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@ARTICLE{Well:22329,
author = {Well, R. and Eschenbach, W. and Flessa, H. and von der
Heide, C. and Weymann, D.},
title = {{A}re dual isotope and isotopomer ratios of {N}2{O} useful
indicators for {N}2{O} turnover during denitrification in
nitrate-contaminated aquifers?},
journal = {Geochimica et cosmochimica acta},
volume = {90},
issn = {0016-7037},
address = {New York, NY [u.a.]},
publisher = {Elsevier},
reportid = {PreJuSER-22329},
pages = {265 - 282},
year = {2012},
note = {This study was supported by the Deutsche
Forschungsgemeinschaft (DFG), the Deutsche Bundestiftung
Umwelt (DBU) and the Oldenburgisch-Ostenfriesischer
Wasserverband (OOWV). We thank Ingrid Ostermeyer and Karin
Schmidt for technical assistance, Christian Ahl for
supplying laboratory facilities, Christian Gliesche for
information on the occurrence of fungi in groundwater and
the Centre for Stable Isotope Research and Analysis at the
University of Gottingen for isotope analysis. We gratefully
acknowledge the constructive comments and valuable
recommendations made by Nathaniel Ostrom and another two
anonymous reviewers on a former version of this paper.},
abstract = {Denitrifying aquifers are sources of the greenhouse gas
N2O. Isotopic signatures reflect processes of production and
reduction of N2O, but it is not clear to which extent these
can be used to quantify those processes. We investigated the
spatial distribution of isotopologue values of N2O (delta
O-18, average delta N-15, and N-15 site preference, SP) in
two denitrifying sandy aquifers to study N2O production and
reduction and associated isotope effects in groundwater. For
the first time, we combined this approach with direct
estimation of N2O reduction from excess-N-2 analysis.
Groundwater samples were collected from 15 monitoring wells
and four multilevel sampling wells and analysed for NO3-,
dissolved N2O, dissolved O-2, excess N-2 from
denitrification and isotopic signatures of NO3- and N2O.
Both aquifers exhibited high NO3- concentrations with
average concentrations of 22 and 15 mg N L-1, respectively.
Evidence of intense denitrification with associated N2O
formation was obtained from mean excess-N-2 of 3.5 and 4.3
mg N L-1, respectively. Isotopic signatures of N2O were
highly variable with ranges of 17.6-113.2 parts per thousand
(delta O-18), 55.4 to 89.4 parts per thousand (delta
N-15(bulk)) and 1.8-97.9 parts per thousand (SP). delta N-15
and delta O-18 of NO3- ranged from 2.1 parts per thousand to
65.5 parts per thousand and from -5 parts per thousand to
33.5 parts per thousand, respectively.The relationships
between delta N-15 of NO3- , delta N-15(bulk) and SP were
not in good agreement with the distribution predicted by a
Rayleigh-model of isotope fractionation. The large ranges of
delta O-18 and SP of N2O as well as the close correlation
between these values could be explained by the fact that N2O
reduction to N-2 was strongly progressed but variable.We
confirm and explain that a large range in SP and delta O-18
is typical for N2O from denitrifying aquifers, showing that
this source signature can be distinguished from the isotopic
fingerprint of N2O emitted from soils without water-logging.
We conclude that isotopologue values of N2O in our sites
were not suitable to quantify production or reduction of N2O
or the contribution of different processes to the total N2O
flux, apparently because these values were not only governed
by individual pathways but eventually also by the spatial
distribution of substrates and activity within the aquifers.
These observations could be explained by the dynamics of N2O
production, reduction and transport in water-saturated
systems with heterogenic distribution of microbial activity
and by a combination of diffusive and enzymatic isotope
effects. (C) 2012 Elsevier Ltd. All rights reserved.},
keywords = {J (WoSType)},
cin = {IBG-3},
ddc = {550},
cid = {I:(DE-Juel1)IBG-3-20101118},
pnm = {Terrestrische Umwelt},
pid = {G:(DE-Juel1)FUEK407},
shelfmark = {Geochemistry $\&$ Geophysics},
typ = {PUB:(DE-HGF)16},
UT = {WOS:000306334200016},
doi = {10.1016/j.gca.2012.04.045},
url = {https://juser.fz-juelich.de/record/22329},
}