<</span< (0.202 %–64.7 %, <span class="inline-formula"<<i<n</i<=10</span<) was an order of magnitude higher than that in PM<span class="inline-formula"<<sub<>1.3</sub<</span<. The PM<span class="inline-formula"<<sub<1.3</sub<</span< contained ferric organic complexes with humic-like substances (Fe(III)-HULIS, but not Fe-oxalate complexes), and the abundance correlated with Fe<span class="inline-formula"<<sub<sol</sub<</span<%. Iron(III)-HULIS was formed during transport in the Pacific Ocean because Fe(III)-HULIS was not found in aerosol particles in Beijing and Japan. The pH estimations of mineral dust in PM<span class="inline-formula"<<sub<1.3</sub<</span< established that Fe was solubilized by proton-promoted dissolution under highly acidic conditions (pH <span class="inline-formula"<<</span< 3.0), whereas Fe(III)-HULIS was stabilized under moderately acidic conditions (pH 3.0–6.0). Since the observed labile Fe concentration could not be reproduced by proton-promoted dissolution under moderately acidic conditions, the pH of mineral dust increased after proton-promoted dissolution. The cloud process in the marine atmosphere increases the mineral dust pH because the dust particles are covered with organic carbon and Na. The precipitation of ferrihydrite was suppressed by Fe(III)-HULIS owing to its high water solubility. Thus, the organic complexation of Fe with HULIS plays a significant role in the stabilization of Fe that was initially solubilized by proton-promoted dissolution.</p< |
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GBV_USEFLAG_A SYSFLAG_A GBV_DOAJ SSG-OLC-PHA GBV_ILN_381 |
| title_short |
Iron (Fe) speciation in size-fractionated aerosol particles in the Pacific Ocean: The role of organic complexation of Fe with humic-like substances in controlling Fe solubility |
| url |
https://doi.org/10.5194/acp-22-9461-2022 https://doaj.org/article/60c21047b1d346f197d745a315a34076 https://acp.copernicus.org/articles/22/9461/2022/acp-22-9461-2022.pdf https://doaj.org/toc/1680-7316 https://doaj.org/toc/1680-7324 |
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| author2 |
M. Kurisu Y. Takeichi A. Sakaguchi H. Tanimoto Y. Tamenori A. Matsuki Y. Takahashi |
| author2Str |
M. Kurisu Y. Takeichi A. Sakaguchi H. Tanimoto Y. Tamenori A. Matsuki Y. Takahashi |
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QC - Physics |
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| doi_str |
10.5194/acp-22-9461-2022 |
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QC1-999 |
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2024-07-03T23:43:30.567Z |
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Sakata</subfield><subfield code="e">verfasserin</subfield><subfield code="4">aut</subfield></datafield><datafield tag="245" ind1="1" ind2="0"><subfield code="a">Iron (Fe) speciation in size-fractionated aerosol particles in the Pacific Ocean: The role of organic complexation of Fe with humic-like substances in controlling Fe solubility</subfield></datafield><datafield tag="264" ind1=" " ind2="1"><subfield code="c">2022</subfield></datafield><datafield tag="336" ind1=" " ind2=" "><subfield code="a">Text</subfield><subfield code="b">txt</subfield><subfield code="2">rdacontent</subfield></datafield><datafield tag="337" ind1=" " ind2=" "><subfield code="a">Computermedien</subfield><subfield code="b">c</subfield><subfield code="2">rdamedia</subfield></datafield><datafield tag="338" ind1=" " ind2=" "><subfield code="a">Online-Ressource</subfield><subfield code="b">cr</subfield><subfield code="2">rdacarrier</subfield></datafield><datafield tag="520" ind1=" " ind2=" "><subfield code="a"><p<Atmospheric deposition is one of the main sources of dissolved iron (Fe) in the ocean surfaces. Atmospheric processes are recognized as controlling fractional Fe solubility (Fe<span class="inline-formula"<<sub<sol</sub<</span<%) in marine aerosol particles. However, the impact of these processes on Fe<span class="inline-formula"<<sub<sol</sub<</span<% remains unclear. One of the reasons for this is the lack of field observations focusing on