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NASA NTRS1984

Tropospheric methane in the mid-latitudes of the Southern Hemisphere

More than 800 methane concentration measurements have been obtained for the Southern Hemisphere's troposphere over the September 1980-March 1983 period. Concentrations are noted to increase throughout the troposphere during the study period, adding further support to the view that CH4 concentrations are currently increasing on a global scale. In the surface methane data, a seasonal cycle with a peak-to-peak amplitude of 28 ppbv is found. Maxima and minima are on September-October and March, respectively. The phase and amplitude of the cycle are qualitatively consistent with the concept that the major sink for methane is oxidation by hydroxyl radicals. Evidence is found for a positive vertical gradient in methane content.

Fraser, P. J.↗

NASA NTRS1994

Methane emission by bubbling from Gatun Lake, Panama

We studied methane emission by bubbling from Gatun Lake, Panama, at water depths of less than 1 m to about 10 m. Gas bubbles were collected in floating traps deployed during 12- to 60-hour observation periods. Comparison of floating traps and floating chambers showed that about 98% of methane emission occurred by bubbling and only 2% occurred by diffusion. Average methane concentration of bubbles at our sites varied from 67% to 77%. Methane emission by bubbling occurred episodically, with greatest rates primarily between the hours of 0800 and 1400 LT. Events appear to be triggered by wind. The flux of methane associated with bubbling was strongly anticorrelated with water depth. Seasonal changes in water depth caused seasonal variation of methane emission. Bubble methane fluxes through the lake surface into the atmosphere measured during 24-hour intervals were least (10-200 mg/m2/d) at deeper sites (greater than 7 m) and greatest (300-2000 mg/m2/d) at shallow sites (less than 2 m).

Keller, Michael↗

DOE OSTI2020

Photoacoustic methane gas analyser based on a 3.3-μm optical parametric oscillator

We demonstrate a bench-scale prototype of a photoacoustic (PA) methane gas analyser that takes advantage of an optical parametric oscillator (OPO) based on a fan-out MgO : PPLN structure and resonant differential PA detector. The OPO emits in a repetitively pulsed mode (∼1750 Hz) at an idler wavelength of ∼3.3 μm with an average power of ∼40 – 50 mW. Using the prototype laser PA gas analyser, we experimentally demonstrate the feasibility of measuring the background methane concentration in air (∼2 – 3 ppm of CH{sub 4}). The threshold sensitivity of the PA gas analyser (1σ) is determined to be ∼ 49 ppb of CH{sub 4}. (paper)

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

NASA NTRS1984

Atmospheric methane in the recent and ancient atmospheres Concentrations, trends, and interhemispheric gradient

Rasmussen and Khalil (1981) have shown that the concentration of methane is increasing in the earth's atmosphere. A continuing increase of methane may perturb the global environment in the future by warming the earth and leading to more ozone and carbon monoxide in the atmosphere. It appears that the present concentration of methane may be more than twice as high as the natural levels of 150 years ago. An analysis of air bubbles buried long ago in polar ice makes it possible to deduce the concentrations of methane in the old and ancient atmospheres. The present investigation is concerned with the results of an analysis of more than 80 ice core samples, taking into account both polar regions of the earth. The samples range in age from about 100 to nearly 3000 years old. It is found that the concentration of methane started changing significantly about 150 years ago. These findings suggest that the increase of methane is probably indirectly caused by the rapid increase of human population.

Rasmussen, R. A.↗

DOE OSTI2022

Age and chemistry of dissolved organic carbon reveal enhanced leaching of ancient labile carbon at the permafrost thaw zone

Abstract. Climate change will alter the balance between frozen and thawed conditions in Arctic systems. Increased temperatures will make the extensive northern permafrost carbon stock vulnerable to decomposition and translocation. Production, cycling, and transport of dissolved organic carbon (DOC) are crucial processes for high-latitude ecosystem carbon loss that result in considerable export off the Arctic landscape. To identify where and under what conditions permafrost DOC is mobilized in an Arctic headwater catchment, we measured radiocarbon (14C) of DOC and assessed DOC composition with ultraviolet–visible spectroscopy (UV–Vis) of surface waters and shallow and deep subsurface porewaters from 17 drainages in the Barrow Environmental Observatory in Alaska. Samples were collected in July and September 2013 to assess changes in age and chemistry of DOC over time. DOC age was highly variable ranging from modern (19 ‰ Δ14C) to approximately 7000 BP (−583 ‰ Δ14C). DOC age increased with depth, over the summer as the active layer deepened, and with increasing drainage size. DOC quality indicators reflected a DOC source rich in high molecular-weight and aromatic compounds, characteristics consistent with vegetation-derived organic matter that had undergone little microbial processing, throughout the summer and a weak relationship with DOC age. In deep porewaters, DOC age was also correlated with several biogeochemical indicators (including dissolved methane concentration, δ13C, and the apparent fractionation factor), suggesting a coupling between carbon and redox biogeochemistry influencing methane production. In the drained thawed lake basins included in this study, DOC concentrations and contributions of vegetation-derived organic matter declined with increasing basin age. The weak relationship between DOC age and chemistry and consistency in DOC chemical indicators over the summer suggest a high lability of old DOC released by thawing permafrost.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS1990

