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Structural effects on encapsulation ...

Chasse, Tyson Lee.

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Structural effects on encapsulation as probed in solution-based and surface-confined redox-active core dendrimers.

紀錄類型:	書目-電子資源 : Monograph/item
正題名/作者:	Structural effects on encapsulation as probed in solution-based and surface-confined redox-active core dendrimers./
作者:	Chasse, Tyson Lee.
面頁冊數:	149 p.
附註:	Source: Dissertation Abstracts International, Volume: 65-01, Section: B, page: 0234.
Contained By:	Dissertation Abstracts International65-01B.
標題:	Chemistry, Physical. -
電子資源:	http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=3120222
ISBN:	049667594X

Structural effects on encapsulation as probed in solution-based and surface-confined redox-active core dendrimers.
Chasse, Tyson Lee.

Structural effects on encapsulation as probed in solution-based and surface-confined redox-active core dendrimers. - 149 p.

Source: Dissertation Abstracts International, Volume: 65-01, Section: B, page: 0234.

Thesis (Ph.D.)--North Carolina State University, 2004.

The purpose of this research was to study structure - property relationships of iron-sulfur core [Fe4S4(S-Dend)4] 2- dendrimers. Previous studies have demonstrated that biasing dendrimer architecture increases the effective encapsulation of redox-active, Fe4S4 clusters. To further examine structure-property relationships of iron-sulfur core dendrimers, studies were carried out to (1) probe the relationship between dendritic architecture and encapsulation via the study of solution-based and surface-confined constitutional isomers differing only in their benzyl substitution patterns, and (2) studying the effects of counterion concentration and permeability on the electronic properties of iron-sulfur core dendrimer thin films.

ISBN: 049667594XSubjects--Topical Terms:

560527
Chemistry, Physical.

Structural effects on encapsulation as probed in solution-based and surface-confined redox-active core dendrimers.
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245 1 0 $a Structural effects on encapsulation as probed in solution-based and surface-confined redox-active core dendrimers.
300 $a 149 p.
500 $a Source: Dissertation Abstracts International, Volume: 65-01, Section: B, page: 0234.
500 $a Director: Christopher B. Gorman.
502 $a Thesis (Ph.D.)--North Carolina State University, 2004.
520 $a The purpose of this research was to study structure - property relationships of iron-sulfur core [Fe4S4(S-Dend)4] 2- dendrimers. Previous studies have demonstrated that biasing dendrimer architecture increases the effective encapsulation of redox-active, Fe4S4 clusters. To further examine structure-property relationships of iron-sulfur core dendrimers, studies were carried out to (1) probe the relationship between dendritic architecture and encapsulation via the study of solution-based and surface-confined constitutional isomers differing only in their benzyl substitution patterns, and (2) studying the effects of counterion concentration and permeability on the electronic properties of iron-sulfur core dendrimer thin films.
520 $a Three pairs of isomeric, iron-sulfur core dendrimers were synthesized. Each isomer pair was distinguished by a 3,5- (extended) and 2,6- (backfolded) aromatic substitution pattern. Several observations were made supporting the hypothesis that the iron-sulfur cluster cores were encapsulated more effectively in the backfolded isomers as compared to their extended counterparts. The backfolded isomers were more difficult to reduce electrochemically, consistent with encapsulation in a less-polar microenvironment. Furthermore, heterogeneous electron-transfer rates for the backfolded molecules were attenuated compared to the extended molecules. From diffusion measurements obtained by pulsed field gradient spin-echo NMR and chronoamperometry, the backfolded dendrimers were found to be smaller than the extended dendrimers. Comparison of longitudinal proton relaxation (T1) time constants also indicated a smaller, compact dendrimer conformation for the backfolded architectures. These findings indicated dendrimer size was not the primary factor in determining electron-transfer rate. Instead, the effective electron-transfer distance, determined by relative core position and mobility, was most relevant for encapsulation.
520 $a In addition to solution studies, the electrochemical behavior of thin films composed of iron-sulfur core dendrimers were studied as a function of the type of counterion available during reduction and re-oxidation. The rate of permeation/migration of counterions into the film appeared to be the bottleneck to electron transfer through the film. As the dendrimer is essentially non-polar, decreasing the relative polarity of the counterion increased the rate and extent of electron hopping within the films.
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790 1 0 $a Gorman, Christopher B., $e advisor
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