Petroleum-derived dissolved organic matter from natural seepage in deep sea environments
Natural petroleum seepage discharges approximately 600,000 tons of oil every year into the marine environment. A fraction of the released petroleum is water-soluble and becomes part of oceanic dissolved organic matter (DOM), one of the largest and most complex pools of organic matter on Earth’s surf...
Ausführliche Beschreibung
Autor*in: |
Brünjes, Jonas [verfasserIn] Schubotz, Florence - 1981- [akademischer betreuerIn] Hinrichs, Kai-Uwe - 1963- [akademischer betreuerIn] Kujawinski, Elizabeth [akademischer betreuerIn] |
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Körperschaften: |
Universität Bremen [Grad-verleihende Institution] |
Hochschulschrift: |
Dissertation ; Universität Bremen ; 2023 |
Format: |
E-Book |
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Sprache: |
Englisch |
Erschienen: |
Bremen: 2023 |
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Rechteinformationen: |
Open Access Namensnennung 4.0 International ; CC BY 4.0 |
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Schlagwörter: |
dissolved organic matter (DOM) |
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Formangabe: |
Hochschulschrift |
Umfang: |
1 Online-Ressource (146 Seiten) ; Illustrationen |
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Links: |
Link aufrufen |
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DOI / URN: |
urn:nbn:de:gbv:46-elib68460 10.26092/elib/2185 |
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Katalog-ID: |
1845521927 |
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520 | |a Natural petroleum seepage discharges approximately 600,000 tons of oil every year into the marine environment. A fraction of the released petroleum is water-soluble and becomes part of oceanic dissolved organic matter (DOM), one of the largest and most complex pools of organic matter on Earth’s surface. Despite the constant discharge of petroleum by natural seepage, the environmental implications and persistence of petroleum-derived DOM are vastly unknown. This thesis investigates molecular transformations of DOM in natural petroleum seepages and assesses the potential release of petroleum-compounds to oceanic deep-sea DOM. In a first step, the release of oil-derived DOM from natural deep sea asphalt seeps was studied using controlled laboratory incubation experiments. Fresh asphalt samples collected at the Chapopote asphalt volcano in the Southern Gulf of Mexico were incubated aerobically in artificial seawater over four weeks. The compositional changes in the water-soluble fraction of asphalt-derived DOM were determined with ultrahigh-resolution mass spectrometry (Fourier-transform ion cyclotron resonance mass spectrometry, FT-ICR-MS) and by excitation-emission matrix spectroscopy to characterize fluorescent DOM (FDOM) applying parallel factor (PARAFAC) analysis. Result showed that highly reduced aliphatic asphalt-derived DOM was readily biodegraded, while aromatic and sulfur-containing DOM (DOS) appeared to be less bioavailable and accumulated in the aqueous phase. This indicates that natural asphalt and potentially other petroleum seepages can be marine sources of recalcitrant dissolved black carbon (DBC) which has apparent radiocarbon ages older than 20,000 years in the deep sea. In order to evaluate this laboratory finding in the natural environment, petroleum-derived DOM was investigated in the Guaymas Basin. The Guaymas Basin in the Gulf of California is a young rift system where hot basaltic sill intrusions into organic-rich sediments lead to the generation of large amounts of complex petroleum compounds. The effect of hydrothermal heating and the resulting presence of petroleum compounds on the porewater DOM composition were investigated. Sediment samples were retrieved from sites with in situ temperatures ranging from 4 to >106 °C that exhibited a strong petroleum smell and partially contained oil droplets. A strong correlation of sediment temperature to both composition and quantity of porewater DOM was observed, driven by enhanced microbial transformation of organic matter at temperatures below ~60 °C and increasingly sulfurized DOM at high-temperature sites. DOM associated with hydrothermal heating had elevated contributions of highly unsaturated, reduced, sulfur-containing DOM and petroleum-associated PARAFAC components. A considerable DOM fraction of hydrothermal origin was present both in overlying bottom waters and in recalcitrant deep-sea DOM, suggesting hydrothermal sediments as a source of recalcitrant DOM to the water column. To assess elemental fluxes in DOM of hydrothermal porewaters, composition and quantities of DOM from sedimentary porewaters and from the hot-water soluble fraction by Soxhlet extraction of the same sediments were evaluated. Results showed highly elevated concentrations of DBC and potentially recalcitrant DOS in porewater, suggesting the release of both DOM fractions from hydrothermal sediments. DBC in porewaters and hot-water extracts originated from two distinct sources: hydrothermal petroleum and re-dissolved presumably terrestrial-derived, pre-aged DBC. This study further assessed quantities of DBC and dissolved organic nitrogen, sulfur and phosphorus that could be discharged into the water column in case of basin-wide hydrothermal heating. Results indicate that hydrothermal alteration and subsequent petroleum impregnation of sediments can be sources of recalcitrant DOS and DBC to deep sea environments. This thesis provides important novel information about the transformation and release of water-soluble petroleum compounds from natural deep-sea seepage into the marine environment. By introducing radiocarbon-depleted DOM to the marine environment, natural petroleum seepages and hydrothermal alteration of sediments with subsequent petroleum impregnation may be an explanation for observed old radiocarbon ages of recalcitrant DOM in the deep ocean. | ||
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urn:nbn:de:gbv:46-elib68460 urn 10.26092/elib/2185 doi (DE-627)1845521927 (DE-599)KXP1845521927 (OCoLC)1379165877 (OAEPFHB)elib/2185 DE-627 ger DE-627 rda eng XA-DE-HB 553.2 DE-101 550 DE-101 Brünjes, Jonas verfasserin (orcid)0000-0001-7759-2583 aut Petroleum-derived dissolved organic matter from natural seepage in deep sea environments vorgelegt von Jonas Brünjes Bremen 2023 1 Online-Ressource (146 Seiten) Illustrationen Text txt rdacontent Computermedien c rdamedia Online-Ressource cr rdacarrier Dissertation Universität Bremen 2023 DE-46 Open Access Controlled Vocabulary for Access Rights http://purl.org/coar/access_right/c_abf2 Natural petroleum seepage discharges approximately 600,000 tons of oil every year into the marine environment. A fraction of the released petroleum is water-soluble and becomes part of oceanic dissolved organic matter (DOM), one of the largest and most complex pools of organic matter on Earth’s surface. Despite the constant discharge of petroleum by natural seepage, the environmental implications and persistence of petroleum-derived DOM are vastly unknown. This thesis investigates molecular transformations of DOM in natural petroleum seepages and assesses the potential release of petroleum-compounds to oceanic deep-sea DOM. In a first step, the release of oil-derived DOM from natural deep sea asphalt seeps was studied using controlled laboratory incubation experiments. Fresh asphalt