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USGS2022

Porewater chemistry of Louisiana marshes with contrasting salinities and its implications for coastal acidification

Dissolved inorganic carbon (DIC) and total alkalinity (TA) are fundamental components of carbonate systems that control pH and buffering capacity of the receiving water body. Three coastal marshes with contrasting salinities in Barataria Basin, Louisiana, USA, were sampled to understand seasonal changes in porewater carbonate chemistry and its impact on surrounding water bodies. Each marsh was sampled five times between December 2018 and October 2019. Porewater DIC and TA increased with depth irrespective of marsh type and ranged from 4.47 to 31.61 mmol/kg and from 1.78 to 28.56 mmol/kg, respectively. The salt marsh had higher porewater DIC and TA compared to the lower salinity intermediate and brackish marshes, probably due to sulfate reduction in the salt marsh. However, it is likely that denitrification is the dominant anaerobic process in these marshes because of low porewater TA/DIC ratios in all three marshes. Porewater TA and DIC concentrations were generally higher during warmer months than colder months. However, the marsh flooding regime had a profound influence on TA and DIC concentrations by changing the redox potential of the marsh soil. Porewater TA/DIC ratios in all three marshes were generally less than 1, while surface water TA/DIC ratios were around 1, suggesting that export of DIC and TA from coastal marshes have the potential to contribute to coastal acidification.

Louisiana↗

USGS2017

Soil microbial community composition is correlated to soil carbon processing along a boreal wetland formation gradient

Climate change is modifying global biogeochemical cycles. Microbial communities play an integral role in soil biogeochemical cycles; knowledge about microbial composition helps provide a mechanistic understanding of these ecosystem-level phenomena. Next generation sequencing approaches were used to investigate changes in microbial functional groups during ecosystem development, in response to climate change, in northern boreal wetlands. A gradient of wetlands that developed following permafrost degradation was used to characterize changes in the soil microbial communities that mediate C cycling: a bog representing an “undisturbed” system with intact permafrost, and a younger bog and an older bog that formed following the disturbance of permafrost thaw. Reference 16S rRNA databases and several diversity indices were used to assess structural differences among these communities, to assess relationships between soil microbial community composition and various environmental variables including redox potential and pH. Rates of potential CO2 and CH4 gas production were quantified to correlate sequence data with gas flux. The abundance of organic C degraders was highest in the youngest bog, suggesting higher rates of microbial processes, including potential CH4 production. In addition, alpha diversity was also highest in the youngest bog, which seemed to be related to a more neutral pH and a lower redox potential. These results could potentially be driven by increased niche differentiation in anaerobic soils. These results suggest that ecosystem structure, which was largely driven by changes in edaphic and plant community characteristics between the “undisturbed” permafrost bog and the two bogs formed following permafrost thaw, strongly influenced microbial function.

European Journal of Soil Biology↗

USGS2009

Methane sources and production in the northern Cascadia margin gas hydrate system

