Composition and sources of lipid compounds in speleothem calcite from southwestern Oregon and their paleoenvironmental implications

Ahmed I. Rushdi, Peter U Clark, Alan C. Mix, Vasile Ersek, Bernd R. T. Simoneit, Hai Cheng, R. Lawrence Edwards

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    Abstract

    We analyzed speleothem calcite from the Oregon Caves National Monument, southwestern Oregon, to determine the preservation, distribution, concentrations and sources of aliphatic lipid compounds preserved in the calcite. Maximum speleothem growth rate occurs during interglaciations and minimum during glacial intervals. Concentrations of the total lipid compounds range from 0.5 to 12.9 μg g−1. They increase at times of low speleothem growth rate, suggesting dilution, whereas the apparent accumulation rate of lipid compounds tends to be highest during times of fastest speleothem growth rate. Such increased accumulation generally corresponds to times of warm (interglacial) climate, suggesting either a greater source of organic materials during interglacial times and/or greater efficiency of compound capture during more rapid calcite growth. Aliphatic lipid compounds include homologous n-alkanoic acids, n-alkanols and methyl n-alkanoates and sterols with concentrations ranging from 0.3 to 7.8 μg g−1, 0.4 to 1.1 μg g−1, 0.5 to 9.6 μg g−1 and 0.1 to 2.7 μg g−1, respectively. Minor amounts of branched methyl n-alkanoates and dimethyl n-alkanedioates are also present. The high concentrations of methyl n-alkanoates are the result of esterification reactions of free fatty acids in alkaline solutions with high pH values associated with the dripping cave waters. The distribution patterns and geochemical parameters and indices indicate that the major sources of the aliphatic lipids involved leaching from higher plants and microbial residues derived from the soil zone above the cave system. The estimated percentage of microbial inputs ranged from 42 to 90% of the total lipids and also showed an increase in accumulation during warm climates. These well-preserved lipid compounds in speleothem calcite could be used as biomarkers for paleoenvironmental study.
    LanguageEnglish
    Pages1245-1261
    JournalEnvironmental Earth Sciences
    Volume62
    Issue number6
    DOIs
    Publication statusPublished - Mar 2011

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    speleothem
    calcite
    lipid
    interglacial
    cave
    cave system
    sterol
    climate
    monument
    accumulation rate
    biomarker
    dilution
    fatty acid
    leaching
    acid

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    Rushdi, Ahmed I. ; Clark, Peter U ; Mix, Alan C. ; Ersek, Vasile ; Simoneit, Bernd R. T. ; Cheng, Hai ; Edwards, R. Lawrence. / Composition and sources of lipid compounds in speleothem calcite from southwestern Oregon and their paleoenvironmental implications. In: Environmental Earth Sciences. 2011 ; Vol. 62, No. 6. pp. 1245-1261.
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    title = "Composition and sources of lipid compounds in speleothem calcite from southwestern Oregon and their paleoenvironmental implications",
    abstract = "We analyzed speleothem calcite from the Oregon Caves National Monument, southwestern Oregon, to determine the preservation, distribution, concentrations and sources of aliphatic lipid compounds preserved in the calcite. Maximum speleothem growth rate occurs during interglaciations and minimum during glacial intervals. Concentrations of the total lipid compounds range from 0.5 to 12.9 μg g−1. They increase at times of low speleothem growth rate, suggesting dilution, whereas the apparent accumulation rate of lipid compounds tends to be highest during times of fastest speleothem growth rate. Such increased accumulation generally corresponds to times of warm (interglacial) climate, suggesting either a greater source of organic materials during interglacial times and/or greater efficiency of compound capture during more rapid calcite growth. Aliphatic lipid compounds include homologous n-alkanoic acids, n-alkanols and methyl n-alkanoates and sterols with concentrations ranging from 0.3 to 7.8 μg g−1, 0.4 to 1.1 μg g−1, 0.5 to 9.6 μg g−1 and 0.1 to 2.7 μg g−1, respectively. Minor amounts of branched methyl n-alkanoates and dimethyl n-alkanedioates are also present. The high concentrations of methyl n-alkanoates are the result of esterification reactions of free fatty acids in alkaline solutions with high pH values associated with the dripping cave waters. The distribution patterns and geochemical parameters and indices indicate that the major sources of the aliphatic lipids involved leaching from higher plants and microbial residues derived from the soil zone above the cave system. The estimated percentage of microbial inputs ranged from 42 to 90{\%} of the total lipids and also showed an increase in accumulation during warm climates. These well-preserved lipid compounds in speleothem calcite could be used as biomarkers for paleoenvironmental study.",
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    Composition and sources of lipid compounds in speleothem calcite from southwestern Oregon and their paleoenvironmental implications. / Rushdi, Ahmed I.; Clark, Peter U; Mix, Alan C.; Ersek, Vasile; Simoneit, Bernd R. T.; Cheng, Hai; Edwards, R. Lawrence.