Consumption of atmospheric methane by tundra soils

The results of field and laboratory experiments on methane consumption by tundra soils are reported. For methane concentrations ranging from below to well above ambient, moist soils are found to consume methane rapidly; in nonwaterlogged soils, equilibration with atmospheric methane is fast relative to microbial oxidation. It is concluded that lowering of the water table in tundra as a resulting from a warmer, drier climate will decrease methane fluxes and could cause these areas to provide negative feedback for atmospheric methane.

Whalen, S. C.↗

DOE OSTI2025

Spatial evidence of cryptic methane cycling and methylotrophic metabolisms along a land–ocean transect in salt marsh sediment

Methylotrophic methanogenesis in the sulfate-rich zone of coastal and marine sediments couples with anaerobic oxidation of methane (AOM), forming the cryptic methane cycle. This study provides evidence of cryptic methane cycling in the sulfate-rich zone across a land–ocean transect of four stations–two brackish, one marine, and one hypersaline–within the Carpinteria Salt Marsh Reserve (CSMR), southern California, USA. Samples from the top 20 cm of sediment from the transect were analyzed through geochemical and molecular (16S rRNA) techniques, in-vitro methanogenesis incubations, and radiotracer incubations utilizing 35 S-SO 4 , 14 C-mono-methylamine, and 14 C-CH 4 . Sediment methane concentrations were consistently low (3 to 28 µM) at all stations, except for the marine station, where methane increased with depth reaching 665 µM. Methanogenesis from mono-methylamine was detected throughout the sediment at all stations with estimated CH 4 production rates in the sub-nanomolar to nanomolar range per cm 3 sediment and day. 16S rRNA analysis identified methanogenic archaea (Methanosarcinaceae, Methanomassiliicoccales, and Methanonatronarchaeacea) capable of producing methane from methylamines in sediment where methylotrophic methanogenesis was found to be active. Metabolomic analysis of porewater showed mono-methylamine was mostly undetectable (<3 µM) or present in trace amounts (<10 µM) suggesting rapid metabolic turnover. In-vitro methanogenesis incubations of natural sediment showed no linear methane buildup, suggesting a process limiting methane emissions. AOM activity, measured with 14 C-CH 4 , overlapped with methanogenesis from mono-methylamine activity at all stations, with rates ranging from 0.03 to 19.4 nmol cm −3 d −1 . Geochemical porewater analysis showed the CSMR sediments are rich in sulfate and iron. Porewater sulfate concentrations (9–91 mM) were non-limiting across the transect, supporting sulfate reduction activity (1.5–2,506 nmol cm −3 d −1 ). Porewater sulfide and iron (II) profiles indicated that the sediment transitioned from a predominantly iron-reducing environment at the two brackish stations to a predominantly sulfate-reducing environment at the marine and hypersaline stations, which coincided with the presence of phyla (Desulfobacterota) involved in these processes. AOM activity overlapped with sulfate reduction and porewater iron (II) concentrations suggesting that AOM is likely coupled to sulfate and possibly iron reduction at all stations. However, 16S rRNA analysis identified anaerobic methanotrophs (ANME-2) only at the marine and hypersaline stations while putative methanogens were found in sediment across all stations. In one sediment horizon at the marine station, methanogen families (Methanosarcinaceae, Methanosaetaceae, Methanomassiliicoccales, and Methanoregulaceae) and ANME 2a,2b, and 2c groups were found together. Collectively, our data suggest that at the brackish stations methanogens alone may be involved in cryptic methane cycling, while at the marine and hypersaline stations both groups may be involved in the process. Differences in rate constants from incubations with 14 C-labeled methane and mono-methylamine suggest a non-methanogenic process oxidizing mono-methylamine to inorganic carbon, likely mediated by sulfate-reducing bacteria. Understanding the potential competition of sulfate reducers with methanogens for mono-methylamine needs further investigation as it might be another important process responsible for low methane emissions in salt marshes.