samples collected at the Chapopote asphalt volcano in the Southern Gulf of Mexico were incubated aerobically in artificial seawater over four weeks. The compositional changes in the water-soluble fraction of asphalt-derived DOM were determined with ultrahigh-resolution mass spectrometry (Fourier-transform ion cyclotron resonance mass spectrometry, FT-ICR-MS) and by excitation-emission matrix spectroscopy to characterize fluorescent DOM (FDOM) applying parallel factor (PARAFAC) analysis. Result showed that highly reduced aliphatic asphalt-derived DOM was readily biodegraded, while aromatic and sulfur-containing DOM (DOS) appeared to be less bioavailable and accumulated in the aqueous phase. This indicates that natural asphalt and potentially other petroleum seepages can be marine sources of recalcitrant dissolved black carbon (DBC) which has apparent radiocarbon ages older than 20,000 years in the deep sea. In order to evaluate this laboratory finding in the natural environment, petroleum-derived DOM was investigated in the Guaymas Basin. The Guaymas Basin in the Gulf of California is a young rift system where hot basaltic sill intrusions into organic-rich sediments lead to the generation of large amounts of complex petroleum compounds. The effect of hydrothermal heating and the resulting presence of petroleum compounds on the porewater DOM composition were investigated. Sediment samples were retrieved from sites with in situ temperatures ranging from 4 to >106 °C that exhibited a strong petroleum smell and partially contained oil droplets. A strong correlation of sediment temperature to both composition and quantity of porewater DOM was observed, driven by enhanced microbial transformation of organic matter at temperatures below ~60 °C and increasingly sulfurized DOM at high-temperature sites. DOM associated with hydrothermal heating had elevated contributions of highly unsaturated, reduced, sulfur-containing DOM and petroleum-associated PARAFAC components. A considerable DOM fraction of hydrothermal origin was present both in overlying bottom waters and in recalcitrant deep-sea DOM, suggesting hydrothermal sediments as a source of recalcitrant DOM to the water column. To assess elemental fluxes in DOM of hydrothermal porewaters, composition and quantities of DOM from sedimentary porewaters and from the hot-water soluble fraction by Soxhlet extraction of the same sediments were evaluated. Results showed highly elevated concentrations of DBC and potentially recalcitrant DOS in porewater, suggesting the release of both DOM fractions from hydrothermal sediments. DBC in porewaters and hot-water extracts originated from two distinct sources: hydrothermal petroleum and re-dissolved presumably terrestrial-derived, pre-aged DBC. This study further assessed quantities of DBC and dissolved organic nitrogen, sulfur and phosphorus that could be discharged into the water column in case of basin-wide hydrothermal heating. Results indicate that hydrothermal alteration and subsequent petroleum impregnation of sediments can be sources of recalcitrant DOS and DBC to deep sea environments. This thesis provides important novel information about the transformation and release of water-soluble petroleum compounds from natural deep-sea seepage into the marine environment. By introducing radiocarbon-depleted DOM to the marine environment, natural petroleum seepages and hydrothermal alteration of sediments with subsequent petroleum impregnation may be an explanation for observed old radiocarbon ages of recalcitrant DOM in the deep ocean. 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spelling |
urn:nbn:de:gbv:46-elib68460 urn 10.26092/elib/2185 doi (DE-627)1845521927 (DE-599)KXP1845521927 (OCoLC)1379165877 (OAEPFHB)elib/2185 DE-627 ger DE-627 rda eng XA-DE-HB 553.2 DE-101 550 DE-101 Brünjes, Jonas verfasserin (orcid)0000-0001-7759-2583 aut Petroleum-derived dissolved organic matter from natural seepage in deep sea environments vorgelegt von Jonas Brünjes Bremen 2023 1 Online-Ressource (146 Seiten) Illustrationen Text txt rdacontent Computermedien c rdamedia Online-Ressource cr rdacarrier Dissertation Universität Bremen 2023 DE-46 Open Access Controlled Vocabulary for Access Rights http://purl.org/coar/access_right/c_abf2 Natural petroleum seepage discharges approximately 600,000 tons of oil every year into the marine environment. A fraction of the released petroleum is water-soluble and becomes part of oceanic dissolved organic matter (DOM), one of the largest and most complex pools of organic matter on Earth’s surface. Despite the constant discharge of petroleum by natural seepage, the environmental implications and persistence of petroleum-derived DOM are vastly unknown. This thesis investigates molecular transformations of DOM in natural petroleum seepages and assesses the potential release of petroleum-compounds to oceanic deep-sea DOM. In a first step, the release of oil-derived DOM from natural deep sea asphalt seeps was studied using controlled laboratory incubation experiments. Fresh asphalt samples collected at the Chapopote asphalt volcano in the Southern Gulf of Mexico were incubated aerobically in artificial seawater over four weeks. The compositional changes in the water-soluble fraction of asphalt-derived DOM were determined with ultrahigh-resolution mass spectrometry (Fourier-transform ion cyclotron resonance mass spectrometry, FT-ICR-MS) and by excitation-emission matrix spectroscopy to characterize fluorescent DOM (FDOM) applying parallel factor (PARAFAC) analysis. Result showed that highly reduced aliphatic asphalt-derived DOM was readily biodegraded, while aromatic and sulfur-containing DOM (DOS) appeared to be less bioavailable and accumulated in the aqueous phase. This indicates that natural asphalt and potentially other petroleum seepages can be marine sources of recalcitrant dissolved black carbon (DBC) which has apparent radiocarbon ages older than 20,000 years in the deep sea. In order to evaluate this laboratory finding in the natural environment, petroleum-derived DOM was investigated in the Guaymas Basin. The Guaymas Basin in the Gulf of California is a young rift system where hot basaltic sill intrusions into organic-rich sediments lead to the generation of large amounts of complex petroleum compounds. The effect of hydrothermal heating and the resulting presence of petroleum compounds on the porewater DOM composition were investigated. Sediment samples were retrieved from sites with in situ temperatures ranging from 4 to >106 °C that exhibited a strong petroleum smell and partially contained oil droplets. A strong correlation of sediment temperature to both composition and quantity of porewater DOM was observed, driven by enhanced microbial transformation of organic matter at temperatures below ~60 °C and increasingly sulfurized DOM at high-temperature sites. DOM associated with hydrothermal heating had elevated contributions of highly unsaturated, reduced, sulfur-containing DOM and petroleum-associated PARAFAC components. A considerable DOM fraction of hydrothermal origin was present both in overlying bottom waters and in recalcitrant deep-sea DOM, suggesting hydrothermal sediments as a source of recalcitrant DOM to the water column. To assess elemental fluxes in DOM of hydrothermal porewaters, composition and quantities of DOM from sedimentary porewaters and from the hot-water soluble fraction by Soxhlet extraction of the same sediments were evaluated. Results