The oceanographic and tectonic conditions of accretionary margins are well-suited for several potential processes governing methane generation, storage and release. To identify the relevant methane evolution pathways in the northern Cascadia accretionary margin, a four-site transect was drilled during Integrated Ocean Drilling Program Expedition 311. The δ13C values of methane range from a minimum value of − 82.2‰ on an uplifted ridge of accreted sediment near the deformation front (Site U1326, 1829 mbsl, meters below sea level) to a maximum value of − 39.5‰ at the most landward location within an area of steep canyons near the shelf edge (Site U1329, 946 mbsl). An interpretation based solely on methane isotope values might conclude the 13C-enrichment of methane indicates a transition from microbially- to thermogenically-sourced methane. However, the co-existing CO2 exhibits a similar trend of 13C-enrichment along the transect with values ranging from − 22.5‰ to +25.7‰. The magnitude of the carbon isotope separation between methane and CO2 (εc = 63.8 ± 5.8) is consistent with isotope fractionation during microbially mediated carbonate reduction. These results, in conjunction with a transect-wide gaseous hydrocarbon content composed of > 99.8% (by volume) methane and uniform δDCH4 values (− 172‰ ± 8) that are distinct from thermogenic methane at a seep located 60 km from the Expedition 311 transect, suggest microbial CO2 reduction is the predominant methane source at all investigated sites. The magnitude of the intra-site downhole 13C-enrichment of CO2 within the accreted ridge (Site U1326) and a slope basin nearest the deformation front (Site U1325, 2195 mbsl) is ~ 5‰. At the mid-slope site (Site U1327, 1304 mbsl) the downhole 13C-enrichment of the CO2 is ~ 25‰ and increases to ~ 40‰ at the near-shelf edge Site U1329. This isotope fractionation pattern is indicative of more extensive diagenetic alteration at sites with greater 13C-enrichment. The magnitude of the 13C-enrichment of CO2 correlates with decreasing sedimentation rates and a diminishing occurrence of stratigraphic gas hydrate. We suggest the decreasing sedimentation rates increase the exposure time of sedimentary organic matter to aerobic and anaerobic degradation, during burial, thereby reducing the availability of metabolizable organic matter available for methane production. This process is reflected in the occurrence and distribution of gas hydrate within the northern Cascadia margin accretionary prism. Our observations are relevant for evaluating methane production and the occurrence of stratigraphic gas hydrate within other convergent margins.

Earth and Planetary Science Letters↗

USGS2016

Insights into methane dynamics from analysis of authigenic carbonates and chemosynthetic mussels at newly-discovered Atlantic Margin seeps

The recent discovery of active methane venting along the US northern and mid-Atlantic margin represents a new source of global methane not previously accounted for in carbon budgets from this region. However, uncertainty remains as to the origin and history of methane seepage along this tectonically inactive passive margin. Here we present the first isotopic analyses of authigenic carbonates and methanotrophic deep-sea mussels, Bathymodiolus sp., and the first direct constraints on the timing of past methane emission, based on samples collected at the upper slope Baltimore Canyon (&sim;385 m water depth) and deepwater Norfolk (&sim;1600 m) seep fields within the area of newly-discovered venting. The authigenic carbonates at both sites were dominated by aragonite, with an average signature of −47&permil; , a value consistent with microbially driven anaerobic oxidation of methane-rich fluids occurring at or near the sediment–water interface. Authigenic carbonate U and Sr isotope data further support the inference of carbonate precipitation from seawater-derived fluids rather than from formation fluids from deep aquifers. Carbonate stable and radiocarbon ( and ) isotope values from living Bathymodiolus sp. specimens are lighter than those of seawater dissolved inorganic carbon, highlighting the influence of fossil carbon from methane on carbonate precipitation. U–Th dates on authigenic carbonates suggest seepage at Baltimore Canyon between 14.7±0.6 ka to 15.7±1.6 ka , and at the Norfolk seep field between 1.0±0.7 ka to 3.3±1.3 ka , providing constraint on the longevity of methane efflux at these sites. The age of the brecciated authigenic carbonates and the occurrence of pockmarks at the Baltimore Canyon upper slope could suggest a link between sediment delivery during Pleistocene sea-level lowstand, accumulation of pore fluid overpressure from sediment compaction, and release of overpressure through subsequent venting. Calculations show that the Baltimore Canyon site probably has not been within the gas hydrate stability zone (GHSZ) in the past 20 ka, meaning that in-situ release of methane from dissociating gas hydrate cannot be sustaining the seep. We cannot rule out updip migration of methane from dissociation of gas hydrate that occurs farther down the slope as a source of the venting at Baltimore Canyon, but consider that the history of rapid sediment accumulation and overpressure may play a more important role in methane emissions at this site.

