The origin of dissolved arsenic in the Ganges Delta has puzzled researchers ever since the report of widespread arsenic poisoning two decades ago. Today, microbially mediated oxidation of organic carbon is thought to drive the geochemical transformations that release arsenic from sediments, but the source of the organic carbon that fuels these processes remains controversial. At a typical site in Bangladesh, where groundwater-irrigated rice fields and constructed ponds are the main sources of groundwater recharge, we combine hydrologic and biogeochemical analyses to trace the origin of contaminated groundwater. Incubation experiments indicate that recharge from ponds contains biologically degradable organic carbon, whereas recharge from rice fields contains mainly recalcitrant organic carbon. Chemical and isotopic indicators as well as groundwater simulations suggest that recharge from ponds carries this degradable organic carbon into the shallow aquifer, and that groundwater flow, drawn by irrigation pumping, transports pond water to the depth where dissolved arsenic concentrations are greatest. Results also indicate that arsenic concentrations are low in groundwater originating from rice fields. Furthermore, solute composition in arsenic-contaminated water is consistent with that predicted using geochemical models of pond-water-aquifer-sediment interactions. We therefore suggest that the construction of ponds has influenced aquifer biogeochemistry, and that patterns of arsenic contamination in the shallow aquifer result from variations in the source of water, and the complex three-dimensional patterns of groundwater flow.
Carbon dioxide (CO 2 ), methane (CH 4 ), and nitrous oxide (N 2 O) are the greenhouse gases largely responsible for anthropogenic climate change. Natural plant and microbial metabolic processes play a major role in the global atmospheric budget of each. We have been studying ecosystem-atmosphere trace gas exchange at a sub-boreal forest in the northeastern United States for over two decades. Historically our emphasis was on turbulent fluxes of CO 2 and water vapor. In 2012 we embarked on an expanded campaign to also measure CH 4 and N 2 O. Here we present continuous tower-based measurements of the ecosystem-atmosphere exchange of CO 2 and CH 4 , recorded over the period 2012–2018 and reported at a 30-minute time step. Additionally, we describe a five-year (2012–2016) dataset of chamber-based measurements of soil fluxes of CO 2 , CH 4 , and N 2 O (2013–2016 only), conducted each year from May to November. These data can be used for process studies, for biogeochemical and land surface model validation and benchmarking, and for regional-to-global upscaling and budgeting analyses.
Forests dominate the global carbon cycle, but their role in methane (CH 4 ) biogeochemistry remains uncertain. We analyzed whole-ecosystem CH 4 fluxes from 2 years, obtained over a lowland evergreen forest in Maine, USA. Gross primary productivity provided the strongest correlation with the CH 4 flux in both years, with an additional significant effect of soil moisture in the second, drier year. This forest was a neutral to net source of CH 4 in 2011 and a small net sink in 2012. Interannual variability in the summer hydrologic cycle apparently shifts the ecosystem from being a net source to a sink for CH 4 . The small magnitude of the CH 4 fluxes and observed control or CH 4 fluxes by forest productivity and summer precipitation provide novel insight into the CH 4 cycle in this globally important forest ecosystem.
Methane (CH4), a potent greenhouse gas, is the second most important greenhouse gas contributor to climate change after carbon dioxide (CO2). The biological emissions of CH4 from wetlands are a major uncertainty in CH4 budgets. Microbial methanogenesis by Archaea is an anaerobic process accounting for most biological CH4 production in nature, yet recent observations indicate that large emissions can originate from oxygenated or frequently oxygenated wetland soil layers. To determine how oxygen (O2) can stimulate CH4 emissions, we used incubations of Sphagnum peat to demonstrate that the temporary exposure of peat to O2 can increase CH4 yields up to 2000‐fold during subsequent anoxic conditions relative to peat without O2 exposure. Geochemical (including ion cyclotron resonance mass spectrometry, X‐ray absorbance spectroscopy) and microbiome (16S rDNA amplicons, metagenomics) analyses of peat showed that higher CH4 yields of redox‐oscillated peat were due to functional shifts in the peat microbiome arising during redox oscillation that enhanced peat carbon (C) degradation. Novosphingobium species with O2‐dependent aromatic oxygenase genes increased greatly in relative abundance during the oxygenation period in redox‐oscillated peat compared to anoxic controls. Acidobacteria species were particularly important for anaerobic processing of peat C, including in the production of methanogenic substrates H2 and CO2. Higher CO2 production during the anoxic phase of redox‐oscillated peat stimulated hydrogenotrophic CH4 production by Methanobacterium species. The persistence of reduced iron (Fe(II)) during prolonged oxygenation in redox‐oscillated peat may further enhance C degradation through abiotic mechanisms (e.g., Fenton reactions). The results indicate that specific functional shifts in the peat microbiome underlie O2 enhancement of CH4 production in acidic, Sphagnum‐rich wetland soils. They also imply that understanding microbial dynamics spanning temporal and spatial redox transitions in peatlands is critical for constraining CH4 budgets; predicting feedbacks between climate change, hydrologic variability, and wetland CH4 emissions; and guiding wetland C management strategies.
We measured the carbon isotopic composition of pore water carbon dioxide from Sallie’s Fen, a New Hampshire poor fen. The isotope profiles are used in combination with a one‐dimensional diffusion–reaction model to calculate rates of methane production, oxidation and transport over an annual cycle. We show how the rates vary with depth over a seasonal cycle, with methane produced deeper during the winter months and at progressively shallower depths into the summer season. The rates of methane production, constrained by the measured δ13Cdic profiles, cannot explain high methane emission during the summer. We suggest that much of the methane produced during this time comes either from the unsaturated peat, or from the top 1–3 cm of saturated peat where episodic exchange with the atmosphere makes it invisible to our method.
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