Kinetics of nitrous oxide production from hydroxylamine oxidation by birnessite in seawater

Cavazos, Amanda R.; Taillefert, Martial; Tang, Yuanzhi; Glass, Jennifer B.

doi:10.1016/j.marchem.2018.03.002

Cited by 20 publications

(15 citation statements)

References 68 publications

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“…With 10–100 pM NO (Ward & Zafiriou, ) and 0.1–300 nM Fe 2+ in modern oxyclines (Hopkinson & Barbeau, ; Kondo & Moffett, , ; Moffett, Goepfert, & Naqvi, ; Staubwasser, Schoenberg, Blanckenburg, Krüger, & Pohl, ; Yemenicioglu, Erdogan, & Tugrul, ), chemodenitrification could yield only 0.1–10 pM N 2 O day −1 , which is several orders of magnitude lower than net N 2 O production rates measured in OMZ oxyclines (1–5 nM N 2 O day −1 ; Babbin et al., ). This result is consistent with current hypotheses suggesting that the bulk of modern N 2 O production in OMZ oxyclines derives from microbial denitrification (Babbin et al., ), with possible contributions from archaeal ammonia oxidation and/or abiotic hydroxylamine oxidation (Cavazos, Taillefert, Tang, & Glass, ; Santoro, Buchwald, Mcilvin, & Casciotti, ).…”

Section: Resultssupporting

confidence: 91%

“…This result is consistent with current hypotheses suggesting that the bulk of modern N 2 O production in OMZ oxyclines derives from microbial denitrification (Babbin et al, 2015), with possible contributions from archaeal ammonia oxidation and/or abiotic hydroxylamine oxidation (Cavazos, Taillefert, Tang, & Glass, 2018;Santoro, Buchwald, Mcilvin, & Casciotti, 2011…”

Section: Oxygen Minimum Zones As Mesoproterozoic Analogssupporting

confidence: 92%

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

et al. 2018

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The potent greenhouse gas nitrous oxide (N O) may have been an important constituent of Earth's atmosphere during Proterozoic (~2.5-0.5 Ga). Here, we tested the hypothesis that chemodenitrification, the rapid reduction of nitric oxide by ferrous iron, would have enhanced the flux of N O from ferruginous Proterozoic seas. We empirically derived a rate law, d N 2 O d t = 7.2 × 10 - 5 [ Fe 2 + ] 0.3 [ NO ] 1 , and measured an isotopic site preference of +16‰ for the reaction. Using this empirical rate law, and integrating across an oceanwide oxycline, we found that low nM NO and μM-low mM Fe concentrations could have sustained a sea-air flux of 100-200 Tg N O-N year , if N fixation rates were near-modern and all fixed N was emitted as N O. A 1D photochemical model was used to obtain steady-state atmospheric N O concentrations as a function of sea-air N O flux across the wide range of possible pO values (0.001-1 PAL). At 100-200 Tg N O-N year and >0.1 PAL O , this model yielded low-ppmv N O, which would produce several degrees of greenhouse warming at 1.6 ppmv CH and 320 ppmv CO . These results suggest that enhanced N O production in ferruginous seawater via a previously unconsidered chemodenitrification pathway may have helped to fill a Proterozoic "greenhouse gap," reconciling an ice-free Mesoproterozoic Earth with a less luminous early Sun. A particularly notable result was that high N O fluxes at intermediate O concentrations (0.01-0.1 PAL) would have enhanced ozone screening of solar UV radiation. Due to rapid photolysis in the absence of an ozone shield, N O is unlikely to have been an important greenhouse gas if Mesoproterozoic O was 0.001 PAL. At low O , N O might have played a more important role as life's primary terminal electron acceptor during the transition from an anoxic to oxic surface Earth, and correspondingly, from anaerobic to aerobic metabolisms.

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Section: Resultssupporting

confidence: 91%

Section: Oxygen Minimum Zones As Mesoproterozoic Analogssupporting

confidence: 92%

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

et al. 2018

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“…Manganese oxides play an important role in global biogeochemical cycles due to their high oxidation state and reactive surface (Hansel et al 2015;Heil et al 2015;Hansel 2017;Cavazos et al 2018). Additionally, Mn(III/IV)O x have important roles in remediation of heavy metals and organics (Remucal and Ginder-Vogel 2014).…”

Section: Discussionmentioning

confidence: 99%

“…Thaumarchaeota use hydroxylamine (NH 2 OH) as the intermediate during ammonia oxidation (Vajrala et al 2013) and NH 2 OH has been detected in coastal waters during periods of high rates of nitrification (Butler et al 1987(Butler et al , 1988Schweiger et al 2007). Our previous research has shown that NH 2 OH reacts rapidly in seawater with MnO 2 , with near-complete conversion to the potent greenhouse gas nitrous oxide (Cavazos et al 2018). We hypothesize that the high flux of nitrous oxide emissions from coastal waters, including the Louisiana Shelf (Walker et al 2010;Kim 2018), may be at least partially due to coupled biotic-abiotic reactions between Mn(III/IV)O x particles and reactive intermediates in nitrogen cycle, such as hydroxylamine similar to reactions in soils (Rue et al 2018).…”

Section: Discussionmentioning

confidence: 99%

Simul‐staining manganese oxides and microbial cells

Cavazos

Glass

2020

Limnology & Ocean Methods

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Manganese oxide minerals (Mn(III/IV)Ox) are ubiquitous in natural environments and interactions between Mn(III/IV)Ox and microbes play important roles in biogeochemical cycles. Current techniques for determining the spatial distribution of microbes with Mn(III/IV)Ox include electron microscopy and synchrotron radiation analyses. However, these techniques may not be readily available in most laboratories or may be cost prohibitive. Here we present a rapid, cost‐effective “simul‐staining” method for imaging particulate Mn(III/IV)Ox and cells on the same filter using epifluorescence microscopy with differential interference contrast (DIC) capability as a prescreening tool before higher resolution and/or more time‐intensive analyses. This method uses leucoberbelin blue (LBB) dye, which turns blue when oxidized by particulate Mn(III/IV)Ox on filters, and the fluorescent nucleic acid stain, SYBR Green, which fluoresces when bound to nucleic acids. First, the DIC configuration is used to locate blue “haloes” of oxidized LBB around Mn(III/IV)Ox particles. Second, a filter set that excites dyes with blue light and emits green fluorescence is used to image SYBR Green bound to nucleic acids in cells. Third, ImageJ is used for image analysis to associate Mn(III/IV)Ox particles and microbes. We demonstrate that this simul‐staining is suitable for laboratory cultures of manganese‐oxidizing bacteria as well as environmental samples from a marine oxycline.

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“…8 Birnessite has the function of catalyzing water oxidation, its low price and environmental protection, so it attracts much attention from researchers. [9][10][11] However, low conductivity and poor cycle performance limit its application in the eld of water oxidation. 12,13 Metalloporphyrin compounds have a planar macrocyclic structure, excellent optical and electrical properties, and light and heat stability, making it an important application prospect in many elds, especially in the eld of biomimetic catalysis.…”

Section: Introductionmentioning

confidence: 99%

A sandwich-type catalytic composite reassembled with a birnessite layer and metalloporphyrin as a water oxidation catalyst

et al. 2019

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Kinetics of nitrous oxide production from hydroxylamine oxidation by birnessite in seawater

Cited by 20 publications

References 68 publications

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

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

Simul‐staining manganese oxides and microbial cells

A sandwich-type catalytic composite reassembled with a birnessite layer and metalloporphyrin as a water oxidation catalyst

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