Baltimore Canyon seep fields, Norfolk seep fields↗

USGS2004

The microbial arsenic cycle in Mono Lake, California

Significant concentrations of dissolved inorganic arsenic can be found in the waters of a number of lakes located in the western USA and in other water bodies around the world. These lakes are often situated in arid, volcanic terrain. The highest concentrations of arsenic occur in hypersaline, closed basin soda lakes and their remnant brines. Although arsenic is a well-known toxicant to eukaryotes and prokaryotes alike, some prokaryotes have evolved biochemical mechanisms to exploit arsenic oxyanions (i.e., arsenate and arsenite); they can use them either as an electron acceptor for anaerobic respiration (arsenate), or as an electron donor (arsenite) to support chemoautotrophic fixation of CO 2 into cell carbon. Unlike in freshwater or marine ecosystems, these processes may assume quantitative significance with respect to the carbon cycle in arsenic-rich soda lakes. For the past several years our research has focused on the occurrence and biogeochemical manifestations of these processes in Mono Lake, a particularly arsenic-rich environment. Herein we review some of our findings concerning the biogeochemical arsenic cycle in this lake, with the hope that it may broaden the understanding of the influence of microorganisms upon the speciation of arsenic in more common, less “extreme” environments, such as drinking water aquifers.

California↗

USGS2008

Soil magnetic susceptibility reflects soil moisture regimes and the adaptability of tree species to these regimes

Flooded, saturated or poorly drained soils are frequently anaerobic, leading to dissolution of the strongly magnetic minerals, magnetite and maghemite, and a corresponding decrease in soil magnetic susceptibility (MS). In this study of five temperate deciduous forests in east-central Illinois, USA, mean surface soil MS was significantly higher adjacent to upland tree species (31 ?? 10-5 SI) than adjacent to floodplain or lowland tree species (17 ?? 10-5 SI), when comparing regional soils with similar parent material of loessal silt. Although the sites differ in average soil MS for each tree species, the relative order of soil MS means for associated tree species at different locations is similar. Lowland tree species, Celtis occidentalis L., Ulmus americana L., Acer saccharinum L., Carya laciniosa (Michx. f.) Loud., and Fraxinus pennsylvanica Marsh. were associated with the lowest measured soil MS mean values overall and at each site. Tree species' flood tolerance rankings increased significantly, as soil MS values declined, the published rankings having significant correlations with soil MS values for the same species groups. The three published classifications of tree species' flood tolerance were significantly correlated with associated soil MS values at all sites, but most strongly at Allerton Park, the site with the widest range of soil drainage classes and MS values. Using soil MS measurements in forests with soil parent material containing similar initial levels of strongly magnetic minerals can provide a simple, rapid and quantitative method to classify soils according to hydric regimes, including dry conditions, and associated plant composition. Soil MS values thus have the capacity to quantify the continuum of hydric tolerances of tree species and guide tree species selection for reforestation. ?? 2007 Elsevier B.V. All rights reserved.

Forest Ecology and Management↗

USGS2020

Methane oxidation dynamics in a karst subterranean estuary

Chemical gradients between fresh, brackish and saline waters shape biogeochemical reactions and organic matter transformation within subterranean estuaries. In the Yucatán Peninsula’s karst subterranean estuary (KSE), methane and dissolved organic matter generated during the anaerobic decomposition of tropical forest vegetation are transported into flooded cave networks where microbial consumption greatly reduces their concentrations in the groundwater. To test the hypothesis that chemoclines associated with salinity gradients of the KSE are sites of methane oxidation, we obtained methane concentration and δ 13 C profiles of unprecedented vertical resolution from within a fully-submerged cave system located 6.6 km inland from the coastline using the ‘OctoPiPi’ (OPP) water sampler. Along a 12–24 cm thick low-salinity-halocline at ∼4.5 m water depth, salinity increased from fresh to brackish (0.2–1.8 psu), methane concentrations decreased, and δ 13 C values increased, as expected for microbial methane oxidation. The underlying brackish water had elevated oxygen concentrations compared to the always anoxic freshwater, suggesting that aerobic methane oxidation is the dominant process facilitating methane consumption. By contrast, as salinity increased from 1.8 to 36 psu through a 24–36 cm thick high-salinity-halocline between the meteoric lens and the saline groundwater at ∼20 m water depth, methane concentrations and δ 13 C values were constant. Conservative mixing and kinetic isotope models incorporating the methane data confirm a hotspot for microbial methane oxidation at the low-salinity-halocline. At least 98% of methane originating in the anoxic freshwaters was removed before its transport via channelized flow towards the coastline. These findings provide novel insight into the spatial constraints of methane dynamics within a karst subterranean estuary.

