Carbon Deposition and Burial in Estuarine Sediments of the Contiguous United States
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J. A. Hutchings↗
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Isotopic Composition of Carbon Dioxide Released from Confidence Hills Sediment as Measured by the Sample Analysis at Mars (SAM) Quadrupole Mass Spectrometer
In October 2014, the Mars Science Laboratory (MSL) "Curiosity" rover drilled into the sediment at the base of Mount Sharp in a location namsed Cionfidence Hills (CH). CH marked the fifth sample pocessed by the Sample Analysis at Mars (SAM) instrument suite since Curiosity arrived in Gale Crater, with previous analyses performed at Rocknest (RN), John Klein (JK), Cumberland (CB), and Windjana (WJ). Evolved gas analysis (EGA) of all samples has indicated H2O as well as O-, C- and S-bearing phases in the samples, often at abundances that would be below the detection limit of the CheMin instrument. By examining the temperatures at which gases are evolved from samples, SAM EGA data can help provide clues to the mineralogy of volatile-bearing phases when their identities are unclear to CheMin. SAM may also detect gases evolved from amorphous material in solid samples, which is not suitable for analysis by CheMin. Finally, the isotopic composition of these gases may suggest possible formation scenarios and relationships between phases. We will discuss C isotope ratios of CO2 evolved from the CH sample as measured with SAM's quadrupole mass spectrometer (QMS) and draw comparisons to samples previously analyzed by SAM.
Franz, H. B.↗
Earth's early atmosphere as seen from carbon and nitrogen isotopic analysis of Archean sediments
The origin and evolution of the Earth's early atmosphere has long been a topic of great interest but determination of actual compositions over geologic time is a difficult problem. However, recent systematic studies of stromatolite deposits (Precambrian Paleobiology Research Group) has extended our knowledge of Archean ecosystems. It has been shown that many stromatolite deposits have undergone negligible alteration since their time of formation. The discovery of primary fluid inclusions within unaltered 3.5 b.y. old Archiean sediments and the observation that the 3.3 b.y. old Barberton cherts have remained closed to argon loss and have not been subjected to thermal metamorphism suggests that an opportunity exists for the direct measurement of the volatile constituents present at their time of formation. Of primary interest to this study was the possibility that the stromatolites and other Archean sediments might retain a vestige of the atmosphere and thus afford an indication of the variations in carbon dioxide and nitrogen isotopic compositions with time. A suite of essentially unaltered Archean stromatolites and the cherts of different ages and geologic sites have been analyzed for their trapped carbon dioxide and nitrogen compositions by the stepped combustion extraction tech nique utilizing static mass spectrometers for the isotope measurements.
Gibson, E. K., Jr.↗
Biologically mediated isotope fractionations - Biochemistry, geochemical significance and preservation in the earth's oldest sediments
Preferential metabolization of isotopically light carbon and sulfur has resulted in a fractionation of the stable isotopes of these elements on a global scale, with the light species (C-12, S-32) markedly concentrated in biogenic materials. Since the biological effects are basically retained when carbon and sulfur are incorporated in sediments, the respective fractionations are propagated into the rock section of the geochemical cycle, this having consequently caused a characteristic bipartition of both elements between 'light' and 'heavy' crustal reservoirs. Preservation of the biological isotope effects in sedimentary rocks makes it possible to trace the underlying biochemical processes back over most of the geological record. According to the available evidence, biological (autotrophic) carbon fixation arose prior to 3.5(if not 3.8) billion years ago, while the emergence of dissimilatory sulfate reduction antedates the appearance of the oldest presumably bacteriogenic sulfur isotope patterns in rocks between 2.7 and 2.8 billion years old. Hence, biological control of the terrestrial carbon and sulfur cycles has been established very early in the earth's history.