Anaerobic oxidation of methane↗

NASA NTRS1982

Sources of atmospheric methane from coastal marine wetlands

Biological methanogenesis in wetlands is believed to be one of the major sources of global tropospheric methane. The present paper reports measurements of methane distribution in the soils, sediments, water and vegetation of coastal marine wetlands. Measurements, carried out in the salt marshes Bay Tree Creek in Virginia and Panacea in northwest Florida, reveal methane concentrations in soils and sediments to vary with depth below the surface and with soil temperature. The fluxes of methane from marsh soils to the atmosphere at the soil-air interface are estimated to range from -0.00067 g CH4/sq m per day (methane sink) to 0.024 g CH4/sq m per day, with an average value of 0.0066 g CH4/sq m per day. Data also demonstrate the important role of tidal waters percolating through marsh soils in removing methane from the soils and releasing it to the atmosphere. The information obtained, together with previous studies, provides a framework for the design of a program based on in situ and remote sensing measurements to study the global methane cycle.

Harriss, R. C.↗

NASA NTRS1983

Investigation of the applicability of using the triple redundant hydrogen sensor for methane sensing

Application specifications for the methane sensor were assembled and design guidelines, development goals and evaluation criteria were formulated. This was done to provide a framework to evaluate sensor performance and any design adjustments to the preprototype sensor that could be required to provide methane sensitivity. Good response to hydrogen was experimentally established for four hydrogen sensor elements to be later evaluated for methane response. Prior results were assembled and analyzed for other prototype hydrogen sensor performance parameters to form a comparison base. The four sensor elements previously shown to have good hydrogen response were experimentally evaluated for methane response in 2.5% methane-in-air. No response was obtained for any of the elements, despite the high methane concentration used (50% of the Lower Flammability Limit). It was concluded that the preprototype sensing elements were insensitive to methane and were hydrogen specific. Alternative sensor operating conditions and hardware design changes were considered to provide methane sensitivity to the preprototype sensor, including a variety of different methane sensing techniques. Minor changes to the existing sensor elements, sensor geometry and operating conditions will not make the preprototype hydrogen sensor respond to methane. New sensor elements that will provide methane and hydrogen sensitivity require replacement of the existing thermistor type elements. Some hydrogen sensing characteristics of the modified sensor will be compromised (larger in situ calibration gas volume and H2 nonspecificity). The preprototype hydrogen sensor should be retained for hydrogen monitoring and a separate methane sensor should be developed.

Lantz, J. B.↗

NASA NTRS2010

Trace Gas Measurements on Mars and Earth Using Optical Parametric Generation

Trace gases and their isotopic ratios in planetary atmospheres offer important but subtle clues as to the origins of a planet's atmosphere, hydrology, geology, and potential for biology. An orbiting laser remote sensing instrument is capable of measuring trace gases on a global scale with unprecedented accuracy, and higher spatial resolution that can be obtained by passive instruments. We have developed an active sensing instrument for the remote measurement of trace gases in planetary atmospheres (including Earth). The technique uses widely tunable, seeded optical parametric generation (OPG) to measure methane, CO2, water vapor, and other trace gases in the near and mid-infrared spectral regions. Methane is a strong greenhouse gas on Earth and it is also a potential biogenic marker on Mars and other planets. Methane in the Earth's atmosphere survives for a shorter time than CO2 but its impact on climate change can be larger than CO2. Methane levels have remained relatively constant over the last decade around 1.78 parts per million (ppm) but recent observations indicate that methane levels may be on the rise. Increasing methane concentrations may trigger a positive feedback loop and a subsequent runaway greenhouse effect, where increasing temperatures result in increasing methane levels. The NRC Decadal Survey recognized the importance of global observations of greenhouse gases and called for simultaneous CH4, CO, and CO2 measurements but also underlined the technological limitations for these observations. For Mars, methane measurements are of great interest because of its potential as a strong biogenic marker. A remote sensing instrument that can measure day and night over all seasons and latitudes can identify and localize sources of biogenic gas plumes produced by subsurface chemistry or biology, and aid in the search for extra-terrestrial life. It can identify the dynamics of methane generation over time and latitude and identify future lander mission sites for more detailed in-situ analysis. In this paper we report on remote sensing measurements of methane using a high peak power, widely tunable optical parametric generator (OPG) operating at 3.3 micron and 1.65 micron. The OPG is pumped by a passively q-switched single frequency laser (3ns, 5KHz, 50uJ) and seeded by a diode laser. The spectral width of both signal and idler of seeded OPG is nearly Fourier transform limited. The output of seeded OPG is single frequency with high spectral purity and is widely tunable. Both 1650 nm and 3300 nm can be generated with a conversion efficiency of more than 30%. We have demonstrated detection of methane at 3274 nm and 1650 nm in a cell and also performed open path atmospheric measurements of methane at the same wavelengths. Finally, we were able to demonstrate simultaneous detection of methane at 3270.4 nm and CO2 at 1578.2 nm. In this paper we will discuss the OPG performance and atmospheric open path measurement results.

