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

Abstract

The potent greenhouse gas nitrous oxide (N 2O) 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 2O from ferruginous Proterozoic seas. We empirically derived a rate law, $$\mathbb d[ N_2O] \atop {dt} $$ = 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 2+ concentrations could have sustained a sea-air flux of 100–200 Tg N 2O–N year -1, if N 2 fixation rates were near-modern and all fixed N 2 was emitted as N 2O. A 1D photochemical model was used to obtain steady-state atmospheric N 2O concentrations as a function of sea-air N 2O flux across the wide range of possible ρO 2 values (0.001–1 PAL). At 100–200 Tg N 2O–N year -1 and >0.1 PAL O 2, this model yielded low-ppmv N 2O, which would produce several degrees of greenhouse warming at 1.6 ppmv CH 4 and 320 ppmv CO 2. These results suggest that enhanced N 2O 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 2O fluxes at intermediate O 2 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 2O is unlikely to have been an important greenhouse gas if Mesoproterozoic O 2 was 0.001 PAL. Furthermore at low O 2, N 2O 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.

Authors:
 [1];  [2]; ORCiD logo [3];  [4];  [4];  [5]; ORCiD logo [2]
  1. Georgia Inst. of Technology, Atlanta, GA (United States); Pennsylvania State Univ., University Park, PA (United States)
  2. Georgia Inst. of Technology, Atlanta, GA (United States)
  3. Pennsylvania State Univ., University Park, PA (United States)
  4. Michigan State Univ., East Lansing, MI (United States)
  5. Univ. of California, Riverside, CA (United States)
Publication Date:
Research Org.:
Great Lakes Bioenergy Research Center, Madison, WI (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23)
OSTI Identifier:
1506446
Alternate Identifier(s):
OSTI ID: 1465903
Grant/Contract Number:  
[SC0018409; FC02-07ER64494]
Resource Type:
Accepted Manuscript
Journal Name:
Geobiology
Additional Journal Information:
[ Journal Volume: 16; Journal Issue: 6]; Journal ID: ISSN 1472-4677
Publisher:
Wiliey
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES

Citation Formats

Stanton, Chloe L., Reinhard, Christopher T., Kasting, James F., Ostrom, Nathaniel E., Haslun, Joshua A., Lyons, Timothy W., and Glass, Jennifer B. Nitrous oxide from chemodenitrification: A possible missing link in the Proterozoic greenhouse and the evolution of aerobic respiration. United States: N. p., 2018. Web. doi:10.1111/gbi.12311.
Stanton, Chloe L., Reinhard, Christopher T., Kasting, James F., Ostrom, Nathaniel E., Haslun, Joshua A., Lyons, Timothy W., & Glass, Jennifer B. Nitrous oxide from chemodenitrification: A possible missing link in the Proterozoic greenhouse and the evolution of aerobic respiration. United States. doi:10.1111/gbi.12311.
Stanton, Chloe L., Reinhard, Christopher T., Kasting, James F., Ostrom, Nathaniel E., Haslun, Joshua A., Lyons, Timothy W., and Glass, Jennifer B. Wed . "Nitrous oxide from chemodenitrification: A possible missing link in the Proterozoic greenhouse and the evolution of aerobic respiration". United States. doi:10.1111/gbi.12311. https://www.osti.gov/servlets/purl/1506446.
@article{osti_1506446,
title = {Nitrous oxide from chemodenitrification: A possible missing link in the Proterozoic greenhouse and the evolution of aerobic respiration},
author = {Stanton, Chloe L. and Reinhard, Christopher T. and Kasting, James F. and Ostrom, Nathaniel E. and Haslun, Joshua A. and Lyons, Timothy W. and Glass, Jennifer B.},
abstractNote = {The potent greenhouse gas nitrous oxide (N2O) 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 N2O from ferruginous Proterozoic seas. We empirically derived a rate law, $\mathbb d[ N_2O] \atop {dt} $ = 7.2 × 10-5[Fe2+]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 Fe2+ concentrations could have sustained a sea-air flux of 100–200 Tg N2O–N year-1, if N2 fixation rates were near-modern and all fixed N2 was emitted as N2O. A 1D photochemical model was used to obtain steady-state atmospheric N2O concentrations as a function of sea-air N2O flux across the wide range of possible ρO2 values (0.001–1 PAL). At 100–200 Tg N2O–N year-1 and >0.1 PAL O2, this model yielded low-ppmv N2O, which would produce several degrees of greenhouse warming at 1.6 ppmv CH4 and 320 ppmv CO2. These results suggest that enhanced N2O 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 N2O fluxes at intermediate O2 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, N2O is unlikely to have been an important greenhouse gas if Mesoproterozoic O2 was 0.001 PAL. Furthermore at low O2, N2O 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.},
doi = {10.1111/gbi.12311},
journal = {Geobiology},
number = [6],
volume = [16],
place = {United States},
year = {2018},
month = {8}
}

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