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The work accomplished under NASA Grant NAG5-6722 was very successful. Our lab was able to document the occurrence and distribution of evaporite-to-carbonate transitions in several basins during Precambrian time, to help constrain the long-term chemical evolution of seawater.
Compilations have been made of sulfate reduction rates and oxic respiration rates over the entire range of marine sedimentation rates, and sedimentary environments, including several euxinic sites. These data show, consistent with the findings of Jorgensen (1982, Nature, 296, 643-645), that sulfate reduction and oxic respiration oxidize equal amounts of organic carbon in nearshore sediments. As sedimentation rates decrease, oxic respiration, becomes progressively more important, and in deep-sea sediments 100-1000 times more organic carbon is oxidized by oxic respiration than by sulfate reduction. By contrast, nearly as much organic carbon is oxidized by sulfate reduction in euxinic sediments as is oxidized by the sum of sulfate reduction and oxic respiration in normal marine sediments of similar deposition rate. This observation appears at odds with the enhanced preservation of organic carbon observed in euxinic sediments. However, only small reductions in (depth-integrated) organic carbon decomposition rates (compared to normal marine) are required to give both high organic carbon concentrations and enhanced carbon preservation in euxinic sediments. Lower rates of organic carbon decomposition (if only by subtle amounts) are explained by the diminished ability of anaerobic bacteria to oxidize the full suite of sedimentary organic compounds.
The pentacyclic triterpene 17 beta(H),21 beta(H)-hop-22(29)-ene (diploptene) occurs in sediments throughout the Columbia River drainage basin and off the southern coast of Washington state in concentrations comparable to long-chain plantwax n-alkanes. The same relationship is evident for diploptene and long-chain n-alkanes in soils from the Willamette Valley. Microorganisms indigenous to soils and soil erosion are indicated as the biological source and physical process, respectively, for diploptene in coastal sediments. Similarity between the stable carbon isotopic composition (delta 13CPDB) of diploptene isolated from soil in the Willamette Valley (-31.2 +/- 0.3%) and from sediments deposited throughout the Washington coastal environment (-31.2 +/- 0.5%) supports this argument. Values of delta for diploptene in river sediments are variable and 8-17% lighter, indicating that an additional biological source such as methane-oxidizing bacteria makes a significant contribution to the diploptene record in river sediments. Selective biodegradation resulting from a difference in the physicochemical association within eroded particles can explain the absence of the more-13C-depleted form of diploptene in Washington coastal sediments, but this mechanism remains unproven.
The organic matter that escapes decomposition is buried and preserved in marine sediments, with much debate as to whether the amount depends on bottom-water O2 concentration. One group argues that decomposition is more efficient with O2, and hence, organic carbon will be preferentially oxidized in its presence, and preserved in its absence. Another group argues that the kinetics of organic matter decomposition are similar in the presence and absence of O2, and there should be no influence of O2 on preservation. A compilation of carbon preservation shows that both groups are right, depending on the circumstances of deposition. At high rates of deposition, such as near continental margins, little difference in preservation is found with varying bottom-water O2. It is important that most carbon in these sediments decomposes by anaerobic pathways regardless of bottom-water O2. Hence, little influence of bottom-water O2 on preservation would, in fact, be expected. As sedimentation rate drops, sediments deposited under oxygenated bottom water become progressively more aerobic, while euxinic sediments remain anaerobic. Under these circumstances, the relative efficiencies of aerobic and anaerobic decomposition could affect preservation. Indeed, enhanced preservation is observed in low-O2 and euxinic environments. To explore in detail the factors contributing to this enhanced carbon preservation, aspects of the biochemistries of the aerobic and anaerobic process are reviewed. Other potential influences on preservation are also explored. Finally, a new model for organic carbon decomposition, the "pseudo-G" model, is developed. This model couples the degradation of refractory organic matter to the overall metabolic activity of the sediment, and has consequences for carbon preservation due to the mixing together of labile and refractory organic matter by bioturbation.
