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Modulation of molecular mobility in sucrose-based amorphous solids detected by phosphorescence of erythrosin B
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Title
Modulation of molecular mobility in sucrose-based amorphous solids detected by phosphorescence of erythrosin B
Name
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You
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Yumin
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Yumin You
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author
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Ludescher
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Richard
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Advisory Committee
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Richard Ludescher
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Takhistov
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Paul
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Advisory Committee
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Paul Takhistov
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internal member
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HUANG
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QINGRONG
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Advisory Committee
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QINGRONG HUANG
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internal member
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Seetharaman
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Koushik
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Advisory Committee
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Koushik Seetharaman
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outside member
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Rutgers University
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degree grantor
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Graduate School - New Brunswick
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school
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Text
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theses
OriginInfo
DateCreated
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2007
DateOther
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2007-10
Language
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English
PhysicalDescription
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electronic
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application/pdf
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text/xml
Extent
xxi, 432 pages
Abstract
This project studied the temperature and composition dependence of molecular mobility in amorphous sucrose. Phosphorescence of erythrosin B provided parameters sensitive to localized molecular mobility in the glass and to more global modes of mobility activated at the glass transition and provided evidence of dynamic site heterogeneity in amorphous sucrose solids. In sucrose-based binary matrices, plasticizer (glycerol), salts (NaCl, CaCl2, MgCl2, Na-citrate, Na-acetate, Na-phosphates), maltodextrins (DE 5 to 18), protein (gelatin), and polysaccharides (xanthan and high amylose starch) were selected to investigate how variations in nature and content of each additive influence the molecular mobility as well as dynamic site heterogeneity in amorphous sucrose matrix.
Measurements of phosphorescence intensity, lifetime, and emission energy were made in amorphous sucrose-additive films containing the probe erythrosin B. Results showed the complex effects of additives on the mobility in a hydrogen-bonded sugar matrix. Glycerol exhibited an antiplasticization effect shown as decreased mobility at glycerol/sucrose mole ratio ≤ 0.27 and at temperature ≤ 45° C. On the contrary, all the polymers studied, including gelatin, xanthan and high amylose starch, displayed a ‘plasticization’ effect (increasing mobility) at very low while a rigidification effect (decreasing mobility) at higher concentration without significant change in Tg. Maltodextrins, mixtures of molecules with a variety of molecular weights, increase the mobility in spite of their high Tg. Sodium chloride showed a strong rigidification effect on the sucrose matrix; however, this effect was weakened at mole ratio NaCl/sucrose above 0.5. Other salts showed effects resulting from a compromise between two opposite actions (decreasing mobility due to salt itself and increasing mobility due to absorbed moisture). All above behaviors are difficult to interpret using Tg alone. Molecular mobility appears to be more accurate to evaluate the physical stability of the matrix.
Phosphorescence of erythrosin B was also able to report dynamic site heterogeneity that is an intrinsic property of the amorphous solid state. The heterogeneity was be evaluated by the variation of lifetime and lifetime heterogeneity across the excitation and emission band and the temperature dependence of bandwidth and lifetime heterogeneity. The composition influence on the dynamic site heterogeneity was discussed as well.
Measurements of phosphorescence intensity, lifetime, and emission energy were made in amorphous sucrose-additive films containing the probe erythrosin B. Results showed the complex effects of additives on the mobility in a hydrogen-bonded sugar matrix. Glycerol exhibited an antiplasticization effect shown as decreased mobility at glycerol/sucrose mole ratio ≤ 0.27 and at temperature ≤ 45° C. On the contrary, all the polymers studied, including gelatin, xanthan and high amylose starch, displayed a ‘plasticization’ effect (increasing mobility) at very low while a rigidification effect (decreasing mobility) at higher concentration without significant change in Tg. Maltodextrins, mixtures of molecules with a variety of molecular weights, increase the mobility in spite of their high Tg. Sodium chloride showed a strong rigidification effect on the sucrose matrix; however, this effect was weakened at mole ratio NaCl/sucrose above 0.5. Other salts showed effects resulting from a compromise between two opposite actions (decreasing mobility due to salt itself and increasing mobility due to absorbed moisture). All above behaviors are difficult to interpret using Tg alone. Molecular mobility appears to be more accurate to evaluate the physical stability of the matrix.
Phosphorescence of erythrosin B was also able to report dynamic site heterogeneity that is an intrinsic property of the amorphous solid state. The heterogeneity was be evaluated by the variation of lifetime and lifetime heterogeneity across the excitation and emission band and the temperature dependence of bandwidth and lifetime heterogeneity. The composition influence on the dynamic site heterogeneity was discussed as well.
Note
(type = degree)
Ph.D.
Note
(type = bibliography)
Includes bibliographical references.
Subject
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Topic
Food Science
Subject
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Topic
Molecular dynamics
Subject
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Topic
Amorphous substances
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Title
Graduate School - New Brunswick Electronic Theses and Dissertations
Identifier
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rucore19991600001
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http://hdl.rutgers.edu/1782.2/rucore10001600001.ETD.17034
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ETD_288
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Identifier
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doi:10.7282/T3930THK
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ETD doctoral
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Copyright protected
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Open
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Yumin You
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Affiliation
Rutgers University. Graduate School - New Brunswick
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Non-exclusive ETD license
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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.
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