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Abstract: Hydrate Ridge off the coast of Oregon, USA, is a prime example for gas hydrate occurrences in active margin settings. It is part of the Cascadia Margin and was the focus of Ocean Drilling Program (ODP) Leg 204, which successfully recovered fluids from nine sites from the southern part of the ridge. Iodide concentrations in pore fluids associated with gas hydrates are strongly enhanced, by factors up to 5000 compared to seawater, which allows the use of this biophilic element as tracer for organic source regions. We applied the cosmogenic isotope 129I (T 1/2 =15.7 Ma) system to determine the age of the organic source formation responsible for the iodide enrichment. In all sites at ODP Leg 204, 129I/I ratios were found to decrease with depth to values around 250×10−15, corresponding to minimum ages of 40 Ma, but in several sites, maxima in the 129I/I ratios point to the local addition of young iodide. The results indicate that a large amount of iodide was derived from deep accreted sediments of Eocene age, and that additional source regions provide iodide of Late Miocene age. The presence of old iodide in the pore waters suggests that fluid pathways are open to allow transport over large distances into the gas hydrate fields. The strong correlation between iodide and methane in hydrate fields coupled with the similarity in transport parameters in aqueous solutions suggests that a large fraction of methane in gas hydrates also has old sources and is transported into the present locations from source regions of Eocene age. [Copyright &y& Elsevier]

Abstract: A gas hydrate field with highly active venting of methane was recently found near Sado Island in the eastern Japan Sea. Piston cores were collected from active venting sites and nearby locations in the Umitaka Spur–Joetsu Knoll area during two cruises in 2004 (UT04) and 2005 (KY05-08). We report here halogen concentrations and 129I/I ratios in pore waters associated with gas hydrates from these expeditions. The strongly biophilic behavior of I and, to a lesser degree, of Br together with the presence of the long-lived iodine radioisotope (129I) allow evaluation of potential source materials for methane in gas hydrate systems. Depth profiles of all three halogens, particularly the very rapid downward increases of Br and I concentrations, strongly suggest input of deep fluids enriched in Br and I, but the profiles also display the effects of gas hydrate formation and dissociation. Although the 129I/I ratios are modified by 129I from seawater and sediments at shallow depth, likely ratios of the deep fluids are estimated to be between 400×10−15 and 600×10−15, equivalent to a Late Oligocene to Early Miocene age. Ages in the active methane venting sites typically are closer to the old end of this range than those in the reference sites. This age range suggests that the methane associated with venting and gas hydrate formation in this area is derived from organic materials accumulated during the initial opening of the Japan Sea. The Umitaka Spur–Joetsu Knoll gas hydrate field demonstrates the movement of deep fluids associated with the release of significant amounts of methane from the seafloor, processes which might be important components of mass transfer and carbon cycle in the shallow geosphere. [Copyright &y& Elsevier]

Abstract: Iodine and its radioisotope 129I have been successfully used to trace the origin of pore waters in submarine fluid escape structures because of their close association with organic material in deeply buried sediments. We report here halogen concentrations and 129I/I ratios for fluids of five mud volcanoes sampled along an E–W transect across the Gulf of Cadiz in the NE Atlantic Ocean. Concentrations of iodide and bromide increase consistently seaward accompanied by a decrease in 129I/I ratios from 6490×10−15 to 663×10−15. The exceptionally high 129I/I ratios at the near-shore locations reflect the presence of fissiogenic 129I, produced in situ by spontaneous fission of 238U within terrigenous sediments and released into pore water during clay mineral diagenetic processes. The observed 129I/I and halogen trends, together with similar changes in 87Sr/86Sr ratios, indicate a progressive seaward transition from inorganic-terrigenous to organic-marine fluid sources. Comparison of our results with literature data for varying geological settings reveals a general relationship between fissiogenic 129I, radiogenic 87Sr and the lithology or provenance of rocks and sediments, respectively. While 129I/I ratios in continental rock-hosted aquifers and terrigenous sedimentary systems are dominated by in situ production of fissiogenic 129I, iodine isotopes in oceanic settings or volcanogenic marine sediments reflect the release of ‘old’ iodine from deeply buried organic matter. The Gulf of Cadiz represents the full transition between these continental and oceanic 129I/I and 87Sr/86Sr end members. This is the first systematic investigation of fissiogenic 129I production in marine sedimentary environments. [Copyright &y& Elsevier]

Iodine concentration and radioisotopic composition (129I/I) were measured in the pore waters from the gas hydrate occurrence in the forearc basin offshore Shimokita Peninsula, north-eastern Japan, to determine the source formation of I and accompanying hydrocarbons. Iodine concentrations correlate well with the alkalinity and SO4 patterns, reflecting degradation stages of I-rich buried organic matter, rapidly increasing in the sulfate reduction interval, and becoming constant below 250 meters below the seafloor with an upwelling flux of 1.5 × 10−11 µmol cm−2 year−1. The 129I/I ratios of 300 × 10−15–400 × 10−15 in deep pore waters suggest ages for iodine and hydrocarbon sources as old as 40 Ma. These ages correlate well with the coaly source formations of the Eocene age thought to be responsible for the conventional natural gas deposits underlying the gas hydrate stability zone. Similar profiles are observed in 129I/I ratios of pore waters in the gas hydrate stability zone from the forearc basin in the eastern Nankai Trough, offshore central Japan, where pore waters are enriched in I and reach ages as old as ∼50 Ma through the sediment column. At the outer ridge site along the trough, on the other hand, relatively younger I are more frequently delivered probably through thrusts/faults associated with subduction. The nature of source formations of I and hydrocarbons in the offshore Shimokita Peninsula has a more terrestrial contribution compared with those in the Nankai Trough, but these formations are also considerably older than the host sediments, suggesting long-term transport of I and hydrocarbons for the accumulation of gas hydrates in both locations. [ABSTRACT FROM AUTHOR]