Schidlowski, M.↗
Isotope Ratio Monitoring Gas Chromatography Mass Spectrometry (IRM-GCMS)
On Earth, the C-13 content of organic compounds is depleted by roughly 13 to 23 permil from atmospheric carbon dioxide. This difference is largely due to isotope effects associated with the fixation of inorganic carbon by photosynthetic organisms. If life once existed on Mars, then it is reasonable to expect to observe a similar fractionation. Although the strongly oxidizing conditions on the surface of Mars make preservation of ancient organic material unlikely, carbon-isotope evidence for the existence of life on Mars may still be preserved. Carbon depleted in C-13 could be preserved either in organic compounds within buried sediments, or in carbonate minerals produced by the oxidation of organic material. A technique is introduced for rapid and precise measurement of the C-13 contents of individual organic compounds. A gas chromatograph is coupled to an isotope-ratio mass spectrometer through a combustion interface, enabling on-line isotopic analysis of isolated compounds. The isotope ratios are determined by integration of ion currents over the course of each chromatographic peak. Software incorporates automatic peak determination, corrections for background, and deconvolution of overlapped peaks. Overall performance of the instrument was evaluated by the analysis of a mixture of high purity n-alkanes of know isotopic composition. Isotopic values measured via IRM-GCMS averaged withing 0.55 permil of their conventionally measured values.
Freeman, K. H.↗
The oxygen content of ocean bottom waters, the burial efficiency of organic carbon, and the regulation of atmospheric oxygen
Data for the burial efficiency of organic carbon with marine sediments have been compiled for 69 locations. The burial efficiency as here defined is the ratio of the quantity of organic carbon which is ultimately buried to that which reaches the sediment-water interface. As noted previously, the sedimentation rate exerts a dominant influence on the burial efficiency. The logarithm of the burial efficiency is linearly related to the logarithm of the sedimentation rate at low sedimentation rates. At high sedimentation rates the burial efficiency can exceed 50% and becomes nearly independent of the sedimentation rate. The residual of the burial efficiency after the effect of the sedimentation rate has been subtracted is a weak function of the O2 concentration in bottom waters. The scatter is sufficiently large, so that the effect of the O2 concentration in bottom waters on the burial efficiency of organic matter could be either negligible or a minor but significant part of the mechanism that controls the level of O2 in the atmosphere.
Non-NASA Center↗
The combined application of organic sulphur and isotope geochemistry to assess multiple sources of palaeobiochemicals with identical carbon skeletons
Five immature sediments from a Messinian evaporitic basin, representing one evaporitic cycle, were studied using molecular organic sulphur and isotope geochemistry. It is shown that a specific carbon skeleton which is present in different "modes of occurrence" ("free" hydrocarbon, alkylthiophene, alkylthiolane, alkyldithiane, alkylthiane, and sulphur-bound in macromolecules) may have different biosynthetic precursors which are possibly derived from different biota. It is demonstrated that the mode of occurrence and the carbon isotopic composition of a sedimentary lipid can be used to "reconstruct" its biochemical precursor. This novel approach of recognition of the suite of palaeobiochemicals present during the time of deposition allows for identification of the biological sources with an unprecedented specificity.
Non-NASA Center↗
Microbial sulfate reduction and organic sulfur formation in sinking marine particles
Climate change is driving an expansion of marine oxygen-deficient zones, which may alter the global cycles of carbon, sulfur, nitrogen, and trace metals. Currently, however, we lack a full mechanistic understanding of how oxygen deficiency affects organic carbon cycling and burial. In this work, we show that cryptic microbial sulfate reduction occurs in sinking particles from the eastern tropical North Pacific oxygen-deficient zone and that some microbially produced sulfide reacts rapidly to form organic sulfur that is resistant to acid hydrolysis. Particle-hosted sulfurization could enhance carbon preservation in sediments underlying oxygen-deficient water columns and serve as a stabilizing feedback between expanding anoxic zones and atmospheric carbon dioxide. A similar mechanism may help explain more-extreme instances of organic carbon preservation associated with marine anoxia in Earth history.
