Journal
GEOPHYSICAL RESEARCH LETTERS
Volume 43, Issue 1, Pages 440-448Publisher
AMER GEOPHYSICAL UNION
DOI: 10.1002/2015GL066438
Keywords
NOx; isotopes; fractionation; nitrogen; nitrate
Categories
Funding
- National Science Foundation [DGE-1333468]
- Purdue Climate Change Research Center (PCCRC) graduate fellowship program [1554]
- Purdue Center for Environment undergraduate research award
- Purdue Chemistry Summer Research Stipend/Margerum Award
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The nitrogen (N) isotope exchange between nitric oxide (NO) and nitrogen dioxide (NO2) has been previously suggested to influence N stable isotope compositions (N-15) of these molecules. However, there is disagreement in the magnitude of the N isotopic fractionation (NO2/NO) resulting from this exchange process between previous experimental and theoretical studies. To this end, we measured NO2/NO associated with this exchange reaction at various temperatures. Our results indicate NO2/NO to be 1.04030.0015, 1.03560.0015, and 1.03360.0014 at 278K, 297K, and 310K, respectively. These measured values are within experimental error of the values we calculated using a modified version of the Bigeleisen-Mayer equation corrected for accurate zero-point energies, indicating an agreement between experiment and theory. Modeling of this exchange reaction demonstrates that N-15-NO2 may exhibit a diurnal and seasonal profile if N isotopic equilibrium is achieved.
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