showed highly elevated concentrations of DBC and potentially recalcitrant DOS in porewater, suggesting the release of both DOM fractions from hydrothermal sediments. DBC in porewaters and hot-water extracts originated from two distinct sources: hydrothermal petroleum and re-dissolved presumably terrestrial-derived, pre-aged DBC. This study further assessed quantities of DBC and dissolved organic nitrogen, sulfur and phosphorus that could be discharged into the water column in case of basin-wide hydrothermal heating. Results indicate that hydrothermal alteration and subsequent petroleum impregnation of sediments can be sources of recalcitrant DOS and DBC to deep sea environments. This thesis provides important novel information about the transformation and release of water-soluble petroleum compounds from natural deep-sea seepage into the marine environment. By introducing radiocarbon-depleted DOM to the marine environment, natural petroleum seepages and hydrothermal alteration of sediments with subsequent petroleum impregnation may be an explanation for observed old radiocarbon ages of recalcitrant DOM in the deep ocean. DE-46 Namensnennung 4.0 International CC BY 4.0 cc https://creativecommons.org/licenses/by/4.0/ Archivierung/Langzeitarchivierung gewährleistet PEHB XA-DE-HB pdager DE-46 deep sea dissolved organic matter (DOM) FT-ICR-MS oil seeps hydrothermal systems dissolved organic sulfur (DOS) black carbon Hochschulschrift (DE-588)4113937-9 (DE-627)105825778 (DE-576)209480580 gnd-content Schubotz, Florence 1981- akademischer betreuerin (DE-588)140326820 (DE-627)703639706 (DE-576)316433551 dgs Hinrichs, Kai-Uwe 1963- akademischer betreuerin (DE-588)115523677 (DE-627)077305647 (DE-576)289929768 dgs Kujawinski, Elizabeth akademischer betreuerin dgs Universität Bremen Grad-verleihende Institution (DE-588)2001386-3 (DE-627)101380429 (DE-576)191575038 dgg Bremen (DE-588)4008135-7 (DE-627)106369636 (DE-576)208874569 uvp https://doi.org/10.26092/elib/2185 Resolving-System kostenfrei https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 Resolving-System kostenfrei https://d-nb.info/1339390582/34 Langzeitarchivierung Nationalbibliothek kostenfrei https://media.suub.uni-bremen.de/handle/elib/6846 Verlag kostenfrei GBV-ODiss GBV_ILN_20 ISIL_DE-84 SYSFLAG_1 GBV_KXP GBV_ILN_21 ISIL_DE-46 GBV_ILN_22 ISIL_DE-18 GBV_ILN_23 ISIL_DE-830 GBV_ILN_30 ISIL_DE-104 GBV_ILN_40 ISIL_DE-7 GBV_ILN_60 ISIL_DE-705 GBV_ILN_63 ISIL_DE-Wim2 GBV_ILN_70 ISIL_DE-89 GBV_ILN_105 ISIL_DE-841 GBV_ILN_110 ISIL_DE-Luen4 GBV_ILN_132 ISIL_DE-959 GBV_ILN_151 ISIL_DE-546 GBV_ILN_161 ISIL_DE-960 GBV_ILN_293 ISIL_DE-960-3 GBV_ILN_370 ISIL_DE-1373 GBV_ILN_2403 ISIL_DE-LFER DSpace BO 20 01 0084 4593080258 x 12-10-24 21 01 0046 4322819990 ebook_2023_dissbremen Kostenloser Zugriff zza 16-05-23 22 01 0018 4593182034 SUBolrd xu 12-10-24 23 01 0830 4593230802 olr-d x 12-10-24 30 01 0104 4593277590 z 12-10-24 40 01 0007 4593312353 xsn 12-10-24 60 01 0705 4593370590 OLRD z 12-10-24 63 01 3401 4593425107 ORD x 12-10-24 70 01 0089 4593478359 z 12-10-24 105 01 0841 459386917X z 12-10-24 110 01 3110 4593580730 x 12-10-24 132 01 0959 4593624347 OLR-DISS x 12-10-24 151 01 0546 4593666236 OLR-ODISS z 12-10-24 161 01 0960 4593689783 ORD z 12-10-24 293 01 3293 4593818494 ORD z 12-10-24 370 01 4370 4593854156 x 12-10-24 2403 01 DE-LFER 4339770167 00 --%%-- --%%-- n --%%-- l01 16-06-23 20 01 0084 https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 21 01 0046 https://doi.org/10.26092/elib/2185 LF 22 01 0018 https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 23 01 0830 https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 30 01 0104 https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 40 01 0007 https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 60 01 0705 https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 63 01 3401 E-Book https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 LF 70 01 0089 https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 105 01 0841 https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 110 01 3110 https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 132 01 0959 https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 151 01 0546 Volltext https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 161 01 0960 https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 293 01 3293 https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 370 01 4370 https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 2403 01 DE-LFER https://doi.org/10.26092/elib/2185 21 00 DE-46 00 Universität Bremen 21 00 DE-46 00 Fachbereich 05: Geowissenschaften (FB 05) 60 01 0705 10 ho 20 01 0084 OLRD 110 01 3110 OLRD 370 01 4370 OLRD 21 01 0046 ebook_2023_dissbremen 22 01 0018 SUBolrd 23 01 0830 olr-d 60 01 0705 OLRD 63 01 3401 ORD 132 01 0959 OLR-DISS 151 01 0546 OLR-ODISS 161 01 0960 ORD 293 01 3293 ORD 23 01 0830 2024-10-12 10:31:16 |
allfields_unstemmed |
urn:nbn:de:gbv:46-elib68460 urn 10.26092/elib/2185 doi (DE-627)1845521927 (DE-599)KXP1845521927 (OCoLC)1379165877 (OAEPFHB)elib/2185 DE-627 ger DE-627 rda eng XA-DE-HB 553.2 DE-101 550 DE-101 Brünjes, Jonas verfasserin (orcid)0000-0001-7759-2583 aut Petroleum-derived dissolved organic matter from natural seepage in deep sea environments vorgelegt von Jonas Brünjes Bremen 2023 1 Online-Ressource (146 Seiten) Illustrationen Text txt rdacontent Computermedien c rdamedia Online-Ressource cr rdacarrier Dissertation Universität Bremen 2023 DE-46 Open Access Controlled Vocabulary for Access Rights http://purl.org/coar/access_right/c_abf2 Natural petroleum seepage discharges approximately 600,000 tons of oil every year into the marine environment. A fraction of the released petroleum is water-soluble and becomes part of oceanic dissolved organic matter (DOM), one of the largest and most complex pools of organic matter on Earth’s surface. Despite the constant discharge of petroleum by natural seepage, the environmental implications and persistence of petroleum-derived DOM are vastly unknown. This thesis investigates molecular transformations of DOM in natural petroleum seepages and assesses the potential release of petroleum-compounds to oceanic deep-sea DOM. In a first step, the release of oil-derived DOM from natural deep sea asphalt seeps was studied using controlled laboratory incubation experiments. Fresh asphalt samples collected at the Chapopote asphalt volcano in the Southern Gulf of Mexico were incubated aerobically in artificial seawater over four weeks. The compositional changes in the water-soluble fraction of asphalt-derived DOM were determined with ultrahigh-resolution mass spectrometry (Fourier-transform ion cyclotron resonance mass spectrometry, FT-ICR-MS) and by excitation-emission matrix spectroscopy to characterize fluorescent DOM (FDOM) applying parallel factor (PARAFAC) analysis. Result showed that highly reduced aliphatic asphalt-derived DOM was readily biodegraded, while aromatic and sulfur-containing DOM (DOS) appeared to be less bioavailable and accumulated in the aqueous phase. This indicates that natural asphalt and potentially other petroleum seepages can be marine sources of recalcitrant dissolved black carbon (DBC) which has apparent radiocarbon ages older than 20,000 years in the deep sea. In order to evaluate this laboratory finding in the natural environment, petroleum-derived DOM was investigated in the Guaymas Basin. The Guaymas Basin in the Gulf of California is a young