Revealing chlorinated ethene transformation hotspots in a nitrate-impacted hyporheic zone

John J. Weatherill, Stefan Krause, Sami Ullah, Nigel J. Cassidy, Amir Levy, Falko P. Drijfhout, Michael O. Rivett

Research output: Contribution to journalArticle

1 Citation (Scopus)

Abstract

Hyporheic zones are increasingly thought of as natural bioreactors, capable of transforming and attenuating groundwater pollutants present in diffuse baseflow. An underappreciated scenario in the understanding of contaminant fate in hyporheic zones is the interaction between point-source trichloroethene (TCE) plumes and ubiquitous, non-point source pollutants such as nitrate. This study aims to conceptualise critical biogeochemical gradients in the hyporheic zone which govern the export potential of these redox-sensitive pollutants from carbon-poor, oxic aquifers. Within the TCE plume discharge zone, discrete vertical profiling of the upper 100 cm of sediment pore water chemistry revealed an 80% increase in dissolved organic carbon (DOC) concentrations and 20e60 cm thick hypoxic zones (<2mg O2 L1) within which most reactive transport was observed. A 33% reduction of nitrate concentrations coincided with elevated pore water nitrous oxide concentrations as well as the appearance of manganese and the TCE metabolite cis-1,2-dichloroethene (cDCE). Elevated groundwater nitrate concentrations (>50 mg L1) create a large stoichiometric demand for bioavailable DOC in discharging groundwater. With the benefit of a high-resolution grid of pore water samplers investigating the shallowest 30 cm of hypoxic groundwater flow paths, we identified DOC-rich hotspots associated with submerged vegetation (Ranunculus spp.), where low-energy metabolic processes such as mineral dissolution/reduction, methanogenesis and ammonification dominate. Using a chlorine index metric, we show that enhanced TCE to cDCE transformation takes place within these biogeochemical hotspots, highlighting their relevance for natural plume attenuation.
Original languageEnglish
Pages (from-to)222-231
Number of pages10
JournalWater Research
Volume161
Early online date26 May 2019
DOIs
Publication statusPublished - 15 Sep 2019

Fingerprint

hyporheic zone
Trichloroethylene
trichloroethylene
ethylene
Nitrates
Organic carbon
nitrate
dissolved organic carbon
Groundwater
porewater
plume
groundwater
pollutant
submerged vegetation
Water
ammonification
Groundwater flow
reactive transport
methanogenesis
baseflow

Keywords

  • hyporheic zone
  • terminal electron-accepting processes
  • chlorinated ethenes
  • nitrate
  • dissolved organic carbon
  • natural attenuation

Cite this

Weatherill, J. J., Krause, S., Ullah, S., Cassidy, N. J., Levy, A., Drijfhout, F. P., & Rivett, M. O. (2019). Revealing chlorinated ethene transformation hotspots in a nitrate-impacted hyporheic zone. Water Research, 161, 222-231. https://doi.org/10.1016/j.watres.2019.05.083
Weatherill, John J. ; Krause, Stefan ; Ullah, Sami ; Cassidy, Nigel J. ; Levy, Amir ; Drijfhout, Falko P. ; Rivett, Michael O. / Revealing chlorinated ethene transformation hotspots in a nitrate-impacted hyporheic zone. In: Water Research. 2019 ; Vol. 161. pp. 222-231.
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Weatherill, JJ, Krause, S, Ullah, S, Cassidy, NJ, Levy, A, Drijfhout, FP & Rivett, MO 2019, 'Revealing chlorinated ethene transformation hotspots in a nitrate-impacted hyporheic zone', Water Research, vol. 161, pp. 222-231. https://doi.org/10.1016/j.watres.2019.05.083

Revealing chlorinated ethene transformation hotspots in a nitrate-impacted hyporheic zone. / Weatherill, John J.; Krause, Stefan; Ullah, Sami; Cassidy, Nigel J.; Levy, Amir ; Drijfhout, Falko P.; Rivett, Michael O.

In: Water Research, Vol. 161, 15.09.2019, p. 222-231.

Research output: Contribution to journalArticle

TY - JOUR

T1 - Revealing chlorinated ethene transformation hotspots in a nitrate-impacted hyporheic zone

AU - Weatherill, John J.

