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Title: Estimation of isotope variation of N 2O during denitrification by Pseudomonas aureofaciens and Pseudomonas chlororaphis: implications for N 2O source apportionment

Abstract

Soil microbial processes, stimulated by agricultural fertilization, account for 90% of anthropogenic nitrous oxide (N 2O), the leading source of ozone depletion and a potent greenhouse gas. Efforts to reduce N 2O flux commonly focus on reducing fertilization rates. Management of microbial processes responsible for N 2O production may also be used to reduce N 2O emissions, but this requires knowledge of the prevailing process. To this end, stable isotopes of N 2O have been applied to differentiate N 2O produced by nitrification and denitrification. To better understand the factors contributing to isotopic variation during denitrification, we characterized the δ 15N, δ 18O and site preference (SP; the intramolecular distribution of 15N in N 2O) of N 2O produced during NO 3 - reduction by Pseudomonas chlororaphis subsp. aureofaciens and P. c. subsp. chlororaphis. The terminal product of denitrification for these two species is N 2O because they lack thegene nitrous oxide reductase, which is responsible for the reduction ofN 2O to N 2. In addition to species, treatments include delectron donor (citrate and succinate) and electron donor concentration(0.01, 0.1, 1 and 10mM) as factors. In contrast to the expectation of a Rayleigh model, all treatments exhibited curvilinear behaviour between δ 15N or δ 18O and the extent of the reaction. The curvilinear behaviour indicates that the fractionation factor changed over the course of the reaction, something that is not unexpected for a multi-step process such as denitrification. Using the derivative of the equation, we estimated that the net isotope effects ( η) vary by as much as 100‰ over the course of a single reaction, presenting challenges for using δ 15N and δ 18O as apportionment tools. In contrast, SP for denitrification was not affected by the extent of the reaction, the electron donor source or concentration, although the mean SP of N 2O produced by each species differed. Hence, SP remains a robust indicator of the origin of N 2O. To improve apportionment estimates with SP, future studies could evaluate other factors that contribute to the variation in SP.

Authors:
ORCiD logo [1];  [1];  [1];  [1]
  1. Michigan State Univ., East Lansing, MI (United States)
Publication Date:
Research Org.:
Univ. of Wisconsin, Madison, WI (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23)
OSTI Identifier:
1503313
Grant/Contract Number:  
FC02-07ER64494
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Biogeosciences (Online)
Additional Journal Information:
Journal Volume: 15; Journal Issue: 12; Journal ID: ISSN 1726-4189
Publisher:
European Geosciences Union
Country of Publication:
United States
Language:
English
Subject:
59 BASIC BIOLOGICAL SCIENCES; 54 ENVIRONMENTAL SCIENCES

Citation Formats

Haslun, Joshua A., Ostrom, Nathaniel E., Hegg, Eric L., and Ostrom, Peggy H. Estimation of isotope variation of N2O during denitrification by Pseudomonas aureofaciens and Pseudomonas chlororaphis: implications for N2O source apportionment. United States: N. p., 2018. Web. doi:10.5194/bg-15-3873-2018.
Haslun, Joshua A., Ostrom, Nathaniel E., Hegg, Eric L., & Ostrom, Peggy H. Estimation of isotope variation of N2O during denitrification by Pseudomonas aureofaciens and Pseudomonas chlororaphis: implications for N2O source apportionment. United States. doi:10.5194/bg-15-3873-2018.
Haslun, Joshua A., Ostrom, Nathaniel E., Hegg, Eric L., and Ostrom, Peggy H. Wed . "Estimation of isotope variation of N2O during denitrification by Pseudomonas aureofaciens and Pseudomonas chlororaphis: implications for N2O source apportionment". United States. doi:10.5194/bg-15-3873-2018. https://www.osti.gov/servlets/purl/1503313.
@article{osti_1503313,
title = {Estimation of isotope variation of N2O during denitrification by Pseudomonas aureofaciens and Pseudomonas chlororaphis: implications for N2O source apportionment},
author = {Haslun, Joshua A. and Ostrom, Nathaniel E. and Hegg, Eric L. and Ostrom, Peggy H.},
abstractNote = {Soil microbial processes, stimulated by agricultural fertilization, account for 90% of anthropogenic nitrous oxide (N2O), the leading source of ozone depletion and a potent greenhouse gas. Efforts to reduce N2O flux commonly focus on reducing fertilization rates. Management of microbial processes responsible for N2O production may also be used to reduce N2O emissions, but this requires knowledge of the prevailing process. To this end, stable isotopes of N2O have been applied to differentiate N2O produced by nitrification and denitrification. To better understand the factors contributing to isotopic variation during denitrification, we characterized the δ15N,δ18O and site preference (SP; the intramolecular distribution of15N in N2O) of N2O produced duringNO3- reduction by Pseudomonas chlororaphis subsp. aureofaciens and P. c. subsp. chlororaphis. The terminal product of denitrification for these two species is N2O because they lack thegene nitrous oxide reductase, which is responsible for the reduction ofN2O to N2. In addition to species, treatments include delectron donor (citrate and succinate) and electron donor concentration(0.01, 0.1, 1 and 10mM) as factors. In contrast to the expectation of a Rayleigh model, all treatments exhibited curvilinear behaviour between δ15N or δ18O and the extent of the reaction. The curvilinear behaviour indicates that the fractionation factor changed over the course of the reaction, something that is not unexpected for a multi-step process such as denitrification. Using the derivative of the equation, we estimated that the net isotope effects (η) vary by as much as 100‰ over the course of a single reaction, presenting challenges for using δ15N and δ18O as apportionment tools. In contrast, SP for denitrification was not affected by the extent of the reaction, the electron donor source or concentration, although the mean SP of N2O produced by each species differed. Hence, SP remains a robust indicator of the origin of N2O. To improve apportionment estimates with SP, future studies could evaluate other factors that contribute to the variation in SP.},
doi = {10.5194/bg-15-3873-2018},
journal = {Biogeosciences (Online)},
issn = {1726-4189},
number = 12,
volume = 15,
place = {United States},
year = {2018},
month = {6}
}

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Figures / Tables:

Figure 1. Figure 1.: δ15N, δ18O and site preference (SP) of N2O produced during denitrification of NO3 by Pseudomonas chlororaphis subsp. aureofaciens and Pseudomonas chlororaphis subsp. chlororaphis with different electron donor sources and concentrations. A larger value of [−f lnf/(1− f)], where f is the fraction of substrate remaining, represents earlier pointsmore » in the reaction. The curved relationships are of the form y = a+eb[x], where y is the isotope value, x is [−f lnf/(1−f)] and a and b are the estimated coefficients that affect the y intercept and curvilinear shape, respectively.« less

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    Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.