Nitrous oxide from chemodenitrification: A possible missing link in the Proterozoic greenhouse and the evolution of aerobic respiration

Stanton, C. L.; Reinhard, Christopher T.; Kasting, James F.; Ostrom, Nathaniel E.; Haslun, Joshua A.; Lyons, Timothy W.; Glass, Jennifer B.

doi:10.1111/gbi.12311

Cited by 49 publications

(46 citation statements)

References 135 publications

(229 reference statements)

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“…Most NO − X reached the surface in the form of HNO, which 10.1029/2018GC008082 in aqueous settings would then undergo dissociation, homologation, and decay reactions, ultimately yielding soluble NO − 2 and NO − 3 and gaseous N 2 O (Mancinelli & McKay, 1988;Summers & Khare, 2007). Stanton et al (2018) have recently demonstrated the reduction of NO to N 2 O in ferrous waters; we may speculate similar chemodenitrification to occur with NO -. It is difficult to calculate the fraction of fixed nitrogen that escapes back to the atmosphere as N 2 O, because the kinetics of these transformations have not been quantified for NO -.…”

Section: Kinetic Steady Statementioning

confidence: 85%

“…Our analysis could be most improved by better characterization of

{NO}_{X}^{-}

reaction kinetics under prebiotically relevant conditions, especially its reduction by Fe 2+ and Mn 2+ and its reduction by UV in prebiotic natural waters (e.g., the extension of studies like Stanton et al, , to

{NO}_{X}^{-}

). Studies with higher‐dimensional models could also help determine if there exist areas in the ocean which should have concentrated

{NO}_{X}^{-}

above the oceanic mean, perhaps to prebiotically relevant levels.…”

Section: Discussionmentioning

confidence: 99%

“…Irradiation by UV light in natural waters net photolyzes

{NO}_{3}^{-}

{NO}_{2}^{-}

, and

{NO}_{2}^{-}

to NO, which escapes the ocean to the atmosphere or is reduced to N 2 O (Carpenter & Nightingale, ; Fanning, ; Mack & Bolton, ; Spokes & Liss, ; Stanton et al, ):

{NO}_{3}^{-} + h ν \to {NO}_{2}^{-} + \frac{1}{2} O_{2}

{NO}_{2}^{-} + H_{2} normalO + h ν \to NO + OH + {OH}^{-}

…”

Section: Kinetic Steady Statementioning

confidence: 99%

“…Determination of these rate constants at prebiotically plausible [Fe 2+ ] (10-600 M) under early Earth conditions (e.g., anoxia) could confirm the applicability of these rate constants at lower [Fe 2+ ]. The extension of studies like Stanton et al (2018) for NO kinematics to NO − X kinematics could improve the precision and potentially accuracy of this work. (4) Measuring the rate constant of NO − X photolysis in simulated prebiotic natural waters, under irradiation by a source simulating the prebiotic UV environment in both magnitude and spectral shape, could directly verify our extrapolation from modern photolysis rates, and in particular could confirm whether the shorter-wavelength UV radiation available on early Earth would affect overall reaction rates.…”

Section: Importance Of Better Kinetic Constraintsmentioning

confidence: 99%

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Nitrogen Oxide Concentrations in Natural Waters on Early Earth

Ranjan

Todd

Rimmer

et al. 2019

Geochem Geophys Geosyst

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A key challenge in origins‐of‐life studies is estimating the abundances of species relevant to the chemical pathways proposed to have contributed to the emergence of life on early Earth. Dissolved nitrogen oxide anions ( NOX−), in particular nitrate ( NO3−) and nitrite ( NO2−), have been invoked in diverse origins‐of‐life chemistry, from the oligomerization of RNA to the emergence of protometabolism. Recent work has calculated the supply of NOX− from the prebiotic atmosphere to the ocean and reported steady state [ NOX−] to be high across all plausible parameter space. These findings rest on the assumption that NOX− is stable in natural waters unless processed at a hydrothermal vent. Here, we show that NOX− is unstable in the reducing environment of early Earth. Sinks due to ultraviolet photolysis and reactions with reduced iron (Fe2+) suppress [ NOX−] by several orders of magnitude relative to past predictions. For pH = 6.5–8 and T = 0–50 °C, we find that it is most probable that [ NOX−] <1μM in the prebiotic ocean. On the other hand, prebiotic ponds with favorable drainage characteristics may have sustained [ NOX−] ≥1μM. As on modern Earth, most NOX− on prebiotic Earth should have been present as NO3−, due to its much greater stability. These findings inform the kind of prebiotic chemistries that would have been possible on early Earth. We discuss the implications for proposed prebiotic chemistries and highlight the need for further studies of NOX− kinetics to reduce the considerable uncertainties in predicting [ NOX−] on early Earth.