59 BASIC BIOLOGICAL SCIENCES↗
Composition and Flux of Dissolved and Particulate Carbon and Nitrogen in the Lower Tocantins River
The Tocantins River contributes ~5 % of the total flux of water to the Amazon River plume in the Atlantic Ocean. Here, we evaluate monthly variability in the composition and abundance of carbon, nitrogen, and suspended sediment in the lower reaches of the Tocantins River from 2014-2016. Dissolved organic carbon (DOC) concentrations generally increased during periods of high discharge and are ~1.5 times lower than average concentrations at the mouth of the Amazon River. Dissolved inorganic carbon (DIC) similarly increased during periods of high discharge. Total dissolved nitrogen (TDN) and individual nitrogen species followed a similar temporal pattern, increasing during high water. $\text{NO}^-_3$ predominated the dissolved inorganic nitrogen (DIN) pool, followed by $\text{NH}_4^+$, and $\text{NO}_2^-$ , characteristic of environments with a relatively low anthropogenic impact. Dissolved fractions represented 92 % of the total carbon exported and 78 % of the total nitrogen exported. The suspended particulate sediment flux was 2.72 x 10 6 t yr -1 , with fine suspended sediment (FSS) dominating (71.3 %). Concentrations of carbon relative to nitrogen indicate a primarily terrigenous source of organic matter and CO 2 derived from in situ respiration of this material during the rainy season and a primarily algal/bacterial source of organic matter during the dry season. Considering past estimates of dissolved carbon and nitrogen fluxes from the Amazon River to the Atlantic Ocean, the Tocantins River contributes 3 and 3.7 % to total fluxes to the Amazon River plume region, respectively. While this contribution is relatively small, it may be influenced by future changes to the basin’s land use and hydrology.
54 ENVIRONMENTAL SCIENCES↗
The Magnetic Properties Of Aggregate Polycrystalline Diamond: Implications For Carbonado Petrogenesis
Carbonados are a type of diamond, which are made up of many aggregrates of small crystalline diamonds or microdiamonds. The term "carbonado" comes from the Portuguese word carbonated. They are only found in sedimentary deposits in the Central African Republic (CAR) and the Bahia Province of Brazil. They were once the source of the world's supply of industrial diamonds. Their origin is uncertain but several mutually exclusive hypotheses have been proposed. This theories are: (1) extraterrestrial, that is they formed from the dust cloud of original solar nebulae; (2) produced by the high temperatures and pressures of the Earth's mantle; (3) or as the result of an extra-terrestrial impact into a carbon rich layer of sediment. Our study was done to further the understanding of their origin. We measured the magnetic properties on some twenty samples from the CAR. An earlier study was done on whole samples of carbonados and the "common" or kimberlitic diamond. Our work differed in that we started at the surface and subsequently removed the surface layers (by days of acid immersion) into the interior; measuring the magnetic properties at each interval. This procedure permits us to monitor the distribution of magnetic substances within the samples. Our results showed that the magnetic carriers are distributed on the surface including the open pores and that the carbonado interior is essentially non-magnetic. This result suggests that the initial formation environment was deficient in magnetic particles. Such a situation could indicate that their formation was the result of an extra-terrestrial body impacting carbon-rich sediment. Obviously, more work will be required on isotopic and chemical analyses before a more detailed ori-in can be determined.
Kleteschka, Gunther↗
Porewater Geochemical Assessment of Seismic Indications for Gas Hydrate Presence and Absence: Mahia Slope, East of New Zealand’s North Island
We compare sediment vertical methane flux off the Mahia Peninsula, on the Hikurangi Margin, east of New Zealand’s North Island, with a combination of geochemical, multichannel seismic and sub-bottom profiler data. Stable carbon isotope data provided an overview of methane contributions to shallow sediment carbon pools. Methane varied considerably in concentration and vertical flux across stations in close proximities. At two Mahia transects, methane profiles correlated well with integrated seismic and TOPAS data for predicting vertical methane migration rates from deep to shallow sediment. However, at our “control site”, where no seismic blanking or indications of vertical gas migration were observed, geochemical data were similar to the two Mahia transect lines. This apparent mismatch between seismic and geochemistry data suggests a potential to underestimate gas hydrate volumes based on standard seismic data interpretations. To accurately assess global gas hydrate deposits, multiple approaches for initial assessment, e.g., seismic data interpretation, heatflow profiling and controlled-source electromagnetics, should be compared to geochemical sediment and porewater profiles. A more thorough data matrix will provide better accuracy in gas hydrate volume for modeling climate change and potential available energy content.