    In: Environmental Earth Sciences, Vol. 62, No. 6, 03.2011, p. 1245-1261.

    Research output: Contribution to journalArticle

    TY - JOUR

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    AU - Rushdi, Ahmed I.

    AU - Clark, Peter U

    AU - Mix, Alan C.

    AU - Ersek, Vasile

    AU - Simoneit, Bernd R. T.

    AU - Cheng, Hai

    AU - Edwards, R. Lawrence

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    N2 - We analyzed speleothem calcite from the Oregon Caves National Monument, southwestern Oregon, to determine the preservation, distribution, concentrations and sources of aliphatic lipid compounds preserved in the calcite. Maximum speleothem growth rate occurs during interglaciations and minimum during glacial intervals. Concentrations of the total lipid compounds range from 0.5 to 12.9 μg g−1. They increase at times of low speleothem growth rate, suggesting dilution, whereas the apparent accumulation rate of lipid compounds tends to be highest during times of fastest speleothem growth rate. Such increased accumulation generally corresponds to times of warm (interglacial) climate, suggesting either a greater source of organic materials during interglacial times and/or greater efficiency of compound capture during more rapid calcite growth. Aliphatic lipid compounds include homologous n-alkanoic acids, n-alkanols and methyl n-alkanoates and sterols with concentrations ranging from 0.3 to 7.8 μg g−1, 0.4 to 1.1 μg g−1, 0.5 to 9.6 μg g−1 and 0.1 to 2.7 μg g−1, respectively. Minor amounts of branched methyl n-alkanoates and dimethyl n-alkanedioates are also present. The high concentrations of methyl n-alkanoates are the result of esterification reactions of free fatty acids in alkaline solutions with high pH values associated with the dripping cave waters. The distribution patterns and geochemical parameters and indices indicate that the major sources of the aliphatic lipids involved leaching from higher plants and microbial residues derived from the soil zone above the cave system. The estimated percentage of microbial inputs ranged from 42 to 90% of the total lipids and also showed an increase in accumulation during warm climates. These well-preserved lipid compounds in speleothem calcite could be used as biomarkers for paleoenvironmental study.

    AB - We analyzed speleothem calcite from the Oregon Caves National Monument, southwestern Oregon, to determine the preservation, distribution, concentrations and sources of aliphatic lipid compounds preserved in the calcite. Maximum speleothem growth rate occurs during interglaciations and minimum during glacial intervals. Concentrations of the total lipid compounds range from 0.5 to 12.9 μg g−1. They increase at times of low speleothem growth rate, suggesting dilution, whereas the apparent accumulation rate of lipid compounds tends to be highest during times of fastest speleothem growth rate. Such increased accumulation generally corresponds to times of warm (interglacial) climate, suggesting either a greater source of organic materials during interglacial times and/or greater efficiency of compound capture during more rapid calcite growth. Aliphatic lipid compounds include homologous n-alkanoic acids, n-alkanols and methyl n-alkanoates and sterols with concentrations ranging from 0.3 to 7.8 μg g−1, 0.4 to 1.1 μg g−1, 0.5 to 9.6 μg g−1 and 0.1 to 2.7 μg g−1, respectively. Minor amounts of branched methyl n-alkanoates and dimethyl n-alkanedioates are also present. The high concentrations of methyl n-alkanoates are the result of esterification reactions of free fatty acids in alkaline solutions with high pH values associated with the dripping cave waters. The distribution patterns and geochemical parameters and indices indicate that the major sources of the aliphatic lipids involved leaching from higher plants and microbial residues derived from the soil zone above the cave system. The estimated percentage of microbial inputs ranged from 42 to 90% of the total lipids and also showed an increase in accumulation during warm climates. These well-preserved lipid compounds in speleothem calcite could be used as biomarkers for paleoenvironmental study.

    U2 - 10.1007/s12665-010-0613-4

    DO - 10.1007/s12665-010-0613-4

    M3 - Article

    VL - 62

    SP - 1245

    EP - 1261

    JO - Environmental Earth Sciences

    T2 - Environmental Earth Sciences

    JF - Environmental Earth Sciences

    SN - 1866-6280

    IS - 6

    ER -