rift system where hot basaltic sill intrusions into organic-rich sediments lead to the generation of large amounts of complex petroleum compounds. The effect of hydrothermal heating and the resulting presence of petroleum compounds on the porewater DOM composition were investigated. Sediment samples were retrieved from sites with in situ temperatures ranging from 4 to >106 °C that exhibited a strong petroleum smell and partially contained oil droplets. A strong correlation of sediment temperature to both composition and quantity of porewater DOM was observed, driven by enhanced microbial transformation of organic matter at temperatures below ~60 °C and increasingly sulfurized DOM at high-temperature sites. DOM associated with hydrothermal heating had elevated contributions of highly unsaturated, reduced, sulfur-containing DOM and petroleum-associated PARAFAC components. A considerable DOM fraction of hydrothermal origin was present both in overlying bottom waters and in recalcitrant deep-sea DOM, suggesting hydrothermal sediments as a source of recalcitrant DOM to the water column. To assess elemental fluxes in DOM of hydrothermal porewaters, composition and quantities of DOM from sedimentary porewaters and from the hot-water soluble fraction by Soxhlet extraction of the same sediments were evaluated. Results showed highly elevated concentrations of DBC and potentially recalcitrant DOS in porewater, suggesting the release of both DOM fractions from hydrothermal sediments. DBC in porewaters and hot-water extracts originated from two distinct sources: hydrothermal petroleum and re-dissolved presumably terrestrial-derived, pre-aged DBC. This study further assessed quantities of DBC and dissolved organic nitrogen, sulfur and phosphorus that could be discharged into the water column in case of basin-wide hydrothermal heating. Results indicate that hydrothermal alteration and subsequent petroleum impregnation of sediments can be sources of recalcitrant DOS and DBC to deep sea environments. This thesis provides important novel information about the transformation and release of water-soluble petroleum compounds from natural deep-sea seepage into the marine environment. By introducing radiocarbon-depleted DOM to the marine environment, natural petroleum seepages and hydrothermal alteration of sediments with subsequent petroleum impregnation may be an explanation for observed old radiocarbon ages of recalcitrant DOM in the deep ocean. DE-46 Namensnennung 4.0 International CC BY 4.0 cc https://creativecommons.org/licenses/by/4.0/ Archivierung/Langzeitarchivierung gewährleistet PEHB XA-DE-HB pdager DE-46 deep sea dissolved organic matter (DOM) FT-ICR-MS oil seeps hydrothermal systems dissolved organic sulfur (DOS) black carbon Hochschulschrift (DE-588)4113937-9 (DE-627)105825778 (DE-576)209480580 gnd-content Schubotz, Florence 1981- akademischer betreuerin (DE-588)140326820 (DE-627)703639706 (DE-576)316433551 dgs Hinrichs, Kai-Uwe 1963- akademischer betreuerin (DE-588)115523677 (DE-627)077305647 (DE-576)289929768 dgs Kujawinski, Elizabeth akademischer betreuerin dgs Universität Bremen Grad-verleihende Institution (DE-588)2001386-3 (DE-627)101380429 (DE-576)191575038 dgg Bremen (DE-588)4008135-7 (DE-627)106369636 (DE-576)208874569 uvp https://doi.org/10.26092/elib/2185 Resolving-System kostenfrei https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 Resolving-System kostenfrei https://d-nb.info/1339390582/34 Langzeitarchivierung Nationalbibliothek kostenfrei https://media.suub.uni-bremen.de/handle/elib/6846 Verlag kostenfrei GBV-ODiss GBV_ILN_20 ISIL_DE-84 SYSFLAG_1 GBV_KXP GBV_ILN_21 ISIL_DE-46 GBV_ILN_22 ISIL_DE-18 GBV_ILN_23 ISIL_DE-830 GBV_ILN_30 ISIL_DE-104 GBV_ILN_40 ISIL_DE-7 GBV_ILN_60 ISIL_DE-705 GBV_ILN_63 ISIL_DE-Wim2 GBV_ILN_70 ISIL_DE-89 GBV_ILN_105 ISIL_DE-841 GBV_ILN_110 ISIL_DE-Luen4 GBV_ILN_132 ISIL_DE-959 GBV_ILN_151 ISIL_DE-546 GBV_ILN_161 ISIL_DE-960 GBV_ILN_293 ISIL_DE-960-3 GBV_ILN_370 ISIL_DE-1373 GBV_ILN_2403 ISIL_DE-LFER DSpace BO 20 01 0084 4593080258 x 12-10-24 21 01 0046 4322819990 ebook_2023_dissbremen Kostenloser Zugriff zza 16-05-23 22 01 0018 4593182034 SUBolrd xu 12-10-24 23 01 0830 4593230802 olr-d x 12-10-24 30 01 0104 4593277590 z 12-10-24 40 01 0007 4593312353 xsn 12-10-24 60 01 0705 4593370590 OLRD z 12-10-24 63 01 3401 4593425107 ORD x 12-10-24 70 01 0089 4593478359 z 12-10-24 105 01 0841 459386917X z 12-10-24 110 01 3110 4593580730 x 12-10-24 132 01 0959 4593624347 OLR-DISS x 12-10-24 151 01 0546 4593666236 OLR-ODISS z 12-10-24 161 01 0960 4593689783 ORD z 12-10-24 293 01 3293 4593818494 ORD z 12-10-24 370 01 4370 4593854156 x 12-10-24 2403 01 DE-LFER 4339770167 00 --%%-- --%%-- n --%%-- l01 16-06-23 20 01 0084 https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 21 01 0046 https://doi.org/10.26092/elib/2185 LF 22 01 0018 https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 23 01 0830 https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 30 01 0104 https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 40 01 0007 https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 60 01 0705 https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 63 01 3401 E-Book https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 LF 70 01 0089 https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 105 01 0841 https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 110 01 3110 https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 132 01 0959 https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 151 01 0546 Volltext https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 161 01 0960 https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 293 01 3293 https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 370 01 4370 https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 2403 01 DE-LFER https://doi.org/10.26092/elib/2185 21 00 DE-46 00 Universität Bremen 21 00 DE-46 00 Fachbereich 05: Geowissenschaften (FB 05) 60 01 0705 10 ho 20 01 0084 OLRD 110 01 3110 OLRD 370 01 4370 OLRD 21 01 0046 ebook_2023_dissbremen 22 01 0018 SUBolrd 23 01 0830 olr-d 60 01 0705 OLRD 63 01 3401 ORD 132 01 0959 OLR-DISS 151 01 0546 OLR-ODISS 161 01 0960 ORD 293 01 3293 ORD 23 01 0830 2024-10-12 10:31:16 |
allfieldsGer |
urn:nbn:de:gbv:46-elib68460 urn 10.26092/elib/2185 doi (DE-627)1845521927 (DE-599)KXP1845521927 (OCoLC)1379165877 (OAEPFHB)elib/2185 DE-627 ger DE-627 rda eng XA-DE-HB 553.2 DE-101 550 DE-101 Brünjes, Jonas verfasserin (orcid)0000-0001-7759-2583 aut Petroleum-derived dissolved organic matter from natural seepage in deep sea environments vorgelegt von Jonas Brünjes Bremen 2023 1 Online-Ressource (146 Seiten) Illustrationen Text txt rdacontent Computermedien c rdamedia Online-Ressource cr rdacarrier Dissertation Universität Bremen 2023 DE-46 Open Access Controlled Vocabulary for Access Rights http://purl.org/coar/access_right/c_abf2 Natural petroleum seepage discharges approximately 600,000 tons of oil every year into the marine environment. A fraction of the released petroleum is water-soluble and becomes part of oceanic dissolved organic matter (DOM), one of the largest and most complex pools of organic matter on Earth’s surface. Despite the constant discharge of petroleum by natural seepage, the environmental implications and persistence of petroleum-derived DOM are vastly unknown. This thesis investigates molecular transformations of DOM in natural petroleum seepages and assesses the potential release of