Numata, Kenji↗

NASA NTRS2021

Half of global methane emissions come from highly variable aquatic ecosystem sources

Atmospheric methane is a potent greenhouse gas that plays a major role in controlling the Earth’s climate. The causes of the renewed increase of methane concentration since 2007 are uncertain given the multiple sources and complex biogeochemistry. Here, we present a metadata analysis of methane fluxes from all major natural, impacted and human-made aquatic ecosystems. Our revised bottom-up global aquatic methane emissions combine diffusive, ebullitive and/or plant-mediated fluxes from 15 aquatic ecosystems. We emphasize the high variability of methane fluxes within and between aquatic ecosystems and a positively skewed distribution of empirical data, making global estimates sensitive to statistical assumptions and sampling design. We find aquatic ecosystems contribute (median) 41% or (mean) 53% of total global methane emissions from anthropogenic and natural sources. We show that methane emissions increase from natural to impacted aquatic ecosystems and from coastal to freshwater ecosystems. We argue that aquatic emissions will probably increase due to urbanization, eutrophication and positive climate feedbacks and suggest changes in land-use management as potential mitigation strategies to reduce aquatic methane emissions.

aquatic ecosystem↗

NASA NTRS2020

Exploring a Potentially Significant New(?) Mechanism for Methane Generation on Mars

An unexplored mechanism for methane production on Mars is presented here. Meteor showers have been hypothesized [1] as an explanation for episodic martian methane events [2-7], as the timing of meteor showers consistently correlates with the episodic methane events. The hypothesis [1] relied on production of methane via UV photolysis of extraterrestrial carbonaceous material [8,9] following dissemination of material into the martian atmosphere and onto the surface. Recently, new insights have emerged about an overlooked mechanism for methane production – plasma methanation [10,11] of martian atmospheric CO2 in meteor plasma. This mechanism can generate methane in addition to that produced by the previously explored methods of direct thermal evolution and UV photolysis, adding to the total methane budget produced through meteor infall. It also delivers methane in a rapid manner consistent with past observations of episodic methane “plumes” on Mars, and at altitudes where methane is rapidly removed afterwards. Methane produced by plasma methanation occurs at high altitude, which matches observations made on Mars where measurements collected through the full thickness of the martian atmosphere are of consistently higher methane concentrations (>10 ppbv [2-6]) than those recorded on the surface by the Mars Science Laboratory (MSL) rover (<10 ppbv [7]). High-altitude methane should be detected by the ESA Trace Gas Orbiter (TGO) which has not noted any methane to date. This result is puzzling regardless of the source of methane, but may be explained by the random nature of meteor shower outbursts – a significant infall may simply not have occurred (yet) during the ~3-Earth-year period of TGO observations.

Fries, M.↗

NASA NTRS1985

Methane emissions to the atmosphere through aquatic plants

The movement of methane (CH4) from anaerobic sediments through the leaves, stems, and flowers of aquatic plants and into the atmosphere was found to provide a significant pathway for the emission of CH4 from the aquatic substrates of flooded wetlands. Methane concentrations well above the surrounding ambient air levels were found in the mesophyll of 16 varies of aquatic plants and are attributed to transpiration, diffusion, and pressure-induced flow of gaseous CH4 from the roots when they are embedded in CH4-saturated anaerobic sediments. Methane emissions from the emergent parts of aquatic plants were measured using floating chamber techniques and by enclosing the plants in polyethylene bags of known volume. Concentration changes were monitored in the trapped air using syringes and gas chromatographic techniques. Vertical profiles of dissolved CH4 in sediment pore water surrounding the aquatic plants' rhizomes were obtained using an interstitial sampling technique. Methane emissions from the aquatic plants studied varied from 14.8 mg CH4/d to levels too low to be detectable. Rooted and unrooted freshwater aquatic plants were studied as well as saltwater and brackish water plants. Included in the experiment is detailed set of measurements on CH4 emissions from the common cattail (Typha latifolia). This paper illustrates that aquatic plants play an important gas exchange role in the C cycle between wetlands and the atmosphere.

