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Kai-Uwe Hinrichs

Publications and source records attributed to Kai-Uwe Hinrichs.

7 recordsLinked to original sources

Methane turnover and environmental change from Holocene biomarker records in a thermokarst lake in Arctic Alaska

Arctic lakes and wetlands contribute a substantial amount of methane to the contemporary atmosphere, yet profound knowledge gaps remain regarding the intensity and climatic control of past methane emissions from this source. In this study, we reconstruct methane turnover and environmental conditions, including estimates of mean annual and summer temperature, from a thermokarst lake (Lake Qalluuraq) on the Arctic Coastal Plain of northern Alaska for the Holocene by using source-specific lipid biomarkers preserved in a radiocarbon-dated sediment core. Our results document a more prominent role for methane in the carbon cycle when the lake basin was an emergent fen habitat between ~12,300 and ~10,000 cal yr BP, a time period closely coinciding with the Holocene Thermal Maximum (HTM) in North Alaska. Enhanced methane turnover was stimulated by relatively warm temperatures, increased moisture, nutrient supply, and primary productivity. After ~10,000 cal yr BP, a thermokarst lake with abundant submerged mosses evolved, and through the mid-Holocene temperatures were approximately 3°C cooler. Under these conditions, organic matter decomposition was attenuated, which facilitated the accumulation of submerged mosses within a shallower Lake Qalluuraq. Reduced methane assimilation into biomass during the mid-Holocene suggests that thermokarst lakes are carbon sinks during cold periods. In the late-Holocene from ~2700 cal yr BP to the most recent time, however, temperatures and carbon deposition rose and methane oxidation intensified, indicating that more rapid organic matter decomposition and enhanced methane production could amplify climate feedback via potential methane emissions in the future.

The Holocene

Nonequilibrium clumped isotope signals in microbial methane

Methane is a key component in the global carbon cycle with a wide range of anthropogenic and natural sources. Although isotopic compositions of methane have traditionally aided source identification, the abundance of its multiply-substituted “clumped” isotopologues, e.g., 13 CH 3 D, has recently emerged as a proxy for determining methane-formation temperatures; however, the impact of biological processes on methane’s clumped isotopologue signature is poorly constrained. We show that methanogenesis proceeding at relatively high rates in cattle, surface environments, and laboratory cultures exerts kinetic control on 13 CH 3 D abundances and results in anomalously elevated formation temperature estimates. We demonstrate quantitatively that H 2 availability accounts for this effect. Clumped methane thermometry can therefore provide constraints on the generation of methane in diverse settings, including continental serpentinization sites and ancient, deep groundwaters.

Science

Carbon flow from volcanic CO 2 into soil microbial communities of a wetland mofette

Effects of extremely high carbon dioxide (CO 2 ) concentrations on soil microbial communities and associated processes are largely unknown. We studied a wetland area affected by spots of subcrustal CO 2 degassing (mofettes) with focus on anaerobic autotrophic methanogenesis and acetogenesis because the pore gas phase was largely hypoxic. Compared with a reference soil, the mofette was more acidic (ΔpH ~0.8), strongly enriched in organic carbon (up to 10 times), and exhibited lower prokaryotic diversity. It was dominated by methanogens and subdivision 1Acidobacteria, which likely thrived under stable hypoxia and acidic pH. Anoxic incubations revealed enhanced formation of acetate and methane (CH 4 ) from hydrogen (H 2 ) and CO 2 consistent with elevated CH 4 and acetate levels in the mofette soil. 13 CO 2 mofette soil incubations showed high label incorporations with ~512   ng 13 C   g   (dry weight (dw)) soil −1   d −1 into the bulk soil and up to 10.7   ng 13 C   g   (dw) soil −1   d −1 into almost all analyzed bacterial lipids. Incorporation of CO 2 -derived carbon into archaeal lipids was much lower and restricted to the first 10   cm of the soil. DNA-SIP analysis revealed that acidophilic methanogens affiliated withMethanoregulaceae and hitherto unknown acetogens appeared to be involved in the chemolithoautotrophic utilization of 13 CO 2 . Subdivision 1 Acidobacteriaceae assimilated 13 CO 2 likely via anaplerotic reactions because Acidobacteriaceae are not known to harbor enzymatic pathways for autotrophic CO 2 assimilation. We conclude that CO 2 -induced geochemical changes promoted anaerobic and acidophilic organisms and altered carbon turnover in affected soils.

The ISME Journal

Carbon isotope equilibration during sulphate-limited anaerobic oxidation of methane

Collectively, marine sediments comprise the largest reservoir of methane on Earth. The flux of methane from the sea bed to the overlying water column is mitigated by the sulphate-dependent anaerobic oxidation of methane by marine microbes within a discrete sedimentary horizon termed the sulphate–methane transition zone. According to conventional isotope systematics, the biological consumption of methane leaves a residue of methane enriched in 13 C (refs 1–3). However, in many instances the methane within sulphate–methane transition zones is depleted in 13 C, consistent with the production of methane, and interpreted as evidence for the intertwined anaerobic oxidation and production of methane 4–6 . Here, we report results from experiments in which we incubated cultures of microbial methane consumers with methane and low levels of sulphate, and monitored the stable isotope composition of the methane and dissolved inorganic carbon pools over time. Residual methane became progressively enriched in 13 C at sulphate concentrations above 0.5 mM, and progressively depleted in 13 C below this threshold. We attribute the shift to 13 C depletion during the anaerobic oxidation of methane at low sulphate concentrations to the microbially mediated carbon isotope equilibration between methane and carbon dioxide. We suggest that this isotopic e ect could help to explain the 13 C-depletion of methane in subseafloor sulphate–methane transition zones.