petroleum-compounds to oceanic deep-sea DOM. In a first step, the release of oil-derived DOM from natural deep sea asphalt seeps was studied using controlled laboratory incubation experiments. Fresh asphalt samples collected at the Chapopote asphalt volcano in the Southern Gulf of Mexico were incubated aerobically in artificial seawater over four weeks. The compositional changes in the water-soluble fraction of asphalt-derived DOM were determined with ultrahigh-resolution mass spectrometry (Fourier-transform ion cyclotron resonance mass spectrometry, FT-ICR-MS) and by excitation-emission matrix spectroscopy to characterize fluorescent DOM (FDOM) applying parallel factor (PARAFAC) analysis. Result showed that highly reduced aliphatic asphalt-derived DOM was readily biodegraded, while aromatic and sulfur-containing DOM (DOS) appeared to be less bioavailable and accumulated in the aqueous phase. This indicates that natural asphalt and potentially other petroleum seepages can be marine sources of recalcitrant dissolved black carbon (DBC) which has apparent radiocarbon ages older than 20,000 years in the deep sea. In order to evaluate this laboratory finding in the natural environment, petroleum-derived DOM was investigated in the Guaymas Basin. The Guaymas Basin in the Gulf of California is a young rift system where hot basaltic sill intrusions into organic-rich sediments lead to the generation of large amounts of complex petroleum compounds. The effect of hydrothermal heating and the resulting presence of petroleum compounds on the porewater DOM composition were investigated. Sediment samples were retrieved from sites with in situ temperatures ranging from 4 to >106 °C that exhibited a strong petroleum smell and partially contained oil droplets. A strong correlation of sediment temperature to both composition and quantity of porewater DOM was observed, driven by enhanced microbial transformation of organic matter at temperatures below ~60 °C and increasingly sulfurized DOM at high-temperature sites. DOM associated with hydrothermal heating had elevated contributions of highly unsaturated, reduced, sulfur-containing DOM and petroleum-associated PARAFAC components. A considerable DOM fraction of hydrothermal origin was present both in overlying bottom waters and in recalcitrant deep-sea DOM, suggesting hydrothermal sediments as a source of recalcitrant DOM to the water column. To assess elemental fluxes in DOM of hydrothermal porewaters, composition and quantities of DOM from sedimentary porewaters and from the hot-water soluble fraction by Soxhlet extraction of the same sediments were evaluated. Results showed highly elevated concentrations of DBC and potentially recalcitrant DOS in porewater, suggesting the release of both DOM fractions from hydrothermal sediments. DBC in porewaters and hot-water extracts originated from two distinct sources: hydrothermal petroleum and re-dissolved presumably terrestrial-derived, pre-aged DBC. This study further assessed quantities of DBC and dissolved organic nitrogen, sulfur and phosphorus that could be discharged into the water column in case of basin-wide hydrothermal heating. Results indicate that hydrothermal alteration and subsequent petroleum impregnation of sediments can be sources of recalcitrant DOS and DBC to deep sea environments. This thesis provides important novel information about the transformation and release of water-soluble petroleum compounds from natural deep-sea seepage into the marine environment. By introducing radiocarbon-depleted DOM to the marine environment, natural petroleum seepages and hydrothermal alteration of sediments with subsequent petroleum impregnation may be an explanation for observed old radiocarbon ages of recalcitrant DOM in the deep ocean. DE-46 Namensnennung 4.0 International CC BY 4.0 cc https://creativecommons.org/licenses/by/4.0/ Archivierung/Langzeitarchivierung gewährleistet PEHB XA-DE-HB pdager DE-46 deep sea dissolved organic matter (DOM) FT-ICR-MS oil seeps hydrothermal systems dissolved organic sulfur (DOS) black carbon Hochschulschrift (DE-588)4113937-9 (DE-627)105825778 (DE-576)209480580 gnd-content Schubotz, Florence 1981- akademischer betreuerin (DE-588)140326820 (DE-627)703639706 (DE-576)316433551 dgs Hinrichs, Kai-Uwe 1963- akademischer betreuerin (DE-588)115523677 (DE-627)077305647 (DE-576)289929768 dgs Kujawinski, Elizabeth akademischer betreuerin dgs Universität Bremen Grad-verleihende Institution (DE-588)2001386-3 (DE-627)101380429 (DE-576)191575038 dgg Bremen (DE-588)4008135-7 (DE-627)106369636 (DE-576)208874569 uvp https://doi.org/10.26092/elib/2185 Resolving-System kostenfrei https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 Resolving-System kostenfrei https://d-nb.info/1339390582/34 Langzeitarchivierung Nationalbibliothek kostenfrei https://media.suub.uni-bremen.de/handle/elib/6846 Verlag kostenfrei GBV-ODiss GBV_ILN_20 ISIL_DE-84 SYSFLAG_1 GBV_KXP GBV_ILN_21 ISIL_DE-46 GBV_ILN_22 ISIL_DE-18 GBV_ILN_23 ISIL_DE-830 GBV_ILN_30 ISIL_DE-104 GBV_ILN_40 ISIL_DE-7 GBV_ILN_60 ISIL_DE-705 GBV_ILN_63 ISIL_DE-Wim2 GBV_ILN_70 ISIL_DE-89 GBV_ILN_105 ISIL_DE-841 GBV_ILN_110 ISIL_DE-Luen4 GBV_ILN_132 ISIL_DE-959 GBV_ILN_151 ISIL_DE-546 GBV_ILN_161 ISIL_DE-960 GBV_ILN_293 ISIL_DE-960-3 GBV_ILN_370 ISIL_DE-1373 GBV_ILN_2403 ISIL_DE-LFER DSpace BO 20 01 0084 4593080258 x 12-10-24 21 01 0046 4322819990 ebook_2023_dissbremen Kostenloser Zugriff zza 16-05-23 22 01 0018 4593182034 SUBolrd xu 12-10-24 23 01 0830 4593230802 olr-d x 12-10-24 30 01 0104 4593277590 z 12-10-24 40 01 0007 4593312353 xsn 12-10-24 60 01 0705 4593370590 OLRD z 12-10-24 63 01 3401 4593425107 ORD x 12-10-24 70 01 0089 4593478359 z 12-10-24 105 01 0841 459386917X z 12-10-24 110 01 3110 4593580730 x 12-10-24 132 01 0959 4593624347 OLR-DISS x 12-10-24 151 01 0546 4593666236 OLR-ODISS z 12-10-24 161 01 0960 4593689783 ORD z 12-10-24 293 01 3293 4593818494 ORD z 12-10-24 370 01 4370 4593854156 x 12-10-24 2403 01 DE-LFER 4339770167 00 --%%-- --%%-- n --%%-- l01 16-06-23 20 01 0084 https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 21 01 0046 https://doi.org/10.26092/elib/2185 LF 22 01 0018 https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 23 01 0830 https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 30 01 0104 https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 40 01 0007 https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 60 01 0705 https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 63 01 3401 E-Book https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 LF 70 01 0089 https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 105 01 0841 https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 110 01 3110 https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 132 01 0959 https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 151 01 0546 Volltext https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 161 01 0960 https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 293 01 3293 https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 370 01 4370 https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 2403 01 DE-LFER https://doi.org/10.26092/elib/2185 21 00 DE-46 00 Universität Bremen 21 00 DE-46 00 Fachbereich 05: Geowissenschaften (FB 05) 60 01 0705 10 ho 20 01 0084 OLRD 110 01 3110 OLRD 370 01 4370 OLRD 21 01 0046 ebook_2023_dissbremen 22 01 0018 SUBolrd 23 01 0830 olr-d 60 01 0705 OLRD 63 01 3401 ORD 132 01 0959 OLR-DISS 151 01 0546 OLR-ODISS 161 01 0960 ORD 293 01 3293 ORD 23 01 0830 2024-10-12 10:31:16 |