Ox Bel Ha cave system↗

USGS2007

Methane-derived authigenic carbonates from the northern Gulf of Mexico - MD02 Cruise

Authigenic carbonates were sampled in piston cores collected from both the Tunica Mound and the Mississippi Canyon area on the continental slope of the northern Gulf of Mexico during a Marion Dufresne cruise in July 2002. The carbonates are present as hardgrounds, porous crusts, concretions or nodules and shell fragments with or without carbonate cements. Carbonates occurred at gas venting sites which are likely to overlie gas hydrates bearing sediments. Electron microprobe, X-ray diffraction (XRD) and thinsection investigations show that these carbonates are high-Mg calcite (6–21 mol% MgCO 3 ), with significant presence of framboidal pyrite. All carbonates are depleted in 13 C ( δ 13 C = − 61.9 to − 31.5‰ PDB) indicating that the carbon is derived mainly from anaerobic methane oxidation (AMO). Age estimates based on 14 C dating of shell fragments and on regional sedimentation rates indicate that these authigenic carbonates formed within the last 1000 yr in the Mississippi Canyon and within 5500 yr at the Tunica Mound. The oxygen isotopic composition of carbonates ranges from + 3.4 to + 5.9‰ PDB. Oxygen isotopic compositions and Mg 2+ contents of carbonates, and present in-situ temperatures of bottom seawater/sediments, show that some of these carbonates, especially from a core associated with underlying massive gas hydrates precipitated in or near equilibrium with bottom-water. On the other hand, those carbonates more enriched in 18 O are interpreted to have precipitated from 18 O-rich fluids which are thought to have been derived from the dissociation of gas hydrates. The dissociation of gas hydrates in the northern Gulf of Mexico within the last 5500 yr may be caused by nearby salt movement and related brines.

Journal of Geochemical Exploration↗

USGS2010

Vadose zone attenuation of organic compounds at a crude oil spill site - Interactions between biogeochemical reactions and multicomponent gas transport

Contaminant attenuation processes in the vadose zone of a crude oil spill site near Bemidji, MN have been simulated with a reactive transport model that includes multicomponent gas transport, solute transport, and the most relevant biogeochemical reactions. Dissolution and volatilization of oil components, their aerobic and anaerobic degradation coupled with sequential electron acceptor consumption, ingress of atmospheric O 2 , and the release of CH 4 and CO 2 from the smear zone generated by the floating oil were considered. The focus of the simulations was to assess the dynamics between biodegradation and gas transport processes in the vadose zone, to evaluate the rates and contributions of different electron accepting processes towards vadose zone natural attenuation, and to provide an estimate of the historical mass loss. Concentration distributions of reactive (O 2 , CH 4 , and CO 2 ) and non-reactive (Ar and N 2 ) gases served as key constraints for the model calibration. Simulation results confirm that as of 2007, the main degradation pathway can be attributed to methanogenic degradation of organic compounds in the smear zone and the vadose zone resulting in a contaminant plume dominated by high CH 4 concentrations. In accordance with field observations, zones of volatilization and CH 4 generation are correlated to slightly elevated total gas pressures and low partial pressures of N 2 and Ar, while zones of aerobic CH 4 oxidation are characterized by slightly reduced gas pressures and elevated concentrations of N 2 and Ar. Diffusion is the most significant transport mechanism for gases in the vadose zone; however, the simulations also indicate that, despite very small pressure gradients, advection contributes up to 15% towards the net flux of CH 4 , and to a more limited extent to O 2 ingress. Model calibration strongly suggests that transfer of biogenically generated gases from the smear zone provides a major control on vadose zone gas distributions and vadose zone carbon balance. Overall, the model was successful in capturing the complex interactions between biogeochemical reactions and multicomponent gas transport processes. However, despite employing a process-based modeling approach, honoring observed parameter ranges, and generally obtaining good agreement between field observations and model simulations, accurate quantification of natural attenuation rates remains difficult. The modeling results are affected by uncertainties regarding gas phase saturations, tortuosities, and the magnitude of CH 4 and CO 2 flux from the smear zone. These findings highlight the need to better delineate gas fluxes at the model boundaries, which will help constrain contaminant degradation rates, and ultimately source zone longevity.

