Date of Award

Summer 8-2017

Embargo Period

9-26-2019

Degree Type

Dissertation (CMU Access Only)

Degree Name

Doctor of Philosophy (PhD)

Department

Civil and Environmental Engineering

Advisor(s)

Greg Lowry

Abstract

Mercury (Hg) is distributed globally through atmospheric transport. The broad range of environmental conditions will lead to various possible speciation of mercury, which will ultimately affect the toxicity and transport of mercury. Hg toxicity, transport and speciation have been widely studied. However, information about effects of Hg speciation on its environmental behavior in unsaturated porous media and on its removal from wastewater stream is still limited. The present work contributes towards understanding the impact of Hg speciation on both the transport of Hg species in unsaturated porous media (e.g., surface soil) and removal of Hg species in wastewater streams. This knowledge is necessary to assess the possible environmental risks of Hg in the environment, where different Hg species can exist and have different properties and impacts on water quality and ecosystems. The first objective of this research was to determine the effect of Hg speciation on its retention in partially saturated soils. The retention of Hg species in model porous media and in real soil was assessed in column breakthrough experiments. Deposition (retention) rates for each Hg species were calculated to evaluate the influence of Hg speciation, porous medium composition and influent solution on the mobility of Hg species in porous media. This study provided information about the relative retention of each Hg species in soils, and identified natural-organic-matter-bound Hg as the most mobile Hg species and that with the greatest potential for vertical migration to groundwater. The second objective of this research was to determine how Hg speciation affects its ability to be removed from water via adsorption by activated carbon and organoclay. The effects of Hg speciation, water quality parameters and adsorbent type on the removal of Hg were compared to explore the potential removal efficacy and mechanism. The result indicated Hg removal efficacy was influenced by Hg speciation differently depending on the solution conditions. Therefore, using total dissolved Hg(II) to predict Hg removal efficacy may not provide a reliable estimate of adsorption. Organoclay was shown to have a highly reactive surface and the highest adsorption capacity per unit specific surface area among the tested adsorbents. The third objective was to determine the Hg speciation in produced water from an oil production well, and to study the influence of Hg speciation on its removal from produced water by adsorbents. Mercury species in a produced water sample were identified as mainly particulate species and hydrophobic species. The removal of the amended Hg species in produced water was measured to evaluate the impact of Hg speciation on its removal. This study showed that produced water composition affected Hg speciation and formed hydrophobic Hg was more difficult to remove than initially added hydrophilic Hg species in produced water.

Available for download on Thursday, September 26, 2019

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