allfieldsSound |
urn:nbn:de:gbv:46-elib68460 urn 10.26092/elib/2185 doi (DE-627)1845521927 (DE-599)KXP1845521927 (OCoLC)1379165877 (OAEPFHB)elib/2185 DE-627 ger DE-627 rda eng XA-DE-HB 553.2 DE-101 550 DE-101 Brünjes, Jonas verfasserin (orcid)0000-0001-7759-2583 aut Petroleum-derived dissolved organic matter from natural seepage in deep sea environments vorgelegt von Jonas Brünjes Bremen 2023 1 Online-Ressource (146 Seiten) Illustrationen Text txt rdacontent Computermedien c rdamedia Online-Ressource cr rdacarrier Dissertation Universität Bremen 2023 DE-46 Open Access Controlled Vocabulary for Access Rights http://purl.org/coar/access_right/c_abf2 Natural petroleum seepage discharges approximately 600,000 tons of oil every year into the marine environment. A fraction of the released petroleum is water-soluble and becomes part of oceanic dissolved organic matter (DOM), one of the largest and most complex pools of organic matter on Earth’s surface. Despite the constant discharge of petroleum by natural seepage, the environmental implications and persistence of petroleum-derived DOM are vastly unknown. This thesis investigates molecular transformations of DOM in natural petroleum seepages and assesses the potential release of petroleum-compounds to oceanic deep-sea DOM. In a first step, the release of oil-derived DOM from natural deep sea asphalt seeps was studied using controlled laboratory incubation experiments. Fresh asphalt samples collected at the Chapopote asphalt volcano in the Southern Gulf of Mexico were incubated aerobically in artificial seawater over four weeks. The compositional changes in the water-soluble fraction of asphalt-derived DOM were determined with ultrahigh-resolution mass spectrometry (Fourier-transform ion cyclotron resonance mass spectrometry, FT-ICR-MS) and by excitation-emission matrix spectroscopy to characterize fluorescent DOM (FDOM) applying parallel factor (PARAFAC) analysis. Result showed that highly reduced aliphatic asphalt-derived DOM was readily biodegraded, while aromatic and sulfur-containing DOM (DOS) appeared to be less bioavailable and accumulated in the aqueous phase. This indicates that natural asphalt and potentially other petroleum seepages can be marine sources of recalcitrant dissolved black carbon (DBC) which has apparent radiocarbon ages older than 20,000 years in the deep sea. In order to evaluate this laboratory finding in the natural environment, petroleum-derived DOM was investigated in the Guaymas Basin. The Guaymas Basin in the Gulf of California is a young rift system where hot basaltic sill intrusions into organic-rich sediments lead to the generation of large amounts of complex petroleum compounds. The effect of hydrothermal heating and the resulting presence of petroleum compounds on the porewater DOM composition were investigated. Sediment samples were retrieved from sites with in situ temperatures ranging from 4 to >106 °C that exhibited a strong petroleum smell and partially contained oil droplets. A strong correlation of sediment temperature to both composition and quantity of porewater DOM was observed, driven by enhanced microbial transformation of organic matter at temperatures below ~60 °C and increasingly sulfurized DOM at high-temperature sites. DOM associated with hydrothermal heating had elevated contributions of highly unsaturated, reduced, sulfur-containing DOM and petroleum-associated PARAFAC components. A considerable DOM fraction of hydrothermal origin was present both in overlying bottom waters and in recalcitrant deep-sea DOM, suggesting hydrothermal sediments as a source of recalcitrant DOM to the water column. To assess elemental fluxes in DOM of hydrothermal porewaters, composition and quantities of DOM from sedimentary porewaters and from the hot-water soluble fraction by Soxhlet extraction of the same sediments were evaluated. Results showed highly elevated concentrations of DBC and potentially recalcitrant DOS in porewater, suggesting the release of both DOM fractions from hydrothermal sediments. DBC in porewaters and hot-water extracts originated from two distinct sources: hydrothermal petroleum and re-dissolved presumably terrestrial-derived, pre-aged DBC. This study further assessed quantities of DBC and dissolved organic nitrogen, sulfur and phosphorus that could be discharged into the water column in case of basin-wide hydrothermal heating. Results indicate that hydrothermal alteration and subsequent petroleum impregnation of sediments can be sources of recalcitrant DOS and DBC to deep sea environments. This thesis provides important novel information about the transformation and release of water-soluble petroleum compounds from natural deep-sea seepage into the marine environment. By introducing radiocarbon-depleted DOM to the marine environment, natural petroleum seepages and hydrothermal alteration of sediments with subsequent petroleum impregnation may be an explanation for observed old radiocarbon ages of recalcitrant DOM in the deep ocean. DE-46 Namensnennung 4.0 International CC BY 4.0 cc https://creativecommons.org/licenses/by/4.0/ Archivierung/Langzeitarchivierung gewährleistet PEHB XA-DE-HB pdager DE-46 deep sea dissolved organic matter (DOM) FT-ICR-MS oil seeps hydrothermal systems dissolved organic sulfur (DOS) black carbon Hochschulschrift (DE-588)4113937-9 (DE-627)105825778 (DE-576)209480580 gnd-content Schubotz, Florence 1981- akademischer betreuerin (DE-588)140326820 (DE-627)703639706 (DE-576)316433551 dgs Hinrichs, Kai-Uwe 1963- akademischer betreuerin (DE-588)115523677 (DE-627)077305647 (DE-576)289929768 dgs Kujawinski, Elizabeth akademischer betreuerin dgs Universität Bremen Grad-verleihende Institution (DE-588)2001386-3 (DE-627)101380429 (DE-576)191575038 dgg Bremen (DE-588)4008135-7 (DE-627)106369636 (DE-576)208874569 uvp https://doi.org/10.26092/elib/2185 Resolving-System kostenfrei https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 Resolving-System kostenfrei https://d-nb.info/1339390582/34 Langzeitarchivierung Nationalbibliothek kostenfrei https://media.suub.uni-bremen.de/handle/elib/6846 Verlag kostenfrei GBV-ODiss GBV_ILN_20 ISIL_DE-84 SYSFLAG_1 GBV_KXP GBV_ILN_21 ISIL_DE-46 GBV_ILN_22 ISIL_DE-18 GBV_ILN_23 ISIL_DE-830 GBV_ILN_30 ISIL_DE-104 GBV_ILN_40 ISIL_DE-7 GBV_ILN_60 ISIL_DE-705 GBV_ILN_63 ISIL_DE-Wim2 GBV_ILN_70 ISIL_DE-89 GBV_ILN_105 ISIL_DE-841 GBV_ILN_110 ISIL_DE-Luen4 GBV_ILN_132 ISIL_DE-959 GBV_ILN_151 ISIL_DE-546 GBV_ILN_161 ISIL_DE-960 GBV_ILN_293 ISIL_DE-960-3 GBV_ILN_370 ISIL_DE-1373 GBV_ILN_2403 ISIL_DE-LFER DSpace BO 20 01 0084 4593080258 x 12-10-24 21 01 0046 4322819990 ebook_2023_dissbremen Kostenloser Zugriff zza 16-05-23 22 01 0018 4593182034 SUBolrd xu 12-10-24 23 01 0830 4593230802 olr-d x 12-10-24 30 01 0104 4593277590 z 12-10-24 40 01 0007 4593312353 xsn 12-10-24 60 01 0705 4593370590 OLRD z 12-10-24 63 01 3401 4593425107 ORD x 12-10-24 70 01 0089 4593478359 z 12-10-24 105 01 0841 459386917X z 12-10-24 110 01 3110 4593580730 x 12-10-24 132 01 0959 4593624347 OLR-DISS x 12-10-24 151 01 0546 4593666236 OLR-ODISS z 12-10-24 161 01 0960 4593689783 ORD z 12-10-24 293 01 3293 4593818494 ORD z 12-10-24 370 01 4370 4593854156 x 12-10-24 2403 01 DE-LFER 4339770167 00 --%%-- --%%-- n --%%-- l01 16-06-23 20 01 0084 https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 21 01 0046 https://doi.org/10.26092/elib/2185 LF 22 01 0018 