Multi-species measurements of nitrogen isotopic composition reveal the spatial constraints and biological drivers of ammonium attenuation across a highly contaminated groundwater system

Wells, Naomi S.; Hakoun, Vivien; Brouyère, Serge; Knoeller, Kay

doi:10.1016/j.watres.2016.04.025

Article (Scientific journals)

Multi-species measurements of nitrogen isotopic composition reveal the spatial constraints and biological drivers of ammonium attenuation across a highly contaminated groundwater system

Wells, Naomi S.; Hakoun, Vivien; Brouyère, Serge et al.

2016 • In Water Research, 98, p. 363-375

Peer Reviewed verified by ORBi

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https://hdl.handle.net/2268/196024

DOI
10.1016/j.watres.2016.04.025

PubMed
27124126

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Keywords :

ammonium attenuation; groundwater; industrial pollution; nitrate reduction; nitrite reduction; stable isotopes

Abstract :

[en] Groundwater under industrial sites is characterised by heterogeneous chemical mixtures, making it difficult to assess the fate and transport of individual contaminants. Quantifying the in-situ biological removal (attenuation) of nitrogen (N) is particularly difficult due to its reactivity and ubiquity. Here a multi-isotope approach is developed to distinguish N sources and sinks within groundwater affected by complex industrial pollution. Samples were collected from 70 wells across the two aquifers underlying a historic industrial area in Belgium. Below the industrial site the groundwater contained up to 1000 mg Nl-1 ammonium (NH4 +) and 300 mg N l-1 nitrate (NO3-), while downgradient concentrations decreased to ~1 mg l-1 DIN ([DIN] = [NH4+-N] + [NO3--N] + [NO2--N]). Mean δ1534 N-DIN increased from ~2‰ to +20‰ over this flow path, broadly confirming that biological N attenuation drove the measured concentration decrease. Multi-variate analysis of water chemistry identified two distinct NH4+ sources (δ15N-NH4+ from -14‰ and +5‰) within the contaminated zone of both aquifers. Nitrate dual isotopes co-varied (δ15 N: -3‰ - +60‰; δ18O: 0‰ - +50‰) within the range expected for coupled nitrification and denitrification of the identified sources. The fact that δ15N-NO2- values were 50‰ to 20‰ less than δ15N-NH4+ values in 40 the majority of wells confirmed that nitrification controlled N turnover across the site. However, the fact that δ15N-NO2- was greater than δ15N-NH4+ in wells with the highest [NH4+] shows that an autotrophic NO2- reduction pathway (anaerobic NH4+ oxidation or nitrifier-denitrification) drove N attenuation closest to the contaminant plume. This direct empirical evidence that both autotrophic and heterotrophic biogeochemical processes drive N attenuation in contaminated aquifers demonstrates the power of multiple N isotopes to untangle N cycling in highly complex systems.

Disciplines :

Geological, petroleum & mining engineering
Earth sciences & physical geography

Author, co-author :

Wells, Naomi S.; Helmholtz Centre for Environmental Research - UFZ Leipzig > Department of Catchment Hydrology

Hakoun, Vivien ; Université de Liège > Département ArGEnCo > Hydrogéologie & Géologie de l'environnement

Brouyère, Serge ; Université de Liège > Département ArGEnCo > Hydrogéologie & Géologie de l'environnement

Knoeller, Kay; Helmholtz Centre for Environmental Research – UFZ Leipzig > Department of Catchment Hydrology

Language :

English

Title :

Multi-species measurements of nitrogen isotopic composition reveal the spatial constraints and biological drivers of ammonium attenuation across a highly contaminated groundwater system

Publication date :

July 2016

Journal title :

Water Research

ISSN :

0043-1354

eISSN :

1879-2448

Publisher :

Pergamon Press, Oxford, United Kingdom

Volume :

Pages :

363-375

Peer reviewed :

Peer Reviewed verified by ORBi

Additional URL :

http://www.sciencedirect.com/science/article/pii/S0043135416302238?np=y

European Projects :

FP7 - 265063 - ADVOCATE - Advancing Sustainable In Situ Remediation for Contaminated Land and Groundwater

Funders :

DG RDT - Commission Européenne. Direction Générale de la Recherche et de l'Innovation
CE - Commission Européenne

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