Minnesota↗

USGS2011

Loss of volatile hydrocarbons from an LNAPL oil source

The light nonaqueous phase liquid (LNAPL) oil pool in an aquifer that resulted from a pipeline spill near Bemidji, Minnesota, was analyzed for volatile hydrocarbons (VHCs) to determine if the composition of the oil remains constant over time. Oil samples were obtained from wells at five locations in the oil pool in an anaerobic part of the glacial outwash aquifer. Samples covering a 21-year period were analyzed for 25 VHCs. Compared to the composition of oil from the pipeline source, VHCs identified in oil from wells sampled in 2008 were 13 to 64% depleted. The magnitude of loss for the VHCs analyzed was toluene ≫ o-xylene, benzene, C 6 and C 10–12 n-alkanes > C 7 –C 9 n-alkanes > m-xylene, cyclohexane, and 1- and 2-methylnaphthalene > 1,2,4-trimethylbenzene and ethylbenzene. Other VHCs including p-xylene, 1,3,5- and 1,2,3-trimethylbenzenes, the tetramethylbenzenes, methyl- and ethyl-cyclohexane, and naphthalene were not depleted during the time of the study. Water–oil and air–water batch equilibration simulations indicate that volatilization and biodegradation is most important for the C 6 –C 9 n-alkanes and cyclohexanes; dissolution and biodegradation is important for most of the other hydrocarbons. Depletion of the hydrocarbons in the oil pool is controlled by: the lack of oxygen and nutrients, differing rates of recharge, and the spatial distribution of oil in the aquifer. The mass loss of these VHCs in the 5 wells is between 1.6 and 7.4% in 29 years or an average annual loss of 0.06–0.26%/year. The present study shows that the composition of LNAPL changes over time and that these changes are spatially variable. This highlights the importance of characterizing the temporal and spatial variabilities of the source term in solute-transport models.

Minnesota↗

USGS2014

Comparison of surficial CO2 efflux to other measures of subsurface crude oil degradation

At a spill site near Bemidji, Minnesota, crude oil at the water table has been undergoing anaerobic biodegradation for over 30 years. Previous work at this site has shown that methane produced from biodegradation of the oil migrates upward and is oxidized in a methanotrophic zone midway between the water table and the surface. To compare microbial activity measurement methods from multiple locations in the oil body, surficial carbon dioxide efflux, methanogen and methanotroph concentrations, and oil degradation state were collected. Carbon dioxide effluxes over the oil body averaged more than four times those at the background site. Methanotrophic bacteria concentrations measured using pmoA were over 10 5 times higher above the oil-contaminated sediments compared with the background site. Methanogenic archaea measured using mcrA ranged from 10 5 to over 10 7 in the oil and were below detection in the background. Methanogens correlated very well with methanotroph concentrations (r = 0.99), n-alkylcyclohexane losses as a proxy for degradation state (r = − 0.96), and somewhat less well with carbon dioxide efflux (r = 0.92). Carbon dioxide efflux similarly correlated to methanotroph concentrations (r = 0.90) and n-alkylcyclohexane losses (r = − 0.91).