Profiles of oxygen, soluble and particulate manganese and iron, organic carbon and nitrogen were examined in Lake Superior sediment cores, along with the distribution and abundance of heterotrophic and manganese oxidizing bacteria. Analyses were performed using cores collected with the submersible Johnson Sea Link II. Three cores, exhibiting a range of organic carbon content, were collected from the deepest basin in Lake Superior and the north and south ends of the Caribou trough, and brought to the surface for immediate analysis. Minielectrode profiles of oxygen concentration of the three cores were carried out using a commercially available minielectrode apparatus. Oxygen depletion to less than 1% occurred within 4 cm of the surface for two of the cores, but not until approximately 15 cm for the core from the south basin of the Caribou trough. The three cores exhibited very different profiles of soluble, as well as leachable, manganese and iron, suggesting different degrees of remobilization of these metals in the sediments. Vertical profiles of viable bacteria and Mn oxidizing bacteria, determined by plating and counting, showed that aerobic (and facultatively aerobic) heterotrophic bacteria were present at the highest concentrations near the surface and decreased steadily with depth, while Mn oxidizing bacteria were concentrations primarily at and above the oxic/anoxic interface. Soluble manganese in the pore waters, along with abundant organic carbon, appeared to enhance the presence of manganese oxidizing bacteria, even below the oxic/anoxic interface. Profiles of solid-phase leachable manganese suggested a microbial role in manganese reprecipitation in these sediments.
Arctic peatlands are an important part of the global carbon cycle, accumulating atmospheric carbon as organic matter since the Late glacial. Current methods for understanding the changing efficiency of the peatland carbon sink rely on peatlands with an undisturbed stratigraphy. Here we present a method of estimating primary carbon accumulation rate from a site where permafrost processes have either vertically or horizontally translocated nearby carbon-rich sediment out of stratigraphic order. Briefly, our new algorithm estimates the probability of the age of deposition of a random increment of sediment in the core. The method assumes that if sediment age is measured at even depth increments, dates are more likely to occur during intervals of higher accumulation rate and vice versa. Multiplying estimated sedimentation rate by measured carbon density yields carbon accumulation rate. We perform this analysis at the Imnavait Creek Peatland, near the Arctic Long Term Ecological Research network site at Toolik Lake, Alaska. Using classical radiocarbon age modeling, we find unreasonably high rates of carbon accumulation at various Holocene intervals. With our new method, we find accumulation rate changes that are in improved agreement within the context of other sites throughout Alaska and the rest of the Circum-Arctic region.
Short-term imbalances in the global cycle of shallow water calcium carbonate deposition and dissolution may be responsible for much of the observed Pleistocene change in atmospheric carbon dioxide content. However, any proposed changes in the alkalinity balance of the ocean must be reconciled with the sedimentary record of deep-sea carbonates. The possible magnitude of the effect of shallow water carbonate deposition on the dissolution of pelagic carbonate can be tested using numerical simulations of the global carbon cycle. Boundary conditions can be defined by using extant shallow water carbonate accumulation data and pelagic carbonate deposition/dissolution data. On timescales of thousands of years carbonate deposition versus dissolution is rarely out of equilibrium by more than 1.5 x 10(13) mole yr-1. Results indicate that the carbonate chemistry of the ocean is rarely at equilibrium on timescales less than 10 ka. This disequilibrium is probably due to sea level-induced changes in shallow water calcium carbonate deposition/dissolution, an interpretation that does not conflict with pelagic sedimentary data from the central Pacific.