03 NATURAL GAS↗
Heterogeneity in Permeability and Particulate Organic Carbon Content Controls the Redox Condition of Riverbed Sediments at Different Timescales
Abstract The hydrological and biogeochemical properties of the hyporheic zone in stream and riverine ecosystems have been extensively studied over the past two decades. Although it is widely acknowledged that sediment heterogeneity can influence biogeochemical reactions, little effort has been made to understand the role of heterogeneity on the spatiotemporal variability of riverbed redox conditions under changing flow dynamics at different timescales. Here we integrate a mechanistic model and field data to demonstrate that heterogeneity in permeability plays a vital role in modulating sediment redox conditions at both seasonal (annual) and event (daily‐to‐weekly) timescales, whereas heterogeneity in particulate organic carbon (POC) content only has a comparable influence on redox conditions at the seasonal timescale. These findings underscore the importance of accurately characterizing sediment heterogeneity, in terms of permeability and POC content, in quantifying biogeochemical dynamics in the riverbed and hyporheic zones of riverine ecosystems.
Geology↗
Archean sedimentary styles and early crustal evolution
The distinctions between and implications of early and late Archean sedimentary styles are presented. Early Archean greenstone belts, such as the Barberton of South Africa and those in the eastern Pilbar Block of Australia are characterized by fresh or slightly reworked pyroclastic debris, orthochemical sediments such as carbonates, evaporites, and silica, and biogenic deposits including cherts and stromatolitic units. Terrigenous deposits are rare, and it is suggested that early Archean sediments were deposited on shallow simatic platforms, with little or no components derived from sialic sources. In contrast, late Archean greenstone belts in the Canadian Shield and the Yilgarn Block of Australia contain coarse terrigenous clastic rocks including conglomerate, sandstone, and shale derived largely from sialic basement. Deposition appears to have taken place in deepwater, tectonically unstable environments. These observations are interpreted to indicate that the early Archean greenstone belts formed as anorogenic, shallow water, simatic platforms, with little or no underlying or adjacent continental crust, an environment similar to modern oceanic islands formed over hot spots.
Lowe, D. R.↗
Inundation and Sediment Supply Predict Annual but Not Centennial Carbon Accumulation in Tidal Wetlands Across Land‐Use Types
Despite growing interest in the contributions of tidal wetlands to natural climate solutions, data remain scarce on how land use affects their carbon accumulation rates (CAR). Additionally, environmental factors driving the large observed variability in CAR among sites are poorly understood. To address these knowledge gaps, we measured short-term (∼1 year) and long-term (∼100 years) CAR using feldspar marker horizons, 210 Pb profiles, and surface elevation tables from 39 sites in seven estuaries in Oregon and Washington, USA. Sites varied in wetland type (tidal marsh, tidal swamp, nontidal pasture), land-use history (reference, restored, and disturbed), and salinity (fresh to polyhaline). Across both timescales, CAR was lowest in disturbed pastures and highest in restored marshes, reflecting patterns in sediment accretion rates. Short-term CAR exceeded long-term CAR by approximately 50% on average and was only weakly correlated with long-term CAR, with differences among hydrogeomorphic setting. Short-term CAR was well predicted by summer inundation frequency and relative sediment load, together explaining 60% of variance, whereas long-term CAR was poorly predicted by contemporary environmental conditions. These findings highlight the importance of aligning predictor and response timescales when modeling blue carbon dynamics, and reinforce the climate mitigation potential of tidal wetland restoration.
land use and land cover change↗
New constraints on Precambrian ocean composition
The Precambrian record of carbonate and evaporite sedimentation is equivocal. In contrast to most previous interpretations, it is possible that Archean, Paleoproterozoic, and to a lesser extent, Meso to Neoproterozoic seawater favored surplus abiotic carbonate precipitation, as aragonite and (hi-Mg?) calcite, in comparison to younger times. Furthermore, gypsum/anhydrite may have been only rarely precipitated prior to halite precipitation during evaporation prior to about 1.8 Ga. Two effects may have contributed to these relationships. First, sulfate concentration of seawater may have been critically low prior to about 1.9 Ga so the product mCa++ x mSO4-- would not have produced gypsum before halite, as in the Mesoproterozoic to modern ocean. Second, the bicarbonate to calcium ratio was sufficiently high so that during progressive evaporation of seawater, calcium would have been exhausted before the gypsum field was reached. The pH of the Archean and Paleoproterozoic ocean need not have been significantly different from the modern value of 8.1, even at CO2 partial pressures of a tenth of an atmosphere. Higher CO2 partial pressures require somewhat lower pH values.
