DOI: 10.1002/2016JD025906
论文题名: Tracking nitrous oxide emission processes at a suburban site with semicontinuous, in situ measurements of isotopic composition
作者: Harris E. ; Henne S. ; Hüglin C. ; Zellweger C. ; Tuzson B. ; Ibraim E. ; Emmenegger L. ; Mohn J.
刊名: Journal of Geophysical Research: Atmospheres
ISSN: 2169897X
出版年: 2017
卷: 122, 期: 3 起始页码: 1850
结束页码: 1870
语种: 英语
英文关键词: inverse modeling
; isotopes
; nitrous oxide
; spectroscopy
; troposphere
Scopus关键词: anthropogenic source
; concentration (composition)
; emission inventory
; in situ measurement
; isotopic composition
; nitrous oxide
; numerical model
; pollutant transport
; pollution monitoring
; suburban area
; tracer
; tracking
; troposphere
; Dubendorf
; Switzerland
; Zurich [Switzerland]
英文摘要: The isotopic composition of atmospheric nitrous oxide (N2O) was measured semicontinuously, at ∼35 min frequency in intermittent periods of 1–6 days over one and a half years, using preconcentration coupled to a quantum cascade laser spectrometer at the suburban site of Dübendorf, Switzerland. The achieved measurement repeatability was 0.08‰, 0.11‰, and 0.10‰ for δ18O, site preference, and δ15Nbulk respectively, which is better than or equal to standard flask sampling-based isotope ratio mass spectrometry performance. The observed mean diurnal cycle reflected the buildup of N2O from isotopically light sources on an isotopically heavy tropospheric background. The measurements were used to determine the source isotopic composition, which varied significantly compared to chemical and meteorological parameters monitored at the site. FLEXPART-COSMO transport modeling in combination with modified Emissions Database for Global Atmospheric Research inventory emissions was used to model N2O mole fractions at the site. Additionally, isotopic signatures were estimated for different source categories using literature data and used to simulate N2O isotopic composition over the measurement period. The model was able to capture variability in N2O mole fraction well, but simulations of isotopic composition showed little agreement with observations. In particular, measured source isotopic composition exhibited one magnitude larger variability than simulated, clearly indicating that the range of isotopic source signatures estimated from literature significantly underestimates true variability of source signatures. Source δ18O signature was found to be the most sensitive tracer for urban/industry versus agricultural N2O. δ15Nbulk and site preference may provide more insight into microbial and chemical emission processes than partitioning of anthropogenic source categories. ©2017. American Geophysical Union. All Rights Reserved. Citation statistics:
资源类型: 期刊论文
标识符: http://119.78.100.158/handle/2HF3EXSE/62716
Appears in Collections: 影响、适应和脆弱性 气候减缓与适应
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作者单位: Laboratory for Air Pollution and Environmental Technology, Empa, Dübendorf, Switzerland; Now at Plant, Soil and Ecosystem Processes Research Group, Institute of Ecology, University of Innsbruck, Innsbruck, Austria
Recommended Citation:
Harris E.,Henne S.,Hüglin C.,et al. Tracking nitrous oxide emission processes at a suburban site with semicontinuous, in situ measurements of isotopic composition[J]. Journal of Geophysical Research: Atmospheres,2017-01-01,122(3)