Minnesota↗

USGS2015

Relating subsurface temperature changes to microbial activity at a crude oil-contaminated site

Crude oil at a spill site near Bemidji, Minnesota has been undergoing aerobic and anaerobic biodegradation for over 30 years, creating a 150–200 m plume of primary and secondary contaminants. Microbial degradation generates heat that should be measurable under the right conditions. To measure this heat, thermistors were installed in wells in the saturated zone and in water-filled monitoring tubes in the unsaturated zone. In the saturated zone, a thermal groundwater plume originates near the residual oil body with temperatures ranging from 2.9 °C above background near the oil to 1.2 °C down gradient. Temperatures in the unsaturated zone above the oil body were up to 2.7 °C more than background temperatures. Previous work at this site has shown that methane produced from biodegradation of the oil migrates upward and is oxidized in a methanotrophic zone midway between the water table and the surface. Enthalpy calculations and observations demonstrate that the temperature increases primarily result from aerobic methane oxidation in the unsaturated zone above the oil. Methane oxidation rates at the site independently estimated from surface CO 2 efflux data are comparable to rates estimated from the observed temperature increases. The results indicate that temperature may be useful as a low-cost measure of activity but care is required to account for the correct heat-generating reactions, other heat sources and the effects of focused recharge.

Minnesota↗

USGS2017

Effects of solid-liquid separation and storage on monensin attenuation in dairy waste management systems

Environmental release of veterinary pharmaceuticals has been of regulatory concern for more than a decade. Monensin is a feed additive antibiotic that is prevalent throughout the dairy industry and is excreted in dairy waste. This study investigates the potential of dairy waste management practices to alter the amount of monensin available for release into the environment. Analysis of wastewater and groundwater from two dairy farms in California consistently concluded that monensin is most present in lagoon water and groundwater downgradient of lagoons. Since the lagoons represent a direct source of monensin to groundwater, the effect of waste management, by mechanical screen separation and lagoon aeration, on aqueous monensin concentration was investigated through construction of lagoon microcosms. The results indicate that monensin attenuation is not improved by increased solid-liquid separation prior to storage in lagoons, as monensin is rapidly desorbed after dilution with water. Monensin is also shown to be easily degraded in lagoon microcosms receiving aeration, but is relatively stable and available for leaching under typical anaerobic lagoon conditions.

Journal of Environmental Management↗

USGS2016

Internal loading of phosphorus in western Lake Erie

This study applied eight techniques to obtain estimates of the diffusive flux of phosphorus (P) from bottom sediments throughout the western basin of Lake Erie. The flux was quantified from both aerobic and anaerobic incubations of whole cores; by monitoring the water encapsulated in bottom chambers; from pore water concentration profiles measured with a phosphate microelectrode, a diffusive equilibrium in thin films (DET) hydrogel, and expressed pore waters; and from mass balance and biogeochemical diagenetic models. Fluxes under aerobic conditions at summertime temperatures averaged 1.35 mg P/m 2 /day and displayed spatial variability on scales as small as a centimeter. Using two different temperature correction factors, the flux was adjusted to mean annual temperature yielding average annual fluxes of 0.43–0.91 mg P/m 2 /day and a western basin-wide total of 378–808 Mg P/year as the diffusive flux from sediments. This is 3–7% of the 11,000 Mg P/year International Joint Commission (IJC) target load for phosphorus delivery to Lake Erie from external sources. Using these average aerobic fluxes, the sediment contributes 3.0–6.3 μg P/L as a background internal contribution that represents 20–42% of the IJC Target Concentration of 15 μg P/L for the western basin. The implication is that this internal diffusive recycling of P is unlikely to trigger cyanobacterial blooms by itself but is sufficiently large to cause blooms when combined with external loads. This background flux may be also responsible for delayed response of the lake to any decrease in the external loading.