Sebacher, D. I.↗

NASA NTRS1988

Laboratory studies of irradiated nitrogen-methane mixtures - Applications to Triton

The characteristics of the near-IR spectrum of Triton is addressed in view of 0.8-2.5 micron laboratory transmission spectra obtained for methane dissolved in liquid nitrogen. It is found that, for methane concentrations greater than 3 percent of the saturation value, the collision-induced, 2.152-micron first-overtone band of molecular nitrogen is overshadowed by the methane band centered at 2.3 microns. While gamma-radiolysis of nitrogen-methane mixtures generates an unstable precipitate whose yellowish color is qualitatively similar to the yellow color of Triton, no specific absorption band in the precipitate can be unambiguously identified on Triton.

Piscitelli, J. R.↗

NASA NTRS2021

Overview of Dragonfly Entry Aerosciences Measurements (DrEAM)

NASA Ames Research Center (ARC) leads the Dragonfly Entry Aerosciences Measurements (DrEAM) project, which is an aeroshell instrumentation suite on the Dragonfly mission that fulfills the Engineering Science Investigation requirement for the New Frontiers mission. NASA ARC is partnering with NASA Langley Research Center (LaRC) and the German Aerospace Center (DLR) to provide a comprehensive sensor suite, including a DLR-provided Data Acquisition System (DAS). DrEAM will provide key aerothermodynamic data and performance analysis for Dragonfly’s forebody and backshell Thermal Protection System (TPS). Titan’s atmosphere predominantly consists of ni-trogen (~98% by mole) with small amounts of me-thane (~2% by mole) and other trace gases. CN is a strong radiator, and is found in nonequilibrium con-centrations for Titan entry. The accurate modeling of nonequilibrium CN radiation has proven to be a diffi-cult task. Prompted by the Huygens mission, many experimental campaigns and analyses were performed to better understand the aerothermal environments experienced by the probe during Titan entry [1]. How-ever, the Huygens probe carried no heatshield instru-mentation. Therefore, the DrEAM sensor suite will sig-nificantly advance the state-of-the-art not only by documenting the environment and performance of Dragonfly’s entry system but also by making key in situ measurements in Titan’s atmosphere for the first time. Aerothermal environments and TPS response will be measured using sensors whose flight heritage is tak-en from the Mars Entry, Descent, and Landing In-strumentation 2 (MEDLI2) thermocouple plugs and the COMbined Aerothermal and Radiometer Sensor (COMARS) suite [2], with the latter supplied by DLR. The MEDLI2 project used embedded thermocouples to directly measure the in-depth TPS temperature-time history at several locations on the heat shield and backshell of the Mars 2020 entry vehicle. These tem-perature measurements, in turn, can be used to infer surface environments via an inverse analysis proce-dure analogous to that used for MEDLI. For DrEAM, the thermocouple plug subsystem will be known as Dragonfly Sensors for Aero-Thermal Reconstruction (DragSTR). On Schiaparelli, the COMARS suite in-cluded three total surface-mounted heat flux sensors, three pressure sensors, and one radiometer. For DrEAM, the COMARS package will be known as the COmbined Sensor System for Titan Atmosphere (COSSTA). Since the methane concentration in the Titan atmos-phere is directly proportional to the radiative heat flux, the COSSTA measurements will be used to reduce the current uncertainty in the methane volume fraction. Atmospheric density measurements and capsule aero-dynamic data will be obtained through the onboard Inertial Measurement Unit (IMU), supplemented by pressure transducers similar to those used by the MEDLI and MEDLI2 projects. The DrEAM pressure sensors will be known as the Dragonfly Atmospheric Flight Transducers. (DrAFT). The pressure measure-ments, when combined with data from the on-board IMU, will allow for reconstruction of such quantities as vehicle Mach number, freestream density, and atmos-pheric winds. DrAFT measurements will enhance Dragonfly trajectory reconstruction and enable a sepa-ration of the aerodynamics from the atmosphere, as was done for MEDLI [3] and is currently in process for the MEDLI2 flight data set.