Chicxulub ejecta deposits in Belize provide the closest exposures of ejecta to the crater and the only exposures of proximal ejecta deposited in a terrestrial environment. A quarry on Albion Island in northern Belize exposes Late Cretaceous, possibly Maastrichtian, carbonate platform sediments that were folded, eroded, and subaerially weathered prior to the deposition of coarse ejecta from Chicxulub. These ejecta deposits are composed of a basal, about 1-m-thick clay and dolomite Spheroid Bed overlain by a about 15-m-thick coarse Diamictite Bed. Many and perhaps most of the clay spheroids are altered glass. Many dolomite spheroids have concentric layers and angular cores are probably of accretionary lapilli origin. A slight Ir concentration (111-152 ppt) was detected in the base of the Spheroid Bed. The Diamictite Bed contains about 10% altered glass, rare shocked quartz, 3-8 m diameter boulders and striated and polished cobbles, one with a penetrating rock chip that plastically deformed the cobble. Ejecta deposits extend to the surface at Albion and the maximum thickness in this area is not known. Ejecta deposits are exposed in several roadside quarries in the Cayo District of central Belize. The Late Cretaceous here is also represented by carbonate platform sediments. The upper surface of the carbonate platform is a highly irregular and extensively recrystallized horizon possibly representing deep karst weathering. Approximately 30 in of diamictite overlies this horizon with a texture similar to the Diamictite Bed at the Albion quarry, but with a more diverse lithology. In three locations the Cayo diamictites, contain red clay layers with abundant polished and striated limestone pebbles and cobbles called Pook's Pebbles, several of which have penetrating rock chips and ablated surfaces. We interpret the Albion Spheroid Bed as a deposit from the impact vapor plume and the Albion and Cayo diamictites as the result of a turbulent flow that contained debris derived from the ejecta curtain and local scouring. The polished, striated, and ablated Pook's Pebbles are interpreted as high altitude ballistic ejecta.
Tidal marshes globally are experiencing erosion with sea level rise. In order to adaptively plan for essential marsh preservation, we recognize the importance of the investigation of marsh archives for the perspective they provide toward resilience. Our objective in this study is to examine the relationship of tidal marsh carbon sequestration with both climate change and human impact throughout past centuries and millennia. A Hudson River marsh sediment core spanning the last 2000 years is analyzed for bulk loss on ignition (LOI), bulk density, sedimentation rate, carbon (C) and mineral flux, and x-ray fluorescence (XRF) analysis including lead, copper, titanium and potassium. We compare this record to previously established pollen and spore stratigraphy from the same site, along with an extensive macrofossil based AMS 14C chronology based upon both cores. Carbon accumulation generally follows sediment accumulation rates, which were higher than 200 g C m−2 yr−1 prior to 1500 years ago. Declines in carbon storage rate during the Medieval Warm Period (MWP) are linked to drought, fire, and charcoal, while lesser declines during the Little Ice Age (LIA) are linked to cooling and a shorter growing season. Subsequent human impact with marsh haying practices also led to carbon accumulation rate decline to 100 g C m−2 yr−1. Increases in C sequestration rates in recent decades may be attributable to nitrogen pollution of the estuary, invasive plants, and/or increased flooding, but the lack of mineral sediment threatens their stability. Ecosystem function is declining with the loss of foundational species, and the crisis is deepening for preservation of this habitat. We strongly recommend strategies for minimizing marsh loss.
In samples of the Julia Creek and Condor oil shales (Australia, Albian, and early Tertiary, respectively) etioporphyrin III is significantly depleted in C-13 (4 per mil) relative to porphyrins derived from chlorophylls. This isotopic difference suggests a large contribution from some independent source. The haem group found in cytochromes derived from microbial sources is the most likely candidate.