AU - Krause, Stefan

AU - Ullah, Sami

AU - Cassidy, Nigel J.

AU - Levy, Amir

AU - Drijfhout, Falko P.

AU - Rivett, Michael O.

PY - 2019/9/15

Y1 - 2019/9/15

N2 - Hyporheic zones are increasingly thought of as natural bioreactors, capable of transforming and attenuating groundwater pollutants present in diffuse baseflow. An underappreciated scenario in the understanding of contaminant fate in hyporheic zones is the interaction between point-source trichloroethene (TCE) plumes and ubiquitous, non-point source pollutants such as nitrate. This study aims to conceptualise critical biogeochemical gradients in the hyporheic zone which govern the export potential of these redox-sensitive pollutants from carbon-poor, oxic aquifers. Within the TCE plume discharge zone, discrete vertical profiling of the upper 100 cm of sediment pore water chemistry revealed an 80% increase in dissolved organic carbon (DOC) concentrations and 20e60 cm thick hypoxic zones (<2mg O2 L1) within which most reactive transport was observed. A 33% reduction of nitrate concentrations coincided with elevated pore water nitrous oxide concentrations as well as the appearance of manganese and the TCE metabolite cis-1,2-dichloroethene (cDCE). Elevated groundwater nitrate concentrations (>50 mg L1) create a large stoichiometric demand for bioavailable DOC in discharging groundwater. With the benefit of a high-resolution grid of pore water samplers investigating the shallowest 30 cm of hypoxic groundwater flow paths, we identified DOC-rich hotspots associated with submerged vegetation (Ranunculus spp.), where low-energy metabolic processes such as mineral dissolution/reduction, methanogenesis and ammonification dominate. Using a chlorine index metric, we show that enhanced TCE to cDCE transformation takes place within these biogeochemical hotspots, highlighting their relevance for natural plume attenuation.

AB - Hyporheic zones are increasingly thought of as natural bioreactors, capable of transforming and attenuating groundwater pollutants present in diffuse baseflow. An underappreciated scenario in the understanding of contaminant fate in hyporheic zones is the interaction between point-source trichloroethene (TCE) plumes and ubiquitous, non-point source pollutants such as nitrate. This study aims to conceptualise critical biogeochemical gradients in the hyporheic zone which govern the export potential of these redox-sensitive pollutants from carbon-poor, oxic aquifers. Within the TCE plume discharge zone, discrete vertical profiling of the upper 100 cm of sediment pore water chemistry revealed an 80% increase in dissolved organic carbon (DOC) concentrations and 20e60 cm thick hypoxic zones (<2mg O2 L1) within which most reactive transport was observed. A 33% reduction of nitrate concentrations coincided with elevated pore water nitrous oxide concentrations as well as the appearance of manganese and the TCE metabolite cis-1,2-dichloroethene (cDCE). Elevated groundwater nitrate concentrations (>50 mg L1) create a large stoichiometric demand for bioavailable DOC in discharging groundwater. With the benefit of a high-resolution grid of pore water samplers investigating the shallowest 30 cm of hypoxic groundwater flow paths, we identified DOC-rich hotspots associated with submerged vegetation (Ranunculus spp.), where low-energy metabolic processes such as mineral dissolution/reduction, methanogenesis and ammonification dominate. Using a chlorine index metric, we show that enhanced TCE to cDCE transformation takes place within these biogeochemical hotspots, highlighting their relevance for natural plume attenuation.

KW - hyporheic zone

KW - terminal electron-accepting processes

KW - chlorinated ethenes

KW - nitrate

KW - dissolved organic carbon

KW - natural attenuation

U2 - 10.1016/j.watres.2019.05.083

DO - 10.1016/j.watres.2019.05.083

M3 - Article

VL - 161

SP - 222

EP - 231

JO - Water Research

JF - Water Research

SN - 0043-1354

ER -

Weatherill JJ, Krause S, Ullah S, Cassidy NJ, Levy A, Drijfhout FP et al. Revealing chlorinated ethene transformation hotspots in a nitrate-impacted hyporheic zone. Water Research. 2019 Sep 15;161:222-231. https://doi.org/10.1016/j.watres.2019.05.083