NASA Discipline Exobiology↗
A high-resolution record of Late Holocene drought in the eastern Sierra Nevada (California, USA) from June Lake carbonate geochemistry
As historic drought conditions become more common in western North America, Late Quaternary hydroclimate records become vital for putting present anthropogenic conditions into a longer-term context. Here, we establish a high-resolution record of drought for the eastern Sierra Nevada (California) using lacustrine carbonates from well-dated sediment cores. We used oxygen and carbon stable-isotope ratios, combined with high-resolution scanning X-ray fluorescence counts of calcium (Ca) and titanium (Ti), to reconstruct the drought record over the last 4600 years in June Lake. We found elevated δ 18 O and δ 13 C carbonate isotope values coinciding with peaks in both total inorganic carbon and Ca/Ti, suggesting enhanced carbonate precipitation in response to evaporative concentration of lake water. At least six intervals of prolonged (centennial-scale) carbonate deposition were identified, including three pulses during the Late Holocene Dry Period (LHDP; ~3500–2000 cal yr BP), the Medieval Climate Anomaly (~1200–800 cal yr BP), and the Current Warm Period, which began around 100 cal yr BP. This record highlights the complexities of the LHDP, an interval that was more variable at June Lake than has been previously described in regional records.
54 ENVIRONMENTAL SCIENCES↗
SIMS Analysis of d18O and d13C of Carbonate Cements in Shale & Mudstone. Final report
This project has had two primary goals: 1) improving new technology for in situ microanalysis of stable isotope ratios by SIMS (secondary ion mass spectrometry) and 2) evaluating the importance of in situ analysis for studies of carbonate cements within shales of the Bakken Petroleum System. The systematic relations of stable isotope ratios provide an important tool to help resolve critical questions in geology. Stable isotope analysis of carbonate cements in shale constrain many topics of interest to DOE including: CO2 sequestration, climate change, and the genesis and quality of rock reservoirs for petroleum, natural gas, and water. However, this evidence is often preserved as fine-scale zonation, which is homogenized by conventional bulk analysis of powders. Recently, analysis of ultra-small spots in polished samples at the University of Wisconsin WiscSIMS Lab. has documented stable isotope zoning in carbonates and other diagenetic cements at smaller scales than previously possible. We have made detailed studies of oxygen and carbon isotope ratios in diagenetic cements from shales of the Bakken Formation from the Williston basin and elsewhere. The Bakken contains both reservoir and source rocks for petroleum. Hydrofracturing has greatly enhanced production of oil in these tight reservoirs. The sediments contain zoned carbonate cements with growth textures that record multiple events. The growth of carbonate (dolomite) cements has been proposed to control reservoir quality, but previous stable isotope studies of homogenized powders could not resolve individual generations of cement and this proposal remains untested. Our better characterization of the multiple growth zones in these carbonates will aid in understanding the genesis of these tight reservoirs and the production of unconventional oil and gas. This study has also developed SIMS standards for analysis of all compositions of Ca-Mg-Fe carbonate and selected Mn-carbonates and hydromagnesite. We have refined techniques for improved accuracy of SIMS stable isotope analysis, and for sub-1-micron spot sizes. We have established protocols for mapping and correlating sample analyses at micron-scale using QGIS software.
04 OIL SHALES AND TAR SANDS↗
Carbon Isotope Biogeochemistry of Methane from Anoxic Sediments
The isotopic composition of naturally occurring methane was used to constrain the tropospheric budget of that radiatively active gas. Numerous studies have shown that the isotopic composition is not constant, even for a specific source, and may vary temporally and spatially. The objective was to develop a process-level model that reproduced the seasonal variations in the C-13/C-12 composition of methane observed at the coastal site, Cape Lookout Bight, NC. Details of the mass balance are provided. Experiments and models designed to determine what factors incluence C-13/C-12 ratio of dissolved CO2 are reported. All the factors described were combined in a model that faithfully reproduces the seasonal C-13/C-12 variations observed at Cape Lookout. The model is described.
Blair, Neal E.↗