Reassessment of the NH4NO3 thermal decomposition technique for calibration of the N2O isotopic composition

Mohn, Joachim; Gutjahr, Wilhelm; Toyoda, Sakae; Harris, Eliza; Ibraim, Erkan; Geilmann, Heike; Schleppi, Patrick; Kühn, Thomas; Lehmann, Moritz F.; Decock, Charlotte; Werner, Roland A.; Yoshida, Naohiro; Brand, Willi A.

doi:10.1002/rcm.7736

Cited by 19 publications

(27 citation statements)

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“…approx. 0 ‰-15 ‰, in agreement with the literature (Mook, 2002;Holland, 2011). We thus used only the δ 15 N-NO − 3 values for the substrate isotopic composition.…”

Section: N 2 O Source Partitioning Using Sp and δ 15 N Bulksupporting

confidence: 92%

“…The international isotope reference scale for 15 N/ 14 N is atmospheric N 2 (AIR-N 2 ) and for 18 O/ 16 O Vienna Standard Mean Ocean Water (VSMOW). Thermal decomposition of isotopically characterized ammonium nitrate (NH 4 NO 3 ) has been suggested as an approach to link the position-dependent nitrogen isotopic composition of N 2 O to AIR-N 2 (Toyoda and Yoshida, 1999;Mohn et al, 2016). The total 15 N content is usually reported as bulk 15 N content (δ 15 N bulk ) according to Eq.…”

Section: Introductionmentioning

confidence: 99%

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Attribution of N2O sources in a grassland soil with laser spectroscopy based isotopocule analysis

et al. 2019

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Nitrous oxide (N 2 O) is the primary atmospheric constituent involved in stratospheric ozone depletion and contributes strongly to changes in the climate system through a positive radiative forcing mechanism. The atmospheric abundance of N 2 O has increased from 270 ppb (parts per billion, 10 −9 mole mole −1 ) during the pre-industrial era to approx. 330 ppb in 2018. Even though it is well known that microbial processes in agricultural and natural soils are the major N 2 O source, the contribution of specific soil processes is still uncertain. The relative abundance of N 2 O isotopocules ( 14 N 14 N 16 N, 14 N 15 N 16 O, 15 N 14 N 16 O, and 14 N 14 N 18 O) carries process-specific information and thus can be used to trace production and consumption pathways. While isotope ratio mass spectroscopy (IRMS) was traditionally used for high-precision measurement of the isotopic composition of N 2 O, quantum cascade laser absorption spectroscopy (QCLAS) has been put forward as a complementary technique with the potential for on-site analysis. In recent years, pre-concentration combined with QCLAS has been presented as a technique to resolve subtle changes in ambient N 2 O isotopic composition.From the end of May until the beginning of August 2016, we investigated N 2 O emissions from an intensively managed grassland at the study site Fendt in southern Germany. In total, 612 measurements of ambient N 2 O were taken by com-bining pre-concentration with QCLAS analyses, yielding δ 15 N α , δ 15 N β , δ 18 O, and N 2 O concentration with a temporal resolution of approximately 1 h and precisions of 0.46 ‰, 0.36 ‰, 0.59 ‰, and 1.24 ppb, respectively. Soil δ 15 N-NO − 3 values and concentrations of NO − 3 and NH + 4 were measured to further constrain possible N 2 O-emitting source processes. Furthermore, the concentration footprint area of measured N 2 O was determined with a Lagrangian particle dispersion model (FLEXPART-COSMO) using local wind and turbulence observations. These simulations indicated that nighttime concentration observations were largely sensitive to local fluxes. While bacterial denitrification and nitrifier denitrification were identified as the primary N 2 O-emitting processes, N 2 O reduction to N 2 largely dictated the isotopic composition of measured N 2 O. Fungal denitrification and nitrification-derived N 2 O accounted for 34 %-42 % of total N 2 O emissions and had a clear effect on the measured isotopic source signatures. This study presents the suitability of on-site N 2 O isotopocule analysis for disentangling source and sink processes in situ and found that at the Fendt site bacterial denitrification or nitrifier denitrification is the major source for N 2 O, while N 2 O reduction acted as a major sink for soil-produced N 2 O.

