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Fluid to Rock Interactions During Deposition, Diagenesis, and Anthropogenic Activities: Application of Stable Barium Isotopes in the Appalachian Basin

Matecha, Rebecca Miriam (2023) Fluid to Rock Interactions During Deposition, Diagenesis, and Anthropogenic Activities: Application of Stable Barium Isotopes in the Appalachian Basin. Doctoral Dissertation, University of Pittsburgh. (Unpublished)

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The study of the interactions between aqueous fluids and geologic materials (rock, sediment, and soil) in both natural and anthropogenic systems is critical to understanding surface processes, development of geologic resources, diagenesis and lithification, and for predicting the fate and transport of environmental contaminants. In this dissertation I integrate field, experimental and petrographic studies with the use of stable barium (Ba) isotopes as a tool to investigate fluid-rock interactions in the Appalachian Basin.
Part 1 details development of an optimized method for the separation of Ba from major and isotopically interfering elements in a variety of geologic and hydrologic materials. Part 2 presents static autoclave and flow-through experiments with synthetic fracturing fluid conducted on Marcellus Shale core samples which indicated minimal Ba release from fluid−shale interactions but was consistent with barite precipitation, driven in part by release of sulfate from the shale, accompanied by a small amount of exchangeable Ba mobilization from shale surfaces. The results also indicate that the high-Ba concentrations in unconventional Marcellus Shale-produced waters are not a result of interaction of injected fluids with shale and/or drilling mud barite during hydraulic fracturing. Instead, they may indicate intrusion of high-Ba, high-δ138Ba formation waters entering the well via subsurface fractures. Finally, Part 3 is focused on a study of barite (BaSO4) and carbonate nodule development in the Upper Devonian Hanover Shale. The δ138Ba values in co-occurring barite and carbonate suggests downward movement of the sulfate methane transition zone after carbonate nodule precipitation and subsequent barite precipitation. Complex micromorphologic relationships between barite and carbonate and the variability in δ138Ba between nodule horizons, and between carbonate nodules and their barite rims, suggest asynchronous and possibly episodic introduction of isotopically distinct Ba during deposition of the Hanover Shale. The range of δ138Ba values suggest that Marcellus Shale formation waters could have diffused upwards with methane and been the source of Ba that led to the precipitation of barite.


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Item Type: University of Pittsburgh ETD
Status: Unpublished
CreatorsEmailPitt UsernameORCID
Matecha, Rebecca Miriamrmm159@pitt.edurmm159
ETD Committee:
TitleMemberEmail AddressPitt UsernameORCID
Committee CoChairCapo, Rosemary C.rcapo@pitt.edurcapo
Committee CoChairStewart, Brian W.bstewart@pitt.edubstewart
Committee MemberHarbert, Williamharbert@pitt.eduharbert
Committee MemberShelef, Eitanshelefeitan@pitt.edushelefeitan
Committee MemberHakala, Jacqueline Alexandraalexandra.hakala@NETL.DOE.GOV
Date: 12 May 2023
Date Type: Publication
Defense Date: 14 March 2023
Approval Date: 12 May 2023
Submission Date: 7 April 2023
Access Restriction: 2 year -- Restrict access to University of Pittsburgh for a period of 2 years.
Number of Pages: 99
Institution: University of Pittsburgh
Schools and Programs: Dietrich School of Arts and Sciences > Geology and Environmental Science
Degree: PhD - Doctor of Philosophy
Thesis Type: Doctoral Dissertation
Refereed: Yes
Uncontrolled Keywords: Barium, Isotopes, Appalachian Basin, Water Rock Interaction,
Date Deposited: 12 May 2023 19:06
Last Modified: 12 May 2023 19:06


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