Nitrate Controls on the Extent and Type of Metal Retention in Fine-Grained Sediments of a Simulated Aquifer

Engel, Maya; Noël, Vincent; Kukkadapu, Ravi K.; Boye, Kristin E.; Bargar, John R.; Fendorf, Scott

doi:10.1021/acs.est.2c03403

Nitrate Controls on the Extent and Type of Metal Retention in Fine-Grained Sediments of a Simulated Aquifer

Journal Article · Fri Oct 07 00:00:00 EDT 2022 · Environmental Science and Technology

DOI:https://doi.org/10.1021/acs.est.2c03403· OSTI ID:1895419

Engel, Maya ^[1]; ^[2]; ^[3]; ^[4]; ^[4]; ^[5]

Stanford Univ., CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
Geochemistry and Biogeochemistry Group, SLAC National Accelerator Laboratory, Menlo Park, California 94025, United States
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Stanford Univ., CA (United States)

Aquifer groundwater quality is largely controlled by sediment composition and physical heterogeneity, which commonly sustain a unique redox gradient pattern. Attenuation of heavy metals within these heterogeneous aquifers is reliant on multiple factors, including redox conditions, and redox-active species that can further influence biogeochemical cycling. Here, we simulated an alluvial aquifer system using columns filled with natural coarse-grained sediments and two domains of fine-grained sediment lenses. Our goal was to examine heavy metal (Ni and Zn) attenuation within a complex aquifer network and further explore nitrate-rich groundwater conditions. The fine-grained sediment lenses sustained reducing conditions and served as a sink for Ni sequestration – in the form of Ni-silicates, Ni-organic matter, and a dominant Ni-sulfide phase. Further, the silicate clay and sulfide pools were also important retention mechanisms for Zn; however, Ni was associated more extensively with organic matter compared to Zn that formed layered double hydroxides. Nitrate-rich conditions promoted denitrification within the lenses that was coupled to the oxidation of Fe(II) and the concomitant precipitation of an Fe(III) phase with higher structural distortion. A decreased metal sulfide pool also resulted, where nitrate-rich conditions generated in an average 20% decrease in solid phase Ni, Zn, and Fe. Ultimately, nitrate plays a significant role in the aquifer’s biogeochemical cycling and capacity to retain heavy metals.

View Accepted Manuscript (DOE)

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Biological and Environmental Research (BER); United States-Israel Binational Agricultural Research and Development Fund (BARD)

Grant/Contract Number:: AC02-76SF00515; AC05-76RL01830; SC0020205

OSTI ID:: 1895419

Report Number(s):: PNNL-SA-172685

Journal Information:: Environmental Science and Technology, Journal Name: Environmental Science and Technology Journal Issue: 20 Vol. 56; ISSN 0013-936X

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Nitrate Controls on the Extent and Type of Metal Retention in Fine-Grained Sediments of a Simulated Aquifer

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