Sediments spanning a 5 meter section across the Cretaceous-Tertiary boundary at ODP holes 689B and 690D, Maud Rise, Wedell Sea and hole 527, Walvis Ridge, are being analyzed for shock deformation, PGE's and other trace elements (including REE's). Mineral separates from each sample were studied with optical microscopy to determine the distribution and microstructural state of quartz and feldspar present in the sediments. Samples from Maud Rise were taken of the K/T transition and at about 50 cm intervals above and below it. These samples consist of carbonate-rich sediments, with the K/T transition marked by a change from white Maastrichtian oozes to a greenish ooze with higher concentrations of altered volcanic clay and vitric ash. The Walvis Ridge site is characterized by more clay-rich sediments with average carbonate content about 60 to 70 percent. Initial results from RNAA studies indicate that iridium is present in all the Maud Rise samples in concentrations equal to or greater than 0.01 ppb (whole-rock basis). Preliminary results from optical microscopy indicate the occurrence of shock mosaicism in quartz and feldspar in all of the samples studied. The pervasiveness of shock mosaicism and presence of planar features to 2 meters from the K/T boundary indicates that a single impact or volcanic explosion 66 ma may be ruled out as responsible for the K/T event. A similar conclusion may be drawn independently from the distribution of iridium and other trace elements. Regardless of the source of the shock waves and sediment contamination, multiple events are required over a ca.0.5 my timespan; currently we favor endogenous sources.
A carbon isotope mass balance was determined for the sediments of Cape Lookout Bight, NC to constrain the carbon budgets published previously. The diffusive, ebullitive and burial fluxes of sigma CO2 and CH4, as well as the carbon isotope signatures of these fluxes, were measured. The flux-weighted isotopic signature of the remineralized carbon (-18.9 plus or minus 2.7 per mil) agreed with the isotopic composition of the remineralized organic carbon determined from the particulate organic carbon (POC) delta(C-13) profiles (-19.2 plus or minus 0.2), verifying the flux and isotopic signature estimates. The measured delta(C-13) values of the sigma CO2 and CH4 diffusive fluxes were significantly different from those calculated from porewater gradients. The differences appear to be influenced by methane oxidation at the sediment-water interface, although other potential processes cannot be excluded. The isotope mass balance provides important information concerning the locations of potential diagenetic isotope effects. Specifically, the absence of downcore change in the delta(C-13) value of the POC fraction and the identical isotopic composition of the POC and the products of remineralization indicate that no isotopic fractionation is expressed during the initial breakdown of the POC, despite its isotopically heterogeneous composition.
We have combined several different methodologies to quantify rates of organic carbon mineralization by the various electron acceptors in sediments from the coast of Denmark and Norway. Rates of NH4+ and Sigma CO2 liberation sediment incubations were used with O2 penetration depths to conclude that O2 respiration accounted for only between 3.6-17.4% of the total organic carbon oxidation. Dentrification was limited to a narrow zone just below the depth of O2 penetration, and was not a major carbon oxidation pathway. The processes of Fe reduction, Mn reduction and sulfate reduction dominated organic carbon mineralization, but their relative significance varied depending on the sediment. Where high concentrations of Mn-oxide were found (3-4 wt% Mn), only Mn reduction occurred. With lower Mn oxide concentrations more typical of coastal sediments, Fe reduction and sulfate reduction were most important and of a similar magnitude. Overall, most of the measured O2 flux into the sediment was used to oxidized reduced inorganic species and not organic carbon. We suspect that the importance of O2 respiration in many coastal sediments has been overestimated, whereas metal oxide reduction (both Fe and Mn reduction) has probably been well underestimated.
The author has identified the following significant results. Possible geologic structures in the basin sediments of Carbon County and vicinity were located by interpretation of ERTS-1 imagery. These same structures are not evident on existing conventional geologic maps of the area. Subsequent field checks confirmed much of the geologic interpretation, but revealed that two apparent closed structures identified on the ERTS-1 imagery were actually topographic pseudostructures in flat or homoclinal sediments. Stereoscopic coverage (where available) allows the interpreter to avoid such misinterpretations.