Nature Geoscience

Evidence for microbial carbon and sulfur cycling in deeply buried ridge flank basalt

Sediment-covered basalt on the flanks of mid-ocean ridges constitutes most of Earth's oceanic crust, but the composition and metabolic function of its microbial ecosystem are largely unknown. By drilling into 3.5-million-year-old subseafloor basalt, we demonstrated the presence of methane- and sulfur-cycling microbes on the eastern flank of the Juan de Fuca Ridge. Depth horizons with functional genes indicative of methane-cycling and sulfate-reducing microorganisms are enriched in solid-phase sulfur and total organic carbon, host δ 13 C- and δ 34 S-isotopic values with a biological imprint, and show clear signs of microbial activity when incubated in the laboratory. Downcore changes in carbon and sulfur cycling show discrete geochemical intervals with chemoautotrophic δ 13 C signatures locally attenuated by heterotrophic metabolism.

Science

Reconstruction of past methane availability in an Arctic Alaska wetland indicates climate influenced methane release during the past ~12,000 years

Atmospheric contributions of methane from Arctic wetlands during the Holocene are dynamic and linked to climate oscillations. However, long-term records linking climate variability to methane availability in Arctic wetlands are lacking. We present a multi-proxy ~12,000 year paleoecological reconstruction of intermittent methane availability from a radiocarbon-dated sediment core (LQ-West) taken from a shallow tundra lake (Qalluuraq Lake) in Arctic Alaska. Specifically, stable carbon isotopic values of photosynthetic biomarkers and methane are utilized to estimate the proportional contribution of methane-derived carbon to lake-sediment-preserved benthic (chironomids) and pelagic (cladocerans) components over the last ~12,000 years. These results were compared to temperature, hydrologic, and habitat reconstructions from the same site using chironomid assemblage data, oxygen isotopes of chironomid head capsules, and radiocarbon ages of plant macrofossils. Cladoceran ephippia from ~4,000 cal year BP sediments have δ13C values that range from ~−39 to −31‰, suggesting peak methane carbon assimilation at that time. These low δ13C values coincide with an apparent decrease in effective moisture and development of a wetland that included Sphagnum subsecundum. Incorporation of methane-derived carbon by chironomids and cladocerans decreased from ~2,500 to 1,500 cal year BP, coinciding with a temperature decrease. Live-collected chironomids with a radiocarbon age of 1,640 cal year BP, and fossil chironomids from 1,500 cal year BP in the core illustrate that ‘old’ carbon has also contributed to the development of the aquatic ecosystem since ~1,500 cal year BP. The relatively low δ13C values of aquatic invertebrates (as low as −40.5‰) provide evidence of methane incorporation by lake invertebrates, and suggest intermittent climate-linked methane release from the lake throughout the Holocene.

Alaska

The stable carbon isotope biogeochemistry of acetate and other dissolved carbon species in deep subseafloor sediments at the northern Cascadia Margin

Ocean drilling has revealed the existence of vast microbial populations in the deep subseafloor, but to date little is known about their metabolic activities. To better understand the biogeochemical processes in the deep biosphere, we investigate the stable carbon isotope chemistry of acetate and other carbon-bearing metabolites in sediment pore-waters. Acetate is a key metabolite in the cycling of carbon in anoxic sediments. Its stable carbon isotopic composition provides information on the metabolic processes dominating acetate turnover in situ. This study reports our findings for a methane-rich site at the northern Cascadia Margin (NE Pacific) where Expedition 311 of the Integrated Ocean Drilling Program (IODP) sampled the upper 190 m of sediment. At Site U1329, δ 13 C values of acetate span a wide range from −46.0‰ to −11.0‰ vs. VPDB and change systematically with sediment depth. In contrast, δ 13 C values of both the bulk dissolved organic carbon (DOC) (−21.6 ± 1.3‰ vs. VPDB) and the low-molecular-weight compound lactate (−20.9 ± 1.8‰ vs. VPDB) show little variability. These species are interpreted to represent the carbon isotopic composition of fermentation products. Relative to DOC, acetate is up to 23.1‰ depleted and up to 9.1‰ enriched in 13 C. Broadly, 13 C-depletions of acetate relative to DOC indicate flux of carbon from acetogenesis into the acetate pool while 13 C-enrichments of pore-water acetate relative to DOC suggest consumption of acetate by acetoclastic methanogenesis. Isotopic relationships between acetate and lactate or DOC provide new information on the carbon flow and the presence and activity of specific functional microbial communities in distinct biogeochemical horizons of the sediment. In particular, they suggest that acetogenic CO 2 -reduction can coexist with methanogenic CO 2 -reduction, a notion contrary to the hypothesis that hydrogen levels are controlled by the thermodynamically most favorable electron-accepting process. Further, the isotopic relationship suggests a relative increase in acetate flow to acetoclastic methanogenesis with depth although its contribution to total methanogenesis is probably small. Our study demonstrates how the stable carbon isotope biogeochemistry of acetate can be used to identify pathways of microbial carbon turnover in subsurface environments. Our observations also raise new questions regarding the factors controlling acetate turnover in marine sediments.

Geochimica et Cosmochimica Acta