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The synthesis and characterization o...

Defreese, Jessica Lynn.

The synthesis and characterization of confined imprinted binding and catalytic sites in bulk silica.

紀錄類型:	書目-電子資源 : Monograph/item
正題名/作者:	The synthesis and characterization of confined imprinted binding and catalytic sites in bulk silica.
作者:	Defreese, Jessica Lynn.
面頁冊數:	120 p.
附註:	Chair: Alexander Katz.
附註:	Source: Dissertation Abstracts International, Volume: 66-08, Section: B, page: 4354.
Contained By:	Dissertation Abstracts International66-08B.
標題:	Engineering, Chemical.
電子資源:	http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=3187015
ISBN:	9780542293368

The synthesis and characterization of confined imprinted binding and catalytic sites in bulk silica.
Defreese, Jessica Lynn.

The synthesis and characterization of confined imprinted binding and catalytic sites in bulk silica. - 120 p.

Chair: Alexander Katz.

Thesis (Ph.D.)--University of California, Berkeley, 2005.

A primary premise of imprinting is confinement, in which the templated pocket forms so closely to the imprint as to impart solid-state characteristics in terms of imprint mobility. In previous systems over the past sixty years, existence of confined imprinted pockets has been inferred indirectly through binding experiments. This work rigorously characterizes the immobilized imprints' molecular motion, doing so on three different classes of imprinted materials using solid-state NMR techniques. The results prove local imprint confinement within bulk microporous and mesoporous materials in comparison to post-synthetically grafted two dimensional surface and are the first to demonstrate that bulk synthesis can provide a degree of confinement that is unattainable via modification of preexisting surfaces.

ISBN: 9780542293368Subjects--Topical Terms:

226989
Engineering, Chemical.

The synthesis and characterization of confined imprinted binding and catalytic sites in bulk silica.
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245 1 4 $a The synthesis and characterization of confined imprinted binding and catalytic sites in bulk silica.
300 $a 120 p.
500 $a Chair: Alexander Katz.
500 $a Source: Dissertation Abstracts International, Volume: 66-08, Section: B, page: 4354.
502 $a Thesis (Ph.D.)--University of California, Berkeley, 2005.
520 # $a A primary premise of imprinting is confinement, in which the templated pocket forms so closely to the imprint as to impart solid-state characteristics in terms of imprint mobility. In previous systems over the past sixty years, existence of confined imprinted pockets has been inferred indirectly through binding experiments. This work rigorously characterizes the immobilized imprints' molecular motion, doing so on three different classes of imprinted materials using solid-state NMR techniques. The results prove local imprint confinement within bulk microporous and mesoporous materials in comparison to post-synthetically grafted two dimensional surface and are the first to demonstrate that bulk synthesis can provide a degree of confinement that is unattainable via modification of preexisting surfaces.
520 # $a Although the synthetic technique of imprinting provides promising routes for control of selective heterogeneous catalysts and adsorption, a number of challenges that are essential for certain applications have remained outside the realm of possibility. These include rigorous characterization of molecular confinement within imprinted pockets, development of hierarchical porosity in imprinted materials, and incorporation of chirality within confined imprinted pockets. This work address the challenges above by enabling the synthesis of new classes of imprinted materials and exploring the local nature of the active site and its related resolution for performing selective molecular recognition.
520 # $a The synthesis and characterization of the mesoporous material is the first of a new class of bulk imprinted silica to contain the hierarchical porosity of imprinted micropores imbedded with a bulk mesoporous network. FT-IR experiments suggest hydrogen-bonding interactions between the bulk network and immobilized imprint that facilitate formation of the templated pocket.
520 # $a With demonstration of confinement, the imprinted pockets synthesized upon imprint deprotection are shown to enable shape-selective discrimination in the covalent rebinding of two homologous molecular probes that differ in size by approximately 2.4 A. Enantioselectivity of the imprinted materials for covalent rebinding is investigated in two situations: one-point binding in a chiral pocket and one-point binding to a chiral inductor in a confined imprinted pocket. The latter required the design and synthesis of chiral imprinted active sites, which have also been characterized and found to be catalytically active and accessible.
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