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Understanding molecular and thermodynamic miscibility of carbohydrate biopolymers
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Understanding molecular and thermodynamic miscibility of carbohydrate biopolymers
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Icoz
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Didem
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Didem Icoz
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author
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Kokini
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Jozef
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Advisory Committee
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Jozef L. Kokini
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chair
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Takhistov
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Paul
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Paul Takhistov
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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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Cuitino
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Alberto
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Advisory Committee
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Alberto Cuitino
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Rutgers University
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Graduate School - New Brunswick
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theses
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2008
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2008-05
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English
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electronic
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xx, 249 pages
Abstract
Most food materials are composed of polymeric molecules with different chemistry and properties. Increasing demand for food products with new/improved functionalities require formulations to include/exclude ingredients. Processability, texture, stability and palatability of the food products are greatly influenced by interactions and miscibility/immiscibility between these polymeric components. Molecular and thermodynamic basis of these phenomena are still not well understood and are the focus of scientific debate. A set of quantitative predictive rules are needed to be developed.
The major objective of this dissertation was to fundamentally understand the molecular and thermodynamic basis of miscibility and to develop quantitative miscibility predictions for carbohydrate mixtures. Dextrans (glucose polymers) with different molecular weights (Mw) and chemically derivatized forms were used as model carbohydrate polymers. Thermal analysis on individual and mixtures of standard dextrans showed that physical blend of dextrans was immiscible due to the diffusion barrier, whereas freeze-dried solution of these dextrans was miscible. In the mixtures of chemically derivatized dextrans, thermal analysis showed miscible or immiscible systems depending on the concentration and ionic strength through addition of salt. Systematic differences in the FTIR spectra of miscible systems with different component ratios were assigned to the change in hydrogen-bonding distribution resulting from changes in intra- and inter-molecular interactions, whereas FTIR spectra of immiscible systems didn't show such systematic changes, indicating insufficient hydrogen-bonding to form miscible systems.
In order to quantitatively predict miscibility, first, a methodology was developed to determine solubility parameters of dextrans with different Mw using their Tg. Using these solubility parameters, thermodynamic ideas based on the number of configurational arrangements and quantitative measures of dispersive interactions (Flory-Huggins theory) were demonstrated to be insufficient to quantitatively explain the miscibility in carbohydrate systems. This failure was due to the limitation of these ideas in underestimating the effect of specific bonding interactions, including hydrogen-bonds. A more advanced framework, Painter-Coleman association model, quantitatively demonstrated that hydrogen-bonding significantly contributed to predictive miscibility in carbohydrate systems. It was shown that with appropriate approximations it was possible to successfully predict miscibility in dextran systems. The quantitative understanding gained with dextrans was validated on real carbohydrate systems by testing miscibility/immiscibility in inulin-amylopectin systems.
The major objective of this dissertation was to fundamentally understand the molecular and thermodynamic basis of miscibility and to develop quantitative miscibility predictions for carbohydrate mixtures. Dextrans (glucose polymers) with different molecular weights (Mw) and chemically derivatized forms were used as model carbohydrate polymers. Thermal analysis on individual and mixtures of standard dextrans showed that physical blend of dextrans was immiscible due to the diffusion barrier, whereas freeze-dried solution of these dextrans was miscible. In the mixtures of chemically derivatized dextrans, thermal analysis showed miscible or immiscible systems depending on the concentration and ionic strength through addition of salt. Systematic differences in the FTIR spectra of miscible systems with different component ratios were assigned to the change in hydrogen-bonding distribution resulting from changes in intra- and inter-molecular interactions, whereas FTIR spectra of immiscible systems didn't show such systematic changes, indicating insufficient hydrogen-bonding to form miscible systems.
In order to quantitatively predict miscibility, first, a methodology was developed to determine solubility parameters of dextrans with different Mw using their Tg. Using these solubility parameters, thermodynamic ideas based on the number of configurational arrangements and quantitative measures of dispersive interactions (Flory-Huggins theory) were demonstrated to be insufficient to quantitatively explain the miscibility in carbohydrate systems. This failure was due to the limitation of these ideas in underestimating the effect of specific bonding interactions, including hydrogen-bonds. A more advanced framework, Painter-Coleman association model, quantitatively demonstrated that hydrogen-bonding significantly contributed to predictive miscibility in carbohydrate systems. It was shown that with appropriate approximations it was possible to successfully predict miscibility in dextran systems. The quantitative understanding gained with dextrans was validated on real carbohydrate systems by testing miscibility/immiscibility in inulin-amylopectin systems.
Note
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Ph.D.
Note
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Includes bibliographical references (p. 237-247).
Subject
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Topic
Food Science
Subject
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Topic
Carbohydrates
Subject
(ID = SUBJ3);
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Topic
Biopolymers
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Graduate School - New Brunswick Electronic Theses and Dissertations
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doi:10.7282/T3XD1218
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ETD doctoral
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Didem Icoz
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Rutgers University. Graduate School - New Brunswick
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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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