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A Study of the Degradative Capabilities of the Bimetallic System: Mg(Pd/C) as Applied in the Destruction of Decafluoropentane, an Environmental Contaminant

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Date Issued:
2012
Abstract/Description:
Pollution from hydrofluorocarbons (HFCs) poses a serious challenge to the environmental community. Released from industrial operations, they have contaminated both the atmosphere and groundwater and are considered persistent in both media. For over the past 20 years, the practice of synthesizing HFCs as alternatives to chlorofluorocarbons (CFCs) has been conducted in an effort to reverse the effects of stratospheric ozone layer depletion. HFCs also exhibit desirable properties as precision cleaning solvents due to their low surface energies but that use has lead to releases contaminating groundwater resulting in recalcitrant pollution in the form of dense non-aqueous phase liquids (DNAPLs). Results from studies requested by the EPA have shown HFCs to exhibit developmental and neurological damage in animal life along with their impact to humans remaining not completely understood. Therefore, the potential hazards of HFCs to human health and the environment necessitates the development of an effective and environmentally responsible technology for their remediation from groundwater. The National Aeronautics and Space Administration (NASA) has employed the use of various halogenated solvents in its spacecraft cleaning operations at its facilities for many years and in that time experienced accidental releases which eventually resulted in environmental contamination. Many of the organic solvents employed in these operations consisted of halogenated compounds with most being partially chlorinated and fluorinated hydrocarbons. Through normal use and operation, releases of these materials found their way into the environs of atmosphere, soil and groundwater. Remediation of fluorinated compounds has not followed the successful path laid by clean-up technologies developed for their chlorinated counterparts. Fluorinated compounds are resistant however to those methods due to their unreactive nature stemming from the properties of the strong carbon-fluorine bond. This unique bonding property also ensures that their environmental persistence endures. One particular fluorinated groundwater contaminant, the HFC 1,1,1,2,2,3,4,5,5,5-decafluoropentane (DFP), which has been used by NASA since the late 1990's was selected as the focus of this study. For this study, various reductive metal systems were evaluated for their capability towards effective degradation of DFP. These included the metals: iron, magnesium, aluminum and zinc and several bimetallic alloys as well as on carbon support. Variations in protic solvent reaction media and acidic metal activation were also explored. The bimetallic reductive catalytic alloy Magnesium with Palladium on Carbon, Mg(Pd/C), in aqueous media proved to be the successful candidate with 100% conversion to simple hydrocarbons. Mechanistic evaluation for degradation is proposed via a series of stepwise catalytic hydrodefluorination reactions. Kinetic studies revealed degradation to obey second order reaction kinetics. Further study should be conducted optimizing an in situ groundwater delivery method for field application. Additionally, the developed technology should be assessed against other groundwater fluorocarbon pollutants; either as a method for remediating multiple fluorinated polluted sites or as a polishing agent where all other pollutants have been abated.
Title: A Study of the Degradative Capabilities of the Bimetallic System: Mg(Pd/C) as Applied in the Destruction of Decafluoropentane, an Environmental Contaminant.
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Name(s): Tomlin, Douglas, Author
Clausen, Christian, Committee Chair
Yestrebsky, Cherie, Committee Member
Hampton, Michael, Committee Member
Elsheimer, Seth, Committee Member
Griffin, Timothy, Committee Member
University of Central Florida, Degree Grantor
Type of Resource: text
Date Issued: 2012
Publisher: University of Central Florida
Language(s): English
Abstract/Description: Pollution from hydrofluorocarbons (HFCs) poses a serious challenge to the environmental community. Released from industrial operations, they have contaminated both the atmosphere and groundwater and are considered persistent in both media. For over the past 20 years, the practice of synthesizing HFCs as alternatives to chlorofluorocarbons (CFCs) has been conducted in an effort to reverse the effects of stratospheric ozone layer depletion. HFCs also exhibit desirable properties as precision cleaning solvents due to their low surface energies but that use has lead to releases contaminating groundwater resulting in recalcitrant pollution in the form of dense non-aqueous phase liquids (DNAPLs). Results from studies requested by the EPA have shown HFCs to exhibit developmental and neurological damage in animal life along with their impact to humans remaining not completely understood. Therefore, the potential hazards of HFCs to human health and the environment necessitates the development of an effective and environmentally responsible technology for their remediation from groundwater. The National Aeronautics and Space Administration (NASA) has employed the use of various halogenated solvents in its spacecraft cleaning operations at its facilities for many years and in that time experienced accidental releases which eventually resulted in environmental contamination. Many of the organic solvents employed in these operations consisted of halogenated compounds with most being partially chlorinated and fluorinated hydrocarbons. Through normal use and operation, releases of these materials found their way into the environs of atmosphere, soil and groundwater. Remediation of fluorinated compounds has not followed the successful path laid by clean-up technologies developed for their chlorinated counterparts. Fluorinated compounds are resistant however to those methods due to their unreactive nature stemming from the properties of the strong carbon-fluorine bond. This unique bonding property also ensures that their environmental persistence endures. One particular fluorinated groundwater contaminant, the HFC 1,1,1,2,2,3,4,5,5,5-decafluoropentane (DFP), which has been used by NASA since the late 1990's was selected as the focus of this study. For this study, various reductive metal systems were evaluated for their capability towards effective degradation of DFP. These included the metals: iron, magnesium, aluminum and zinc and several bimetallic alloys as well as on carbon support. Variations in protic solvent reaction media and acidic metal activation were also explored. The bimetallic reductive catalytic alloy Magnesium with Palladium on Carbon, Mg(Pd/C), in aqueous media proved to be the successful candidate with 100% conversion to simple hydrocarbons. Mechanistic evaluation for degradation is proposed via a series of stepwise catalytic hydrodefluorination reactions. Kinetic studies revealed degradation to obey second order reaction kinetics. Further study should be conducted optimizing an in situ groundwater delivery method for field application. Additionally, the developed technology should be assessed against other groundwater fluorocarbon pollutants; either as a method for remediating multiple fluorinated polluted sites or as a polishing agent where all other pollutants have been abated.
Identifier: CFE0004798 (IID), ucf:49742 (fedora)
Note(s): 2012-12-01
Ph.D.
Sciences, Chemistry
Doctoral
This record was generated from author submitted information.
Subject(s): hydrofluorocarbon -- catalytic reduction -- hydrodefluorination -- bimetal -- groundwater
Persistent Link to This Record: http://purl.flvc.org/ucf/fd/CFE0004798
Restrictions on Access: campus 2014-06-15
Host Institution: UCF

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