https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 23 01 0830 https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 30 01 0104 https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 40 01 0007 https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 60 01 0705 https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 63 01 3401 E-Book https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 LF 70 01 0089 https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 105 01 0841 https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 110 01 3110 https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 132 01 0959 https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 151 01 0546 Volltext https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 161 01 0960 https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 293 01 3293 https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 370 01 4370 https://nbn-resolving.org/urn:nbn:de:gbv:46-elib68460 2403 01 DE-LFER https://doi.org/10.26092/elib/2185 21 00 DE-46 00 Universität Bremen 21 00 DE-46 00 Fachbereich 05: Geowissenschaften (FB 05) 60 01 0705 10 ho 20 01 0084 OLRD 110 01 3110 OLRD 370 01 4370 OLRD 21 01 0046 ebook_2023_dissbremen 22 01 0018 SUBolrd 23 01 0830 olr-d 60 01 0705 OLRD 63 01 3401 ORD 132 01 0959 OLR-DISS 151 01 0546 OLR-ODISS 161 01 0960 ORD 293 01 3293 ORD 23 01 0830 2024-10-12 10:31:16 |
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petroleum-derived dissolved organic matter from natural seepage in deep sea environments |
title_auth |
Petroleum-derived dissolved organic matter from natural seepage in deep sea environments |
abstract |
Natural petroleum seepage discharges approximately 600,000 tons of oil every year into the marine environment. A fraction of the released petroleum is water-soluble and becomes part of oceanic dissolved organic matter (DOM), one of the largest and most complex pools of organic matter on Earth’s surface. Despite the constant discharge of petroleum by natural seepage, the environmental implications and persistence of petroleum-derived DOM are vastly unknown. This thesis investigates molecular transformations of DOM in natural petroleum seepages and assesses the potential release of petroleum-compounds to oceanic deep-sea DOM. In a first step, the release of oil-derived DOM from natural deep sea asphalt seeps was studied using controlled laboratory incubation experiments. Fresh asphalt samples collected at the Chapopote asphalt volcano in the Southern Gulf of Mexico were incubated aerobically in artificial seawater over four weeks. The compositional changes in the water-soluble fraction of asphalt-derived DOM were determined with ultrahigh-resolution mass spectrometry (Fourier-transform ion cyclotron resonance mass spectrometry, FT-ICR-MS) and by excitation-emission matrix spectroscopy to characterize fluorescent DOM (FDOM) applying parallel factor (PARAFAC) analysis. Result showed that highly reduced aliphatic asphalt-derived DOM was readily biodegraded, while aromatic and sulfur-containing DOM (DOS) appeared to be less bioavailable and accumulated in the aqueous phase. This indicates that natural asphalt and potentially other petroleum seepages can be marine sources of recalcitrant dissolved black carbon (DBC) which has apparent radiocarbon ages older than 20,000 years in the deep sea. In order to evaluate this laboratory finding in the natural environment, petroleum-derived DOM was investigated in the Guaymas Basin. The Guaymas Basin in the Gulf of California is a young rift system where hot basaltic sill intrusions into organic-rich sediments lead to the generation of large amounts of complex petroleum compounds. The effect of hydrothermal heating and the resulting presence of petroleum compounds on the porewater DOM composition were investigated. Sediment samples were retrieved from sites with in situ temperatures ranging from 4 to >106 °C that exhibited a strong petroleum smell and partially contained oil droplets. A strong correlation of sediment temperature to both composition and quantity of porewater DOM was observed, driven by enhanced microbial transformation of organic matter at temperatures below ~60 °C and increasingly sulfurized DOM at high-temperature sites. DOM associated with hydrothermal heating had elevated contributions of highly unsaturated, reduced, sulfur-containing DOM and petroleum-associated PARAFAC components. A considerable DOM fraction of hydrothermal origin was present both in overlying bottom waters and in recalcitrant deep-sea DOM, suggesting hydrothermal sediments as a source of recalcitrant DOM to the water column. To assess elemental fluxes in DOM of hydrothermal porewaters, composition and quantities of DOM from sedimentary porewaters and from the hot-water soluble fraction by Soxhlet extraction of the same sediments were evaluated. Results showed highly elevated concentrations of DBC and potentially recalcitrant DOS in porewater, suggesting the release of both DOM fractions from hydrothermal sediments. DBC in porewaters and hot-water extracts originated from two distinct sources: hydrothermal petroleum and re-dissolved presumably terrestrial-derived, pre-aged DBC. This study further assessed quantities of DBC and dissolved organic nitrogen, sulfur and phosphorus that could be discharged into the water column in case of basin-wide hydrothermal heating. Results indicate that hydrothermal alteration and subsequent petroleum impregnation of sediments can be sources of recalcitrant DOS and DBC to deep sea environments. This thesis provides important novel information about the transformation and release of water-soluble petroleum compounds from natural deep-sea seepage into the marine environment. By introducing radiocarbon-depleted DOM to the marine environment, natural petroleum seepages and hydrothermal alteration of sediments with subsequent petroleum impregnation may be an explanation for observed old radiocarbon ages of recalcitrant DOM in the deep ocean. |
abstractGer |
Natural petroleum seepage discharges approximately 600,000 tons of oil every year into the marine environment. A fraction of the released petroleum is water-soluble and becomes part of oceanic dissolved organic matter (DOM), one of the largest and most complex pools of organic matter on Earth’s surface. Despite the constant discharge of petroleum by natural seepage, the environmental implications and persistence of petroleum-derived DOM are vastly unknown. This thesis investigates molecular transformations of DOM in natural petroleum seepages and assesses the potential release of petroleum-compounds to oceanic deep-sea DOM. In a first step, the release of oil-derived DOM from natural deep sea asphalt seeps was studied using controlled laboratory incubation experiments. Fresh asphalt samples collected at the Chapopote asphalt volcano in the Southern Gulf of Mexico were incubated aerobically in artificial seawater over four weeks. The compositional changes in the water-soluble fraction of asphalt-derived DOM were determined with ultrahigh-resolution mass spectrometry (Fourier-transform ion cyclotron resonance mass spectrometry, FT-ICR-MS) and by excitation-emission matrix spectroscopy to characterize fluorescent DOM (FDOM) applying parallel factor (PARAFAC) analysis. Result showed that highly reduced aliphatic asphalt-derived DOM was readily biodegraded, while aromatic and sulfur-containing DOM (DOS) appeared to be less bioavailable and accumulated in the