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Title: Influence of iron redox cycling on organo-mineral associations in Arctic tundra soil

Abstract

Arctic tundra stores large quantities of soil organic matter under varying redox conditions. As the climate warms, these carbon reservoirs are susceptible to increased rates of decomposition and release to the atmosphere as the greenhouse gases carbon dioxide (CO2) and methane (CH4). Geochemical interactions between soil organic matter and minerals influence decomposition in many environments but remain poorly understood in Arctic tundra systems and are not considered in decomposition models. The accumulation of iron (Fe) oxyhydroxides and organo- iron precipitates at redox interfaces may be particularly important for carbon cycling given that ferric iron [Fe(III)] species can enhance decomposition by serving as terminal electron acceptors in anoxic soils or inhibit microbial decomposition by binding organic molecules. Here in this paper, we examine chemical properties of solid-phase Fe and organic matter in organic and mineral horizons within the seasonally thawed active layer of Arctic tundra on the North Slope of Alaska. Spectroscopic techniques, including micro-X-ray fluorescence ( XRF) mapping, micro-X-ray absorption near-edge structure ( XANES) spectroscopy, and Fourier transform infrared spectroscopy (FTIR), were coupled with chemical sequential extractions and physical density fractionations to evaluate the spatial distribution and speciation of Fe-bearing phases and associated organic matter in soils. Organic horizons weremore » enriched in poorly crystalline and crystalline iron oxides, and approximately 60% of total Fe stored in organic horizons was calculated to derive from upward translocation from anoxic mineral horizons. Ferrihydrite and goethite were present as coatings on mineral grains and plant debris, and in aggregates with clays and particulate organic matter. Minor amounts of ferrous iron [Fe(II)] were present in iron sulfides (i.e., pyrite and greigite) in mineral horizon soils and iron phosphates (vivianite) in organic horizons. Concentrations of organic carbon in the organic horizons (28 ± 5% wt. % C) were approximately twice the concentrations in the mineral horizons (14 ± 2 % wt. C), and organic matter was dominated by base-extractable and insoluble organics enriched in aromatic and aliphatic moieties. Conversely, water-soluble organic molecules and organics solubilized through acid-dissolution of iron oxides comprised < 2% of soil organic C and were consistent with a mixture of alcohols, sugars, and small molecular weight organic acids and aromatics released through decomposition of larger molecules. Integrated over the entire depth of the active layer, soils contained 11± 4 kg m-2 low- density, particulate organic C and 19 ± 6 kg m-2 high-density, mineral-associated organic C, indicating that 63 ±19% of organic C in the active layer was associated with the mineral fraction. We conclude that organic horizons were enriched in poorly crystalline and crystalline iron oxide phases derived from upward translocation of dissolved Fe(II) and Fe(III) from mineral horizons. Precipitation of iron oxides at the redox interface has the potential to contribute to mineral protection of organic matter and increase the residence time of organic carbon in arctic soils. Our results suggest that iron oxides may inhibit organic carbon degradation by binding low-molecular-weight organic compounds, stabilizing soil aggregates, and forming thick coatings around particulate organic matter. Organic matter released through acid-dissolution of iron oxides could represent a small pool of readily-degradable organic molecules temporarily stabilized by sorption to iron oxyhydroxide surfaces. The distribution of iron in organic complexes and inorganic phases throughout the soil column constrains Fe(III) availability to anaerobic iron-reducing microorganisms that oxidize organic matter to produce CO2 and CH4 in these anoxic environments. Future predictions of carbon storage and respiration in the arctic tundra should consider such influences of mineral stabilization under changing redox conditions.« less

Authors:
 [1];  [2];  [1];  [3];  [1];  [4];  [5];  [6]
+ Show Author Affiliations
  1. Kent State Univ., Kent, OH (United States). Dept. of Geology
  2. (ORNL), Oak Ridge, TN (United States). Environmental Sciences Division
  3. (United States). Dept. of Geology
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Biosciences Division
  5. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Environmental Sciences Division
  6. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Biosciences Divisio
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER); National Science Foundation (NSF)
OSTI Identifier:
1356942
Alternate Identifier(s):
OSTI ID: 1398654
Grant/Contract Number:  
AC05-00OR22725; AC02-06CH11357; FG02-94ER14466; DBI-1263263
Resource Type:
Accepted Manuscript
Journal Name:
Geochimica et Cosmochimica Acta
Additional Journal Information:
Journal Volume: 207; Journal Issue: C; Journal ID: ISSN 0016-7037
Publisher:
The Geochemical Society; The Meteoritical Society
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; 59 BASIC BIOLOGICAL SCIENCES; Iron; Soil organic matter; Arctic; Tundra