Lake Erie↗

USGS2026

PFAS remediation in a bioelectrochemical system inoculated with the west branch consortium (WBC-2)

Groundwater contamination by per - and polyfluoroalkyl substances (PFAS) poses a persistent environmental and public health concern. This study evaluates a two-chambered bioelectrochemical system (BES) inoculated with the West Branch Consortium (WBC-2) for PFAS remediation. Under an applied cathodic potential of −450 mV (versus Ag/AgCl), the BES with active WBC-2 achieved >99.0% perfluorooctanesulfonic acid (PFOS) removal within 21 days in deionized water with culture medium and > 98.9% removal of PFOS, perfluorooctanoic acid (PFOA), perfluorohexanoic acid (PFHxA), and perfluorohexanesulfonic acid (PFHxS) in contaminated groundwater after 102 days. Intermediate formation (e.g., PFOA, 6:2 fluorotelomer sulfonate (6:2 FTS), perfluoropropionic acid (PFPrA), perfluorobutanoic acid (PFBA)) and background-corrected fluoride release were consistent with PFOS transformation under anaerobic reducing conditions potentially involving defluorination. Following repeated PFOS spikes (100 μg/L on Days 0, 50, and 399), PFOA, PFPrA, and PFBA accumulated over 664 days. Despite being the dominant accumulated compound, PFOA accounted for <1.8% of the total spiked PFOS mass. Minimal PFOS transformation occurred in controls without active WBC-2, highlighting the importance of microbial metabolism. Biofilm analysis revealed dense colonization of rod-shaped bacteria on carbon fiber brushes. Enrichment of Bacillus , Agrobacterium , and other low-abundance taxa suggests selective adaptation to BES and PFAS conditions. These findings highlight BES driven by electrochemically stimulated microbial activity as a promising strategy for PFAS remediation.

Journal of Water Process Engineering↗

USGS2025

Tracking diagenetic alteration of magnetic susceptibility in thrust ridge and slope basin sediments of the Cascadia margin (ODP Sites 1249 and 1252; IODP Site U1325)

We investigated sediment core records from the Cascadia Margin (Ocean Drilling Program Sites 1249 and 1252 at Hydrate Ridge; Integrated Ocean Drilling Program Site U1325 offshore Vancouver Island) using a Zr/Rb heavy mineral proxy from X-ray fluorescence (XRF) core scanning to identify intervals of primary detrital magnetic susceptibility (κ) and predict intervals where diagenesis caused magnetite dissolution by hydrogen sulfide. We also measured total sulfur (TS) content, grain size distributions, total organic carbon (TOC) content, and the magnetic mineral assemblage to further constrain the role of diagenesis on κ. Understanding how κ can be used to better characterize the varied effects of detrital and diagenetic signals in marine settings is important for understanding biogeochemical cycling and records of paleoenvironmental change. The upper 100 m of slope basin Site 1252 contains multiple intervals (> 90 m total) of decreased κ correlated with elevated TS content, consistent with dissolution of magnetite and precipitation of pyrite, iron monosulfides, and/or elemental sulfur. Similarly at the other slope basin site, Site U1325, κ is lower and TS is elevated in the interval between 24 and 51 mbsf, due to sulfide formation. At both slope basin sites, these low κ intervals correspond with high TOC, suggesting the possibility that organoclastic sulfate reduction (OSR) is likely a major driver of diagenetic alteration of κ at these sites. High TS:TOC ratios at Site U1325 suggests anaerobic oxidation of methane (AOM) during sulfate-methane transition zone (SMTZ) migration may have contributed to alteration of κ. In contrast, within the upper 90 m of Site 1249, a methane seep site at the summit of Hydrate Ridge, κ is almost entirely altered by diagenetic processes, with much of the low κ explained by a high degree of iron sulfide formation, while some intervals are affected by precipitation of magnetic iron sulfides that maintain or even increase κ. The presence of abundant methane seepage and gas hydrate as well as chemosynthetic seafloor fauna at this site, suggests that sulfide is released to the water column and AOM, rather than OSR, drives diagenetic alteration of κ at this site. Overall, the slope basin sites show episodic variation of κ that is influenced by TOC content, likely driven by changes in marine primary productivity and sedimentation rate, while the seep site shows consistently altered κ with lower TS content and no correlation with TOC. Methane seep environments likely experience loss of hydrogen sulfide to the water column and oxidation of hydrogen sulfide by seafloor seep fauna, which limits the amount of solid phase sulfur (pyrite, iron monosulfides, elemental sulfur) that can be precipitated within the sediments. In contrast, the migration of a buried SMTZ at slope basin sites results in enhanced sulfur precipitation within the sediments. This integrated magnetic and geochemical approach reveals the diagenetic production pathway and residence time of sulfide with the sediment column ultimately controls the style and degree of diagenetic loss of κ in marine sediments. This approach works best in environments with unaltered reference intervals/sites, consistent magnetic mineralogy, and clay-to-silt grain sizes.