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Section: Kinetic Steady Statementioning

confidence: 85%

“…Our analysis could be most improved by better characterization of

{NO}_{X}^{-}

{NO}_{X}^{-}

). Studies with higher‐dimensional models could also help determine if there exist areas in the ocean which should have concentrated

{NO}_{X}^{-}

above the oceanic mean, perhaps to prebiotically relevant levels.…”

Section: Discussionmentioning

confidence: 99%

“…Irradiation by UV light in natural waters net photolyzes

{NO}_{3}^{-}

{NO}_{2}^{-}

, and

{NO}_{2}^{-}

to NO, which escapes the ocean to the atmosphere or is reduced to N 2 O (Carpenter & Nightingale, ; Fanning, ; Mack & Bolton, ; Spokes & Liss, ; Stanton et al, ):

{NO}_{3}^{-} + h ν \to {NO}_{2}^{-} + \frac{1}{2} O_{2}

{NO}_{2}^{-} + H_{2} normalO + h ν \to NO + OH + {OH}^{-}

…”

Section: Kinetic Steady Statementioning

confidence: 99%

Section: Importance Of Better Kinetic Constraintsmentioning

confidence: 99%

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Nitrogen Oxide Concentrations in Natural Waters on Early Earth

Ranjan

Todd

Rimmer

et al. 2019

Geochem Geophys Geosyst

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“…The microbial production of greenhouse gases under ferruginous conditions has led to the suggestion that gases such as CH 4 or N 2 O could have been important in regulating early Earth's climate when solar luminosities were lower (e.g., Kasting, 2005;Stanton et al, 2018). However, biosphere models for oceanic CH 4 emissions during the Archean and Proterozoic eons generally only consider transport of CH 4 by turbulent diffusion (Olson, Reinhard, & Lyons, 2016), which favors efficient oxidation of CH 4 at an oxycline (Oswald, Jegge, et al, 2016a).…”

Section: Methane Emissions From Ancient Ferruginous Oceansmentioning

confidence: 99%

Biogeochemical and physical controls on methane fluxes from two ferruginous meromictic lakes

et al. 2019

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Meromictic lakes with anoxic bottom waters often have active methane cycles whereby methane is generally produced biogenically under anoxic conditions and oxidized in oxic surface waters prior to reaching the atmosphere. Lakes that contain dissolved ferrous iron in their deep waters (i.e., ferruginous) are rare, but valuable, as geochemical analogues of the conditions that dominated the Earth's oceans during the Precambrian when interactions between the iron and methane cycles could have shaped the greenhouse regulation of the planet's climate. Here, we explored controls on the methane fluxes from Brownie Lake and Canyon Lake, two ferruginous meromictic lakes that contain similar concentrations (max. >1 mM) of dissolved methane in their bottom waters. The order Methanobacteriales was the dominant methanogen detected in both lakes. At Brownie Lake, methanogen abundance, an increase in methane concentration with respect to depths closer to the sediment, and isotopic data suggest methanogenesis is an active process in the anoxic water column. At Canyon Lake, methanogenesis occurred primarily in the sediment. The most abundant aerobic methane‐oxidizing bacteria present in both water columns were associated with the Gammaproteobacteria, with little evidence of anaerobic methane oxidizing organisms being present or active. Direct measurements at the surface revealed a methane flux from Brownie Lake that was two orders of magnitude greater than the flux from Canyon Lake. Comparison of measured versus calculated turbulent diffusive fluxes indicates that most of the methane flux at Brownie Lake was non‐diffusive. Although the turbulent diffusive methane flux at Canyon Lake was attenuated by methane oxidizing bacteria, dissolved methane was detected in the epilimnion, suggestive of lateral transport of methane from littoral sediments. These results highlight the importance of direct measurements in estimating the total methane flux from water columns, and that non‐diffusive transport of methane may be important to consider from other ferruginous systems.

