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Probing the chemistry, structure, and dynamics of the water-silica interface
Descriptive
TitleInfo
Title
Probing the chemistry, structure, and dynamics of the water-silica interface
Name
(type = personal)
NamePart
(type = family)
Lockwood
NamePart
(type = given)
Glenn K.
NamePart
(type = date)
1985-
DisplayForm
Glenn Lockwood
Role
RoleTerm
(authority = RULIB)
author
Name
(type = personal)
NamePart
(type = family)
Garofalini
NamePart
(type = given)
Stephen H.
DisplayForm
Stephen H. Garofalini
Affiliation
Advisory Committee
Role
RoleTerm
(authority = RULIB)
chair
Name
(type = personal)
NamePart
(type = family)
Klein
NamePart
(type = given)
Lisa C.
DisplayForm
Lisa C. Klein
Affiliation
Advisory Committee
Role
RoleTerm
(authority = RULIB)
internal member
Name
(type = personal)
NamePart
(type = family)
Danforth
NamePart
(type = given)
Stephen C.
DisplayForm
Stephen C. Danforth
Affiliation
Advisory Committee
Role
RoleTerm
(authority = RULIB)
internal member
Name
(type = personal)
NamePart
(type = family)
Cuitiño
NamePart
(type = given)
Alberto M.
DisplayForm
Alberto M. Cuitiño
Affiliation
Advisory Committee
Role
RoleTerm
(authority = RULIB)
outside member
Name
(type = corporate)
NamePart
Rutgers University
Role
RoleTerm
(authority = RULIB)
degree grantor
Name
(type = corporate)
NamePart
Graduate School - New Brunswick
Role
RoleTerm
(authority = RULIB)
school
TypeOfResource
Text
Genre
(authority = marcgt)
theses
OriginInfo
DateCreated
(qualifier = exact)
2013
DateOther
(qualifier = exact);
(type = degree)
2013-01
Place
PlaceTerm
(type = code)
xx
Language
LanguageTerm
(authority = ISO639-2b);
(type = code)
eng
Abstract
(type = abstract)
Despite its natural abundance and wide-ranging technological relevance, much remains unknown or unclear about water-silica interfaces. Computer simulation stands to bridge the gaps of knowledge left by experiment, and a recently developed Dissociative Water Potential has enabled the simulation of large amorphous silica surfaces in contact with water without having to impose a model of surface chemistry a priori. Earlier work with this model has revealed the existence of several protonated surface sites such as SiOH2+ and Si-(OH+)-Si that have yet to be extensively characterized. However, both experiment and quantum mechanical simulation have provided an increasing body of evidence that suggests these sites exist, and these sites may play key roles in some of the unexplained phenomena observed in water-silica systems. To this end, this Dissociative Water Potential has been applied to develop a comprehensive picture of the chemistry, structure, and dynamics of the water-silica interface that is unbiased by any expectation of what sites should form. The bridging OH site, Si-(OH+)-Si, does form and is characterized as a highly acidic site that occurs predominantly on strained Si-O-Si bridges near the interface. Similarly, the transient formation of SiOH2+ is observed, and this site is found to be more acidic than Si-(OH+)-Si. In addition to H3O+ that forms near the interface, all of these sites readily deprotonate and are expected to play a role in the enhanced proton conductivity experimentally observed in hydrated mesoporous silica. The reactions between water and silica are particularly relevant to the engineering of nuclear waste forms, and the role of water-silica interactions are also explored within the context of the degradation of silica-based waste forms exposed to radiation. Despite the significant simulation effort employed in glassy waste form research, no molecular models of radiation damage in silica include the effects of moisture. This deficiency is addressed, and water is found to play a significant role in accelerating the degradation of amorphous silica under irradiation. Water inhibits healing of the network and promotes the formation of voids into which more water can penetrate, giving way to new damage accumulation mechanisms not seen in any past simulations.
Subject
(authority = RUETD)
Topic
Materials Science and Engineering
Subject
(authority = ETD-LCSH)
Topic
Silica
Subject
(authority = ETD-LCSH)
Topic
Amorphous substances
RelatedItem
(type = host)
TitleInfo
Title
Rutgers University Electronic Theses and Dissertations
Identifier
(type = RULIB)
ETD
Identifier
ETD_4422
PhysicalDescription
Form
(authority = gmd)
electronic resource
InternetMediaType
application/pdf
InternetMediaType
text/xml
Extent
xxi, 197 p. : ill.
Note
(type = degree)
Ph.D.
Note
(type = bibliography)
Includes bibliographical references
Note
(type = vita)
Includes vita
Note
(type = statement of responsibility)
by Glenn K. Lockwood
Subject
(authority = ETD-LCSH)
Topic
Surface chemistry
Identifier
(type = hdl)
http://hdl.rutgers.edu/1782.1/rucore10001600001.ETD.000067796
RelatedItem
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TitleInfo
Title
Graduate School - New Brunswick Electronic Theses and Dissertations
Identifier
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rucore19991600001
Location
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(displayLabel = Rutgers, The State University of New Jersey)
NjNbRU
Identifier
(type = doi)
doi:10.7282/T3B856T3
Genre
(authority = ExL-Esploro)
ETD doctoral
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Rights
RightsDeclaration
(ID = rulibRdec0006)
The author owns the copyright to this work.
RightsHolder
(type = personal)
Name
FamilyName
Lockwood
GivenName
Glenn
Role
Copyright Holder
RightsEvent
Type
Permission or license
DateTime
(encoding = w3cdtf);
(qualifier = exact);
(point = start)
2012-12-15 13:41:50
AssociatedEntity
Name
Glenn Lockwood
Role
Copyright holder
Affiliation
Rutgers University. Graduate School - New Brunswick
AssociatedObject
Type
License
Name
Author Agreement License
Detail
I hereby grant to the Rutgers University Libraries and to my school the non-exclusive right to archive, reproduce and distribute my thesis or dissertation, in whole or in part, and/or my abstract, in whole or in part, in and from an electronic format, subject to the release date subsequently stipulated in this submittal form and approved by my school. I represent and stipulate that the thesis or dissertation and its abstract are my original work, that they do not infringe or violate any rights of others, and that I make these grants as the sole owner of the rights to my thesis or dissertation and its abstract. I represent that I have obtained written permissions, when necessary, from the owner(s) of each third party copyrighted matter to be included in my thesis or dissertation and will supply copies of such upon request by my school. I acknowledge that RU ETD and my school will not distribute my thesis or dissertation or its abstract if, in their reasonable judgment, they believe all such rights have not been secured. I acknowledge that I retain ownership rights to the copyright of my work. I also retain the right to use all or part of this thesis or dissertation in future works, such as articles or books.
Copyright
Status
Copyright protected
Availability
Status
Open
Reason
Permission or license
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Technical
RULTechMD
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ContentModel
ETD
OperatingSystem
(VERSION = 5.1)
windows xp
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