Cascadia margin, Pacific Ocean↗

USGS2008

Assessing sulfate reduction and methane cycling in a high salinity pore water system in the northern Gulf of Mexico

Pore waters extracted from 18 piston cores obtained on and near a salt-cored bathymetric high in Keathley Canyon lease block 151 in the northern Gulf of Mexico contain elevated concentrations of chloride (up to 838 mM) and have pore water chemical concentration profiles that exhibit extensive departures (concavity) from steady-state (linear) diffusive equilibrium with depth. Minimum ??13C dissolved inorganic carbon (DIC) values of -55.9??? to -64.8??? at the sulfate-methane transition (SMT) strongly suggest active anaerobic oxidation of methane (AOM) throughout the study region. However, the nonlinear pore water chemistry-depth profiles make it impossible to determine the vertical extent of active AOM or the potential role of alternate sulfate reduction pathways. Here we utilize the conservative (non-reactive) nature of dissolved chloride to differentiate the effects of biogeochemical activity (e.g., AOM and/or organoclastic sulfate reduction) relative to physical mixing in high salinity Keathley Canyon sediments. In most cases, the DIC and sulfate concentrations in pore waters are consistent with a conservative mixing model that uses chloride concentrations at the seafloor and the SMT as endmembers. Conservative mixing of pore water constituents implies that an undetermined physical process is primarily responsible for the nonlinearity of the pore water-depth profiles. In limited cases where the sulfate and DIC concentrations deviated from conservative mixing between the seafloor and SMT, the ??13C-DIC mixing diagrams suggest that the excess DIC is produced from a 13C-depleted source that could only be accounted for by microbial methane, the dominant form of methane identified during this study. We conclude that AOM is the most prevalent sink for sulfate and that it occurs primarily at the SMT at this Keathley Canyon site.

Marine and Petroleum Geology↗

USGS2008

Thermal stability of ladderane lipids as determined by hydrous pyrolysis

Anaerobic ammonium oxidation (anammox) has been recognized as a major process resulting in loss of fixed inorganic nitrogen in the marine environment. Ladderane lipids, membrane lipids unique to anammox bacteria, have been used as markers for the detection of anammox in marine settings. However, the fate of ladderane lipids after sediment burial and maturation is unknown. In this study, anammox bacterial cell material was artificially matured by hydrous pyrolysis at constant temperatures ranging from 120 to 365 ??C for 72 h to study the stability of ladderane lipids during progressive dia- and catagenesis. HPLC-MS/MS analysis revealed that structural alterations of ladderane lipids already occurred at 120 ??C. At temperatures >140 ??C, ladderane lipids were absent and only more thermally stable products could be detected, i.e., ladderane derivatives in which some of the cyclobutane rings were opened. These diagenetic products of ladderane lipids were still detectable up to temperatures of 260 ??C using GC-MS. Thus, ladderane lipids are unlikely to occur in ancient sediments and sedimentary rocks, but specific diagenetic products of ladderane lipids will likely be present in sediments and sedimentary rocks of relatively low maturity (i.e., C31 hopane 22S/(22S + 22R) ratio <0.2 or ????/(???? + ???? + ????) ratio of >0.5). ?? 2008 Elsevier Ltd.

Organic Geochemistry↗