the relationship between Fe<span class="inline-formula"<<sub<sol</sub<</span<% and Fe species in marine aerosol particles. In particular, the effects of organic ligands on Fe<span class="inline-formula"<<sub<sol</sub<</span<% have not been thoroughly investigated in observational studies. In this study, Fe species in size-fractionated aerosol particles in the Pacific Ocean were determined using X-ray absorption fine structure (XAFS) spectroscopy. The internal mixing states of Fe and organic carbon were investigated using scanning transmission X-ray microscopy (STXM). The effects of atmospheric processes on Fe<span class="inline-formula"<<sub<sol</sub<</span<% in marine aerosol particles were investigated based on the speciation results. Iron in size-fractionated aerosol particles was mainly derived from mineral dust, regardless of aerosol diameter, because the enrichment factor of Fe was almost 1 in both coarse (PM<span class="inline-formula"<<sub<&gt;1.3</sub<</span<) and fine aerosol particles (PM<span class="inline-formula"<<sub<1.3</sub<</span<). Approximately 80 % of the total Fe (insoluble <span class="inline-formula"<+</span< labile Fe) was present in PM<span class="inline-formula"<<sub<&gt;1.3</sub<</span<, whereas labile Fe was mainly present in PM<span class="inline-formula"<<sub<1.3</sub<</span<. The Fe<span class="inline-formula"<<sub<sol</sub<</span<% in PM<span class="inline-formula"<<sub<&gt;1.3</sub<</span< was not significantly increased (<span class="inline-formula"<2.56±2.53</span< %, 0.00 %–8.50 %, <span class="inline-formula"<<i<n</i<=20</span<) by the atmospheric processes because mineral dust was not acidified beyond the buffer capacity of calcite. In contrast, mineral dust in PM<span class="inline-formula"<<sub<1.3</sub<</span< was acidified beyond the buffer capacity of calcite. As a result, Fe<span class="inline-formula"<<sub<sol</sub<</span<% in PM<span class="inline-formula"<<sub<1.3</sub<</span< (0.202 %–64.7 %, <span class="inline-formula"<<i<n</i<=10</span<) was an order of magnitude higher than that in PM<span class="inline-formula"<<sub<&gt;1.3</sub<</span<. The PM<span class="inline-formula"<<sub<1.3</sub<</span< contained ferric organic complexes with humic-like substances (Fe(III)-HULIS, but not Fe-oxalate complexes), and the abundance correlated with Fe<span class="inline-formula"<<sub<sol</sub<</span<%. Iron(III)-HULIS was formed during transport in the Pacific Ocean because Fe(III)-HULIS was not found in aerosol particles in Beijing and Japan. The pH estimations of mineral dust in PM<span class="inline-formula"<<sub<1.3</sub<</span< established that Fe was solubilized by proton-promoted dissolution under highly acidic conditions (pH <span class="inline-formula"<&lt;</span< 3.0), whereas Fe(III)-HULIS was stabilized under moderately acidic conditions (pH 3.0–6.0). Since the observed labile Fe concentration could not be reproduced by proton-promoted dissolution under moderately acidic conditions, the pH of mineral dust increased after proton-promoted dissolution. The cloud process in the marine atmosphere increases the mineral dust pH because the dust particles are covered with organic carbon and Na. The precipitation of ferrihydrite was suppressed by Fe(III)-HULIS owing to its high water solubility. Thus, the organic complexation of Fe with HULIS plays a significant role in the stabilization of Fe that was initially solubilized by proton-promoted dissolution.</p<</subfield></datafield><datafield tag="653" ind1=" " ind2="0"><subfield code="a">Physics</subfield></datafield><datafield tag="653" ind1=" " ind2="0"><subfield code="a">Chemistry</subfield></datafield><datafield tag="700" ind1="0" ind2=" "><subfield code="a">M. Kurisu</subfield><subfield code="e">verfasserin</subfield><subfield code="4">aut</subfield></datafield><datafield tag="700" ind1="0" ind2=" "><subfield code="a">M. Kurisu</subfield><subfield code="e">verfasserin</subfield><subfield code="4">aut</subfield></datafield><datafield tag="700" ind1="0" ind2=" "><subfield code="a">Y. 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