aqueous phase. This indicates that natural asphalt and potentially other petroleum seepages can be marine sources of recalcitrant dissolved black carbon (DBC) which has apparent radiocarbon ages older than 20,000 years in the deep sea. In order to evaluate this laboratory finding in the natural environment, petroleum-derived DOM was investigated in the Guaymas Basin. The Guaymas Basin in the Gulf of California is a young rift system where hot basaltic sill intrusions into organic-rich sediments lead to the generation of large amounts of complex petroleum compounds. The effect of hydrothermal heating and the resulting presence of petroleum compounds on the porewater DOM composition were investigated. Sediment samples were retrieved from sites with in situ temperatures ranging from 4 to >106 °C that exhibited a strong petroleum smell and partially contained oil droplets. A strong correlation of sediment temperature to both composition and quantity of porewater DOM was observed, driven by enhanced microbial transformation of organic matter at temperatures below ~60 °C and increasingly sulfurized DOM at high-temperature sites. DOM associated with hydrothermal heating had elevated contributions of highly unsaturated, reduced, sulfur-containing DOM and petroleum-associated PARAFAC components. A considerable DOM fraction of hydrothermal origin was present both in overlying bottom waters and in recalcitrant deep-sea DOM, suggesting hydrothermal sediments as a source of recalcitrant DOM to the water column. To assess elemental fluxes in DOM of hydrothermal porewaters, composition and quantities of DOM from sedimentary porewaters and from the hot-water soluble fraction by Soxhlet extraction of the same sediments were evaluated. Results showed highly elevated concentrations of DBC and potentially recalcitrant DOS in porewater, suggesting the release of both DOM fractions from hydrothermal sediments. DBC in porewaters and hot-water extracts originated from two distinct sources: hydrothermal petroleum and re-dissolved presumably terrestrial-derived, pre-aged DBC. This study further assessed quantities of DBC and dissolved organic nitrogen, sulfur and phosphorus that could be discharged into the water column in case of basin-wide hydrothermal heating. Results indicate that hydrothermal alteration and subsequent petroleum impregnation of sediments can be sources of recalcitrant DOS and DBC to deep sea environments. This thesis provides important novel information about the transformation and release of water-soluble petroleum compounds from natural deep-sea seepage into the marine environment. By introducing radiocarbon-depleted DOM to the marine environment, natural petroleum seepages and hydrothermal alteration of sediments with subsequent petroleum impregnation may be an explanation for observed old radiocarbon ages of recalcitrant DOM in the deep ocean. |
abstract_unstemmed |
Natural petroleum seepage discharges approximately 600,000 tons of oil every year into the marine environment. A fraction of the released petroleum is water-soluble and becomes part of oceanic dissolved organic matter (DOM), one of the largest and most complex pools of organic matter on Earth’s surface. Despite the constant discharge of petroleum by natural seepage, the environmental implications and persistence of petroleum-derived DOM are vastly unknown. This thesis investigates molecular transformations of DOM in natural petroleum seepages and assesses the potential release of petroleum-compounds to oceanic deep-sea DOM. In a first step, the release of oil-derived DOM from natural deep sea asphalt seeps was studied using controlled laboratory incubation experiments. Fresh asphalt samples collected at the Chapopote asphalt volcano in the Southern Gulf of Mexico were incubated aerobically in artificial seawater over four weeks. The compositional changes in the water-soluble fraction of asphalt-derived DOM were determined with ultrahigh-resolution mass spectrometry (Fourier-transform ion cyclotron resonance mass spectrometry, FT-ICR-MS) and by excitation-emission matrix spectroscopy to characterize fluorescent DOM (FDOM) applying parallel factor (PARAFAC) analysis. Result showed that highly reduced aliphatic asphalt-derived DOM was readily biodegraded, while aromatic and sulfur-containing DOM (DOS) appeared to be less bioavailable and accumulated in the aqueous phase. This indicates that natural asphalt and potentially other petroleum seepages can be marine sources of recalcitrant dissolved black carbon (DBC) which has apparent radiocarbon ages older than 20,000 years in the deep sea. In order to evaluate this laboratory finding in the natural environment, petroleum-derived DOM was investigated in the Guaymas Basin. The Guaymas Basin in the Gulf of California is a young rift system where hot basaltic sill intrusions into organic-rich sediments lead to the generation of large amounts of complex petroleum compounds. The effect of hydrothermal heating and the resulting presence of petroleum compounds on the porewater DOM composition were investigated. Sediment samples were retrieved from sites with in situ temperatures ranging from 4 to >106 °C that exhibited a strong petroleum smell and partially contained oil droplets. A strong correlation of sediment temperature to both composition and quantity of porewater DOM was observed, driven by enhanced microbial transformation of organic matter at temperatures below ~60 °C and increasingly sulfurized DOM at high-temperature sites. DOM associated with hydrothermal heating had elevated contributions of highly unsaturated, reduced, sulfur-containing DOM and petroleum-associated PARAFAC components. A considerable DOM fraction of hydrothermal origin was present both in overlying bottom waters and in recalcitrant deep-sea DOM, suggesting hydrothermal sediments as a source of recalcitrant DOM to the water column. To assess elemental fluxes in DOM of hydrothermal porewaters, composition and quantities of DOM from sedimentary porewaters and from the hot-water soluble fraction by Soxhlet extraction of the same sediments were evaluated. Results showed highly elevated concentrations of DBC and potentially recalcitrant DOS in porewater, suggesting the release of both DOM fractions from hydrothermal sediments. DBC in porewaters and hot-water extracts originated from two distinct sources: hydrothermal petroleum and re-dissolved presumably terrestrial-derived, pre-aged DBC. This study further assessed quantities of DBC and dissolved organic nitrogen, sulfur and phosphorus that could be discharged into the water column in case of basin-wide hydrothermal heating. Results indicate that hydrothermal alteration and subsequent petroleum impregnation of sediments can be sources of recalcitrant DOS and DBC to deep sea environments. This thesis provides important novel information about the transformation and release of water-soluble petroleum compounds from natural deep-sea seepage into the marine environment. By introducing radiocarbon-depleted DOM to the marine environment, natural petroleum seepages and hydrothermal alteration of sediments with subsequent petroleum impregnation may be an explanation for observed old radiocarbon ages of recalcitrant DOM in the deep ocean. |
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title_short |
Petroleum-derived dissolved organic matter from natural seepage in deep sea environments |
url |
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