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Methane is a major greenhouse gas and a key component of global biogeochemical cycles. Microbial methane often deviates from isotope and isotopolog equilibrium in surface environments but approaches equilibrium in deep subsurface sediments. The origin of this near-equilibrium isotopic signature in methane, whether directly produced by methanogens or achieved through anaerobic oxidation of methane (AOM), remains uncertain. Here, we show that, in the absence of AOM, microbial methane produced from deep-sea sediments exhibits isotopolog compositions approaching thermodynamic equilibrium due to energy limitation. In contrast, microbial methane from salt marsh and thermokarst lakes exhibits significant hydrogen and clumped isotopic disequilibrium due to high free-energy availability. We propose that clumped isotopologs of methane provide a proxy for characterizing the bioenergetics of environments for methane production. Together, these observations demonstrate methane clumped isotopes as a powerful tool to better understand the relation between methane metabolisms and the energy landscape in natural environments. 

The Ediacaran Gametrail Formation of northwestern Canada chronicles the evolution of a complex carbonate ramp system in response to fluctuations in relative sea level and regional tectonic subsidence alongside exceptional global change associated with the Shuram carbon isotope excursion (CIE). Here, we use extensive outcrop exposures of the Gametrail Formation in the Wernecke Mountains of Yukon, Canada, to construct a shelf-slope transect across the Shuram CIE. Twelve stratigraphic sections of the Gametrail Formation are combined with geological mapping and a suite of geochemical analyses to develop an integrated litho-, chemo-, and sequence stratigraphic model for these strata. In the more proximal Corn/Goz Creek region, the Gametrail Formation represents a storm-dominated inner to outer ramp depositional setting, while slope depositional environments in the Nadaleen River region are dominated by hemipelagic sedimentation, turbidites, and debris flows. The magnitude of the Shuram CIE is largest in slope limestones which underwent sediment-buffered diagenesis, while the CIE is notably smaller in the inner-outer ramp dolostones which experienced fluid-buffered diagenesis. Our regional mapping identified a distinct structural panel within the shelf-slope transect that was transported ~30 km via strike-slip motion during the Mesozoic–Cenozoic Cordilleran orogeny. One location in this transported structural block contains a stromatolite reef complex with extremely negative carbon isotope values down to ~ -30‰, while the other location contains an overthickened ooid shoal complex that does not preserve the characteristic negative CIE associated with the Shuram event. These deviations from the usual expression of the Shuram CIE along the shelf-slope transect in the Wernecke Mountains, and elsewhere globally, provide useful examples for how local tectonic, stratigraphic, and/or geochemical complexities can result in unusually large or completely absent expressions of a globally recognized CIE. 

Cambrian–Devonian sedimentary rocks of the northern Canadian Cordillera record both the establishment and demise of the Great American Carbonate Bank, a widespread carbonate platform system that fringed the ancestral continental margins of North America (Laurentia). Here, we present a new examination of the deep-water Road River Group of the Richardson Mountains, Yukon, Canada, which was deposited in an intra-platformal embayment or seaway within the Great American Carbonate Bank called the Richardson trough. Eleven detailed stratigraphic sections through the Road River Group along the upper canyon of the Peel River are compiled and integrated with geological mapping, facies analysis, carbonate and organic carbon isotope chemostratigraphy, and new biostratigraphic results to formalize four new formations within the type area of the Richardson Mountains (Cronin, Mount Hare, Tetlit, and Vittrekwa). We recognize nine mixed carbonate and siliciclastic deep-water facies associations in the Road River Group and propose these strata were deposited in basin-floor to slope environments. New biostratigraphic data suggest the Road River Group spans the late Cambrian (Furongian) – Middle Devonian (Eifelian), and new chemostratigraphic data record multiple global carbon isotopic events, including the late Cambrian Steptoean positive carbon isotope excursion, the Late Ordovician Guttenberg excursion, the Silurian Aeronian, Valgu, Mulde (mid-Homerian), Ireviken (early Sheinwoodian), and Lau excursions, and the Early Devonian Klonk excursion. Together, these new data not only help clarify nomenclatural debate centered around the Road River Group, but also provide critical new sedimentological, biostratigraphic, and isotopic data for these widely distributed rocks of the northern Canadian Cordillera. 

High concentrations of barium (Ba), strontium (Sr) and radium (Ra) are present in both the liquid and suspended solid portions of wastewater produced from hydraulic fracturing. These high concentrations often require special treatment in which the solid and liquid portions are separated and then independently treated prior to disposal. The solids are typically disposed in landfills while the liquids are further treated, recycled for future hydraulic fracturing, or disposed via injection wells. Finding optimal treatment methods of both the solid and the liquid fractions requires a thorough understanding of potential Ra mobility from both the raw suspended solids and mineral precipitates formed during treatment. Using a sequential extraction procedure, we found that, without treatment, more than 50% of Ra-226 in the suspended solids was associated with soluble salts and readily exchangeable fractions. When the liquid portion of the wastewater was treated by mixing with acid mine drainage (AMD), which contained high sulfate concentrations, approximately 80–97% of the total Ra-226 in the mixture solution is found in the insoluble sulfate fraction of the precipitate. The activity of Ra-226 sequestered in the precipitated solid sulfate fractions is positively correlated with the Sr/Ba ratio of the wastewater-AMD solution. We discuss implications of these findings for effective long-term management of elevated radium in both solid and liquid wastes. 

During the last deglaciation temperatures over midcontinental North America warmed dramatically through the Bølling-Allerød, underwent a cool period associated with the Younger-Dryas and then reverted to warmer, near modern temperatures during the early Holocene. However, paleo proxy records of the hydroclimate of this period have presented divergent evidence. We reconstruct summer relative humidity (RH) across the last deglacial period using a mechanistic model of cellulose and leaf water δ 18 O and δD combined with a pollen-based temperature proxy to interpret stable isotopes of sub-fossil wood. Midcontinental RH was similar to modern conditions during the Last Glacial Maximum, progressively increased during the Bølling-Allerød, peaked during the Younger-Dryas, and declined sharply during the early Holocene. This RH record suggests deglacial summers were cooler and characterized by greater advection of moisture-laden air-masses from the Gulf of Mexico and subsequent entrainment over the mid-continent by a high-pressure system over the Laurentide ice sheet. These patterns help explain the formation of dark-colored cumulic horizons in many Great Plains paleosol sequences and the development of no-analog vegetation types common to the Midwest during the last deglacial period. Likewise, reduced early Holocene RH and precipitation correspond with a diminished glacial high-pressure system during the latter stages of ice-sheet collapse.