EDL↗

DOE OSTI2022

The behavior of methane–water mixtures under elevated pressures from simulations using many-body potentials

Non-polarizable empirical potentials have been proven to be incapable of capturing the mixing of methane–water mixtures at elevated pressures. Although density functional theory-based ab initio simulations may circumvent this discrepancy, they are limited in terms of the relevant time and length scales associated with mixing phenomena. Here, we show that the many-body MB-nrg potential, designed to reproduce methane–water interactions with coupled cluster accuracy, successfully captures this phenomenon up to 3 GPa and 500 K with varying methane concentrations. Two-phase simulations and long time scales that are required to fully capture the mixing, affordable due to the speed and accuracy of the MBX software, are assessed. Constructing the methane–water equation of state across the phase diagram shows that the stable mixtures are denser than the sum of their parts at a given pressure and temperature. As a result, we find that many-body polarization plays a central role, enhancing the induced dipole moments of methane by 0.20 D during mixing under pressure. Overall, the mixed system adopts a denser state, which involves a significant enthalpic driving force as elucidated by a systematic many-body energy decomposition analysis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS1988

The isotopic composition of methane in polar ice cores

Air bubbles in polar ice cores indicate that about 300 years ago the atmospheric mixing ratio of methane began to increase rapidly. Today the mixing ratio is about 1.7 parts per million by volume, and, having doubled once in the past several hundred years, it will double again in the next 60 years if current rates continue. Carbon isotope ratios in methane up to 350 years in age have been measured with as little as 25 kilograms of polar ice recovered in 4-meter-long ice-core segments. The data show that: (1) in situ microbiology or chemistry has not altered the ice-core methane concentrations, and (2) that the carbon-13 to carbon-12 ratio of atmospheric CH4 in ice from 100 years and 300 years ago was about 2 per mil lower than at present. Atmospheric methane has a rich spectrum of isotopic sources: the ice-core data indicate that anthropogenic burning of the earth's biomass is the principal cause of the recent C-13H4 enrichment, although other factors may also contribute.

Craig, H.↗

DOE OSTI2023

Climate drivers alter nitrogen availability in surface peat and decouple N 2 fixation from CH 4 oxidation in the Sphagnum moss microbiome

Peat mosses (Sphagnum spp.) are keystone species in boreal peatlands, where they dominate net primary productivity and facilitate the accumulation of carbon in thick peat deposits. Sphagnum mosses harbor a diverse assemblage of microbial partners, including N 2 -fixing (diazotrophic) and CH 4 -oxidizing (methanotrophic) taxa that support ecosystem function by regulating transformations of carbon and nitrogen. In this work, we investigate the response of the Sphagnum phytobiome (plant + constituent microbiome + environment) to a gradient of experimental warming (+0°C to +9°C) and elevated CO 2 (+500 ppm) in an ombrotrophic peatland in northern Minnesota (USA). By tracking changes in carbon (CH 4 , CO 2 ) and nitrogen (NH 4 -N) cycling from the belowground environment up to Sphagnum and its associated microbiome, we identified a series of cascading impacts to the Sphagnum phytobiome triggered by warming and elevated CO 2 . Under ambient CO 2 , warming increased plant-available NH 4 -N in surface peat, excess N accumulated in Sphagnum tissue, and N 2 fixation activity decreased. Elevated CO 2 offset the effects of warming, disrupting the accumulation of N in peat and Sphagnum tissue. Methane concentrations in porewater increased with warming irrespective of CO 2 treatment, resulting in a ~10× rise in methanotrophic activity within Sphagnum from the +9°C enclosures. Warming's divergent impacts on diazotrophy and methanotrophy caused these processes to become decoupled at warmer temperatures, as evidenced by declining rates of methane-induced N 2 fixation and significant losses of keystone microbial taxa. In addition to changes in the Sphagnum microbiome, we observed ~94% mortality of Sphagnum between the +0°C and +9°C treatments, possibly due to the interactive effects of warming on N-availability and competition from vascular plant species. Collectively, these results highlight the vulnerability of the Sphagnum phytobiome to rising temperatures and atmospheric CO 2 concentrations, with significant implications for carbon and nitrogen cycling in boreal peatlands.

54 ENVIRONMENTAL SCIENCES↗