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Isotopic signatures of biotic and abiotic N₂O production and consumption in the water column of meromictic, ferruginous Lake La Cruz (Spain)

Tischer

Zopfi

Frey

et al. 2022

Limnology & Oceanography

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Lakes can be important sources of the potent greenhouse gas nitrous oxide (N 2 O) to the atmosphere, but to what extent abiotic processes may contribute to lacustrine N 2 O production remains uncertain. We assessed pathways of N 2 O production and reduction in the water column of meromictic and iron-rich Lake La Cruz, Spain, including chemodenitrification-induced N 2 O formation via the reaction of reactive nitrogen (N) (e.g., NO À2 ) with ferrous iron (Fe [II]). In the oxic waters ($8-10 m), N 2 O concentrations above atmospheric equilibrium were associated with comparatively low δ 15 N-N 2 O, high δ 15 N-NH þ 4 , and high N 2 O 15 N-site-preference (SP) values (up to $29‰), suggesting N 2 O production by nitrification. N 2 O concentrations were highest (23-33 nM) near the depth of oxygen depletion ($11-14.5 m), likely due to production by nitrifier denitrification and/or denitrification, as indicated by decreasing SP values (as low as 12‰). Further below ($14.5-17 m), N 2 O consumption was indicated by increasing SP values and a δ 18 O-vs.-δ 15 N relationship (1.8-2.9) typical for stand-alone N 2 O reduction. The coupled N-vs.-O isotope signatures thus highlight the spatial, redox-dependent separation of incomplete and complete denitrification. In incubations with sterile-filtered lake water and 15 N-labeled or unlabeled substrate, NO À 2 was reduced by Fe 2+ to N 2 O, even at low nitrite concentrations (5 μM NO À 2 ). In the water column, the spatial separation of NO À 2 and Fe(II) during our samplings appears to preclude elevated rates of chemodenitrification, but during periods of overlapping NO À 2 and Fe(II) in Lake La Cruz, and potentially in other lakes, its distinct N 2 O δ 18 Ovs.-δ 15 N relationship of $1 : 1, as experimentally determined, could help to detect it.Nitrous oxide (N 2 O) is a potent greenhouse gas and an important ozone-layer-depleting substance in the atmosphere (Wang et al. 1976;Ravishankara et al. 2009). Terrestrial ecosystems including inland waters are relevant sources of both natural and anthropogenic N 2 O, but with a high uncertainty in their contribution to global N 2 O emissions (Maavara et al. 2019). N 2 O production in these ecosystems has been attributed primarily to microbially mediated nitrogen (N)-transforming processes (Tian et al. 2020). The relative contribution of abiotic N 2 O production mechanisms is still a matter of debate, particularly in lakes.The main microbial N 2 O-producing processes are nitrification, nitrifier denitrification, and denitrification. During the first step of nitrification, where ammonia-oxidizing bacteria (AOB) and/or ammonia-oxidizing archaea (AOA) oxidize

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Nitrous oxide from chemodenitrification: A possible missing link in the Proterozoic greenhouse and the evolution of aerobic respiration

Cited by 49 publications

References 135 publications

Nitrogen Oxide Concentrations in Natural Waters on Early Earth

Nitrogen Oxide Concentrations in Natural Waters on Early Earth

Biogeochemical and physical controls on methane fluxes from two ferruginous meromictic lakes

Isotopic signatures of biotic and abiotic N₂O production and consumption in the water column of meromictic, ferruginous Lake La Cruz (Spain)

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Nitrous oxide from chemodenitrification: A possible missing link in the Proterozoic greenhouse and the evolution of aerobic respiration

Cited by 49 publications

References 135 publications

Nitrogen Oxide Concentrations in Natural Waters on Early Earth

Nitrogen Oxide Concentrations in Natural Waters on Early Earth

Biogeochemical and physical controls on methane fluxes from two ferruginous meromictic lakes

Isotopic signatures of biotic and abiotic N2O production and consumption in the water column of meromictic, ferruginous Lake La Cruz (Spain)

Contact Info

Product

Resources

About

Isotopic signatures of biotic and abiotic N₂O production and consumption in the water column of meromictic, ferruginous Lake La Cruz (Spain)