Measurements of the natural abundances of carbon isotopes were made in acetate samples isolated from the anoxic marine sediment of Cape Lookout Bight, North Carolina. The typical value of the total acetate carbon isotope ratio (delta 13C) was -16.1 +/- 0.2 per mil. The methyl and carboxyl groups were determined to be -26.4 +/- 0.3 and -6.0 +/- 0.3 per mil, respectively, for one sample. The isotopic composition of the acetate is thought to have resulted from isotopic discriminations that occurred during the cycling of that molecule. Measurements of this type, which have not been made previously in the natural environment, may provide information about the dominant microbial pathways in anoxic sediments as well as the processes that influence the carbon isotopic composition of biogenic methane from many sources.
The natural abundance C-13/C-12 ratio of methane from anoxic marine and freshwater sediments in temperate climates varies seasonally. Carbon isotopic measurements of the methanogenic precursors, acetate and dissolved inorganic carbon, from the marine sediments of Cape Lookout Bight, North Carolina were used to determine the sources of the seasonal variations at that site. Movement of the methanogenic zone over an isotopic gradient within the dissolved CO2 pool appears to be the dominant control of the methane C-13/C-12 ratio from February to June. The onset of acetoclastic methane-production is a second important controlling process during mid-summer. An apparent temperature dependence on the fractionation factor for CO2-reduction may have a significant influence on the isotopic composition of methane throughout the year.
Demand for mangrove forest resources has led to a steady decline in mangrove area over the past century. Land conversions in the form of agriculture, aquaculture and urbanization account for much of the deforestation of mangrove wetlands. However, natural processes at the transition zone between land and ocean can also rapidly change mangrove spread. In this study, we applied a robust field-based carbon inventory and new structural and temporal remote sensing techniques to quantify the magnitude and change of mangrove carbon stocks in major deltas across Africa and Asia. From 2000–2016, approximately 1.6% (12 270 ha) of the total mangrove area within these deltas disappeared, primarily through erosion and conversion to agriculture. However, the rapid expansion of mangroves in some regions during this same period resulted in new forests that were taller and more carbon-dense than the deforested areas. Because of the rapid vertical growth rates and horizontal expansion, new mangrove forests were able to offset the total carbon losses of 5 332 843 Mg C by 44%. Each hectare of new mangrove forest accounted for ∼84% to ∼160% of the aboveground carbon for each hectare of mangrove forest lost, regardless of the net change in mangrove area. Our study highlights the significance of the natural dynamics of erosion and sedimentation on carbon loss and sequestration potential for mangroves over time. Areas of naturally regenerating mangroves will have a much larger carbon sequestration potential if the rate of mangrove deforestation of taller forests is curbed.
Iron is the most important micronutrient in the ocean, but the nature and magnitude of its sources and sinks to the ocean are poorly constrained. Here we assess our understanding of the sources and sinks of iron in margin environments by synthesizing observations from the U.S. GEOTRACES GP16 Eastern Tropical Pacific Zonal Transect (EPZT) cruise near the Peru margin. GP16 observations showed elevated dissolved iron (dFe) concentrations along the margin, but a larger westward plume of dFe at slope depths (1000-3000 m) in oxygenated waters, rather than at shelf depths (100-300 m) in oxygen deficient waters. We examine the potential explanations for this unexpected observation. Multiple tracers from GP16 suggest that sediment resuspension was important at slope depths, which would lead to enhanced benthic flux of dFe above what was previously measured. The difference in the apparent persistence and penetration of shelf vs slope plumes of dFe into the interior of the ocean likely results from faster removal rates of the shelf dFe compared to slope dFe. DFe sourced from the shelf was almost entirely in the dFe(II) form, whereas dFe sourced from the slope was almost entirely in the dFe(III) form. Although benthic dFe(II) diffuses into oxygen deficient overlying waters, there is still oxidation of dFe(II), which precipitates to particulate Fe(III). In contrast, the slope plume appears to persist in a stabilized dFe(III) form. We hypothesize that sediment porewaters with moderate organic carbon delivery to sediments and shallow oxygen penetration are especially good sources of persistent dFe to the water column.