Citation Formats

Herndon, Elizabeth, Oak Ridge National Lab., AlBashaireh, Amineh, College of Wooster, OH, Singer, David, Chowdhury, Taniya Roy, Gu, Baohua, and Graham, David. Influence of iron redox cycling on organo-mineral associations in Arctic tundra soil. United States: N. p., 2017. Web. doi:10.1016/j.gca.2017.02.034.
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Herndon, Elizabeth, Oak Ridge National Lab., AlBashaireh, Amineh, College of Wooster, OH, Singer, David, Chowdhury, Taniya Roy, Gu, Baohua, & Graham, David. Influence of iron redox cycling on organo-mineral associations in Arctic tundra soil. United States. https://doi.org/10.1016/j.gca.2017.02.034
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Herndon, Elizabeth, Oak Ridge National Lab., AlBashaireh, Amineh, College of Wooster, OH, Singer, David, Chowdhury, Taniya Roy, Gu, Baohua, and Graham, David. Sat . "Influence of iron redox cycling on organo-mineral associations in Arctic tundra soil". United States. https://doi.org/10.1016/j.gca.2017.02.034. https://www.osti.gov/servlets/purl/1356942.
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@article{osti_1356942,
title = {Influence of iron redox cycling on organo-mineral associations in Arctic tundra soil},
author = {Herndon, Elizabeth and Oak Ridge National Lab. and AlBashaireh, Amineh and College of Wooster, OH and Singer, David and Chowdhury, Taniya Roy and Gu, Baohua and Graham, David},
abstractNote = {Arctic tundra stores large quantities of soil organic matter under varying redox conditions. As the climate warms, these carbon reservoirs are susceptible to increased rates of decomposition and release to the atmosphere as the greenhouse gases carbon dioxide (CO2) and methane (CH4). Geochemical interactions between soil organic matter and minerals influence decomposition in many environments but remain poorly understood in Arctic tundra systems and are not considered in decomposition models. The accumulation of iron (Fe) oxyhydroxides and organo- iron precipitates at redox interfaces may be particularly important for carbon cycling given that ferric iron [Fe(III)] species can enhance decomposition by serving as terminal electron acceptors in anoxic soils or inhibit microbial decomposition by binding organic molecules. Here in this paper, we examine chemical properties of solid-phase Fe and organic matter in organic and mineral horizons within the seasonally thawed active layer of Arctic tundra on the North Slope of Alaska. Spectroscopic techniques, including micro-X-ray fluorescence ( XRF) mapping, micro-X-ray absorption near-edge structure ( XANES) spectroscopy, and Fourier transform infrared spectroscopy (FTIR), were coupled with chemical sequential extractions and physical density fractionations to evaluate the spatial distribution and speciation of Fe-bearing phases and associated organic matter in soils. Organic horizons were enriched in poorly crystalline and crystalline iron oxides, and approximately 60% of total Fe stored in organic horizons was calculated to derive from upward translocation from anoxic mineral horizons. Ferrihydrite and goethite were present as coatings on mineral grains and plant debris, and in aggregates with clays and particulate organic matter. Minor amounts of ferrous iron [Fe(II)] were present in iron sulfides (i.e., pyrite and greigite) in mineral horizon soils and iron phosphates (vivianite) in organic horizons. Concentrations of organic carbon in the organic horizons (28 ± 5% wt. % C) were approximately twice the concentrations in the mineral horizons (14 ± 2 % wt. C), and organic matter was dominated by base-extractable and insoluble organics enriched in aromatic and aliphatic moieties. Conversely, water-soluble organic molecules and organics solubilized through acid-dissolution of iron oxides comprised < 2% of soil organic C and were consistent with a mixture of alcohols, sugars, and small molecular weight organic acids and aromatics released through decomposition of larger molecules. Integrated over the entire depth of the active layer, soils contained 11± 4 kg m-2 low- density, particulate organic C and 19 ± 6 kg m-2 high-density, mineral-associated organic C, indicating that 63 ±19% of organic C in the active layer was associated with the mineral fraction. We conclude that organic horizons were enriched in poorly crystalline and crystalline iron oxide phases derived from upward translocation of dissolved Fe(II) and Fe(III) from mineral horizons. Precipitation of iron oxides at the redox interface has the potential to contribute to mineral protection of organic matter and increase the residence time of organic carbon in arctic soils. Our results suggest that iron oxides may inhibit organic carbon degradation by binding low-molecular-weight organic compounds, stabilizing soil aggregates, and forming thick coatings around particulate organic matter. Organic matter released through acid-dissolution of iron oxides could represent a small pool of readily-degradable organic molecules temporarily stabilized by sorption to iron oxyhydroxide surfaces. The distribution of iron in organic complexes and inorganic phases throughout the soil column constrains Fe(III) availability to anaerobic iron-reducing microorganisms that oxidize organic matter to produce CO2 and CH4 in these anoxic environments. Future predictions of carbon storage and respiration in the arctic tundra should consider such influences of mineral stabilization under changing redox conditions.},
doi = {10.1016/j.gca.2017.02.034},
journal = {Geochimica et Cosmochimica Acta},
number = C,
volume = 207,
place = {United States},
year = {Sat Mar 25 00:00:00 EDT 2017},
month = {Sat Mar 25 00:00:00 EDT 2017}
}
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