Novel Tracer Method To Measure Isotopic Labeled Gas-Phase Nitrous Acid (HO15NO) in Biogeochemical Studies

Autoren

Dianming Wu
Christopher J Kampf
Ulrich Pöschl
Robert Oswald
Junfang Cui
Michael Ermel
Chunsheng Hu
Ivonne Trebs
Matthias Sörgel

DOI

10.1021/es501353x

eISSN

1520-5851

ISSN

0013-936X

Ausgabe der Veröffentlichung

14

Zeitschrift

Environmental Science & Technology

Sprache

en

Online publication date

2014

Paginierung

8021 - 8027

Datum der Veröffentlichung

2014

Status

Published

Herausgeber

American Chemical Society (ACS)

Herausgeber URL

http://dx.doi.org/10.1021/es501353x

Datum der Datenerfassung

2023

Titel

Novel Tracer Method To Measure Isotopic Labeled Gas-Phase Nitrous Acid (HO<sup>15</sup>NO) in Biogeochemical Studies

Ausgabe der Zeitschrift

48

Datenquelle: Crossref

Abstract

Gaseous nitrous acid (HONO), the protonated form of nitrite, contributes up to ∼60% to the primary formation of hydroxyl radical (OH), which is a key oxidant in the degradation of most air pollutants. Field measurements and modeling studies indicate a large unknown source of HONO during daytime. Here, we developed a new tracer method based on gas-phase stripping-derivatization coupled to liquid chromatography-mass spectrometry (LC-MS) to measure the 15N relative exceedance, ψ(15N), of HONO in the gas-phase. Gaseous HONO is quantitatively collected and transferred to an azo dye, purified by solid phase extraction (SPE), and analyzed using high performance liquid chromatography coupled to mass spectrometry (HPLC-MS). In the optimal working range of ψ(15N)=0.2-0.5, the relative standard deviation of ψ(15N) is <4%. The optimum pH and solvents for extraction by SPE and potential interferences are discussed. The method was applied to measure HO15NO emissions from soil in a dynamic chamber with and without spiking 15) labeled urea. The identification of HO15NO from soil with 15N urea addition confirmed biogenic emissions of HONO from soil. The method enables a new approach of studying the formation pathways of HONO and its role for atmospheric chemistry (e.g., ozone formation) and environmental tracer studies on the formation and conversion of gaseous HONO or aqueous NO2- as part of the biogeochemical nitrogen cycle, e.g., in the investigation of fertilization effects on soil HONO emissions and microbiological conversion of NO2- in the hydrosphere.

Addresses

Biogeochemistry Department, Max Plank Institute for Chemistry , P.O. Box 3060, 55020 Mainz, Germany.

Autoren

Dianming Wu
Christopher J Kampf
Ulrich Pöschl
Robert Oswald
Junfang Cui
Michael Ermel
Chunsheng Hu
Ivonne Trebs
Matthias Sörgel

DOI

10.1021/es501353x

eISSN

1520-5851

Externe Identifier

PubMed Identifier: 24954648

Open access

false

ISSN

0013-936X

Ausgabe der Veröffentlichung

14

Zeitschrift

Environmental science & technology

Schlüsselwörter

Nitrous Acid
Gases
Nitrogen Isotopes
Azo Compounds
Soil
Soil Pollutants
Calibration
Chromatography, High Pressure Liquid
Isotope Labeling
Reference Standards
Mass Spectrometry

Sprache

eng

Medium

Print-Electronic

Online publication date

2014

Paginierung

8021 - 8027

Datum der Veröffentlichung

2014

Status

Published

Datum der Datenerfassung

2014

Titel

Novel tracer method to measure isotopic labeled gas-phase nitrous acid (HO15NO) in biogeochemical studies.

Sub types

Research Support, Non-U.S. Gov't
Journal Article

Ausgabe der Zeitschrift

48

Datenquelle: Europe PubMed Central

Abstract

Gaseous nitrous acid (HONO), the protonated form of nitrite, contributes up to ∼60% to the primary formation of hydroxyl radical (OH), which is a key oxidant in the degradation of most air pollutants. Field measurements and modeling studies indicate a large unknown source of HONO during daytime. Here, we developed a new tracer method based on gas-phase stripping-derivatization coupled to liquid chromatography-mass spectrometry (LC-MS) to measure the 15N relative exceedance, ψ(15N), of HONO in the gas-phase. Gaseous HONO is quantitatively collected and transferred to an azo dye, purified by solid phase extraction (SPE), and analyzed using high performance liquid chromatography coupled to mass spectrometry (HPLC-MS). In the optimal working range of ψ(15N)=0.2-0.5, the relative standard deviation of ψ(15N) is <4%. The optimum pH and solvents for extraction by SPE and potential interferences are discussed. The method was applied to measure HO15NO emissions from soil in a dynamic chamber with and without spiking 15) labeled urea. The identification of HO15NO from soil with 15N urea addition confirmed biogenic emissions of HONO from soil. The method enables a new approach of studying the formation pathways of HONO and its role for atmospheric chemistry (e.g., ozone formation) and environmental tracer studies on the formation and conversion of gaseous HONO or aqueous NO2- as part of the biogeochemical nitrogen cycle, e.g., in the investigation of fertilization effects on soil HONO emissions and microbiological conversion of NO2- in the hydrosphere.

Autoren

Dianming Wu
Christopher J Kampf
Ulrich Pöschl
Robert Oswald
Junfang Cui
Michael Ermel
Chunsheng Hu
Ivonne Trebs
Matthias Sörgel

Autoren-URL

https://www.ncbi.nlm.nih.gov/pubmed/24954648

DOI

10.1021/es501353x

eISSN

1520-5851

Ausgabe der Veröffentlichung

14

Zeitschrift

Environ Sci Technol

Schlüsselwörter

Azo Compounds
Calibration
Chromatography, High Pressure Liquid
Gases
Isotope Labeling
Mass Spectrometry
Nitrogen Isotopes
Nitrous Acid
Reference Standards
Soil
Soil Pollutants

Sprache

eng

Country

United States

Paginierung

8021 - 8027

Datum der Veröffentlichung

2014

Status

Published

Datum, an dem der Datensatz öffentlich gemacht wurde

2014

Titel

Novel tracer method to measure isotopic labeled gas-phase nitrous acid (HO15NO) in biogeochemical studies.

Sub types

Journal Article
Research Support, Non-U.S. Gov't

Ausgabe der Zeitschrift

48

Datenquelle: PubMed

Novel Tracer Method To Measure Isotopic Labeled Gas-Phase Nitrous Acid (HO15NO) in Biogeochemical Studies

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