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“…approx. 0 ‰-15 ‰, in agreement with the literature (Mook, 2002;Holland, 2011). We thus used only the δ 15 N-NO − 3 values for the substrate isotopic composition.…”

Section: N 2 O Source Partitioning Using Sp and δ 15 N Bulksupporting

confidence: 92%

Section: Introductionmentioning

confidence: 99%

Attribution of N2O sources in a grassland soil with laser spectroscopy based isotopocule analysis

et al. 2019

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“…If the ammonium and nitrate δ 15 N values in ammonium nitrate are known, N 2 O can be generated with known δ 15 N α and δ15 N β values that are anchored to the Air-N 2 nitrogen-isotope scale. Unfortunately, this reaction is difficult to reproduce, potentially explosive, and non-quantitative 3,15,28,29. Consequently, few laboratories have used this approach for calibration.…”

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confidence: 99%

Preliminary assessment of stable nitrogen and oxygen isotopic composition of USGS51 and USGS52 nitrous oxide reference gases and perspectives on calibration needs

Ostrom

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et al. 2018

Rapid Comm Mass Spectrometry

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The agreement of isotope-delta values obtained in the interlaboratory comparison was not sufficient to provide reliable accurate isotope measurement values for USGS51 and USGS52. We propose that provisional values for the isotopic composition of USGS51 and USGS52 determined at the Tokyo Institute of Technology can be adopted for normalizing and reporting sample data until further refinements are achieved through additional calibration efforts.

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“…During decomposition, the nitrogen atom of the NO − 3 ion is converted into the central nitrogen position of N 2 O, while the end nitrogen comes from the NH + 4 ion. However, the accuracy of this approach for the calibration of δ 15 N α and δ 15 N β was found to be limited by nonquantitative ammonium nitrate decomposition in combination with substantially different isotope enrichment factors for the conversion of the NO − 3 or NH + 4 nitrogen atom into the α or β position of the nitrous oxide molecule [111]. The yield of the ammonium nitrate decomposition reaction to nitrous oxide was found to be dependent on reaction conditions, e.g.…”

Section: Isotopic Analyses Of Atmospheric Carbon Dioxide Methane Andmentioning

confidence: 99%

Advances in reference materials and measurement techniques for greenhouse gas atmospheric observations

et al. 2019

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We present the global research landscape which aims to deliver a measurement infrastructure to underpin atmospheric observations of key greenhouse gases governing changes in the Earth's climate. These measurements present a significant challenge to the metrological community, analytical laboratories and major producers of reference materials. The review focuses on the progress made in the Gas Analysis Working Group of the Consultative Committee for Amount of Substance: Metrology in Chemistry and Biology (CCQM-GAWG) in establishing the primary realisation of the amount-of-substance fraction for carbon dioxide, methane and nitrous oxide in an air matrix. It also focuses on the importance of providing traceable measurements of isotopic composition of these components for commutability of reference materials and for isotope ratio measurements for greenhouse gas source attribution. Metrologia 56 (2019) 034006 (29pp) P J Brewer et al 2 of the World Meteorological Organization (WMO) for providing the framework for the development and implementation of integrated greenhouse gas observations, which is vital for understanding the global carbon cycle and the role greenhouse gases play in climate change. The developments in analytical techniques are also discussed which have shaped the direction of the metrology required to meet the evolving and future needs of stakeholders.

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Reassessment of the NH₄NO₃ thermal decomposition technique for calibration of the N₂O isotopic composition

Cited by 19 publications

References 44 publications

Attribution of N<sub>2</sub>O sources in a grassland soil with laser spectroscopy based isotopocule analysis

Attribution of N<sub>2</sub>O sources in a grassland soil with laser spectroscopy based isotopocule analysis

Preliminary assessment of stable nitrogen and oxygen isotopic composition of USGS51 and USGS52 nitrous oxide reference gases and perspectives on calibration needs

Advances in reference materials and measurement techniques for greenhouse gas atmospheric observations

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Reassessment of the NH4NO3 thermal decomposition technique for calibration of the N2O isotopic composition

Cited by 19 publications

References 44 publications

Attribution of N&lt;sub&gt;2&lt;/sub&gt;O sources in a grassland soil with laser spectroscopy based isotopocule analysis

Attribution of N&lt;sub&gt;2&lt;/sub&gt;O sources in a grassland soil with laser spectroscopy based isotopocule analysis

Preliminary assessment of stable nitrogen and oxygen isotopic composition of USGS51 and USGS52 nitrous oxide reference gases and perspectives on calibration needs

Advances in reference materials and measurement techniques for greenhouse gas atmospheric observations

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Product

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Reassessment of the NH₄NO₃ thermal decomposition technique for calibration of the N₂O isotopic composition

Attribution of N<sub>2</sub>O sources in a grassland soil with laser spectroscopy based isotopocule analysis

Attribution of N<sub>2</sub>O sources in a grassland soil with laser spectroscopy based isotopocule analysis