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Polymers and Metal-Organic Framework...

Zhang, Wenyu.

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Polymers and Metal-Organic Frameworks Containing Mechanically Interlocked Components.

紀錄類型:	書目-語言資料,印刷品 : Monograph/item
正題名/作者:	Polymers and Metal-Organic Frameworks Containing Mechanically Interlocked Components./
作者:	Zhang, Wenyu.
面頁冊數:	141 p.
附註:	Source: Dissertation Abstracts International, Volume: 72-03, Section: B, page: 1508.
Contained By:	Dissertation Abstracts International72-03B.
標題:	Chemistry, Organic. -
電子資源:	http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=3441515
ISBN:	9781124450575

Polymers and Metal-Organic Frameworks Containing Mechanically Interlocked Components.
Zhang, Wenyu.

Polymers and Metal-Organic Frameworks Containing Mechanically Interlocked Components. - 141 p.

Source: Dissertation Abstracts International, Volume: 72-03, Section: B, page: 1508.

Thesis (Ph.D.)--University of California, Los Angeles, 2010.

Mechanically interlocked molecules (MIMs), such as bistable catenanes and bistable rotaxanes, have been used to bring about actuation in nanoelectromechanical systems and molecular electronic devices. The elaboration of the structural features of MIMs into polymers and metal-organic frameworks (MOFs) might allow the utilization of molecular motion to impact the bulk properties of the solid-state materials. This dissertation describes successful attempts in realizing such concept. First of all, polymers which contain pi-electron-donating 1,5-dioxynaphthalene (DNP) units encircled by cyclobis-(paraquat- p-phenylene) (CBPQT4+), a pi electron-accepting tetracationic cyclophane, synthesized by using the copper(I)-catalyzed azide-alkyne cycloaddition (CuAAC) was reported. These poly[n]rotaxanes adopt a well-defined "folded" secondary structure by virtue of the judicious design of two DNP-containing monomers with different binding affinities for CBPQT4+. Secondly, obtained by a similar approach, a poly[ n]rotaxane containing alternating DNP and tetrathiofulvalene (TTF) units encircled by CBPQT4+ rings was studied, which shows reversible bistability controlled by electrochemical redox processes. The poly[ n]rotaxane was incorporated into solid-state devices by means of spin-coating, which exhibit switching behavior depending on electrode choices. In order to extend the exploration to the area of MOFs, rigid organic dicarboxylic acids containing crown ethers were synthesized. These novel compounds retain the characteristics of their parent crown ethers since they can bind cationic guests and serve as templates for making MIMs. The binding behavior of BPP34C10DA with the paraquat dication (PQT2+) has been investigated, and the BPP34C10DA-based [2]catenane (H2BPP34C10DC-CAT) were prepared. The former was used to synthesize MOF-1001, which adopts the primitive cubic structure and is capable of docking PQT2+ guests within the macrocycles in a stereoelectronically controlled fashion. The latter was used to construct MOF-1011, whose two-dimensional layered structure contains [2]catenanes in an extremely dense and highly ordered fashion. These studies not only represent efficient approaches to the preparation of polymers and metal-organic frameworks with previously undescribed functionalities, but also set the stage for the development of next-generation solid-state materials with unprecedented complex functions.

ISBN: 9781124450575Subjects--Topical Terms:

516206
Chemistry, Organic.

Polymers and Metal-Organic Frameworks Containing Mechanically Interlocked Components.
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520 $a Mechanically interlocked molecules (MIMs), such as bistable catenanes and bistable rotaxanes, have been used to bring about actuation in nanoelectromechanical systems and molecular electronic devices. The elaboration of the structural features of MIMs into polymers and metal-organic frameworks (MOFs) might allow the utilization of molecular motion to impact the bulk properties of the solid-state materials. This dissertation describes successful attempts in realizing such concept. First of all, polymers which contain pi-electron-donating 1,5-dioxynaphthalene (DNP) units encircled by cyclobis-(paraquat- p-phenylene) (CBPQT4+), a pi electron-accepting tetracationic cyclophane, synthesized by using the copper(I)-catalyzed azide-alkyne cycloaddition (CuAAC) was reported. These poly[n]rotaxanes adopt a well-defined "folded" secondary structure by virtue of the judicious design of two DNP-containing monomers with different binding affinities for CBPQT4+. Secondly, obtained by a similar approach, a poly[ n]rotaxane containing alternating DNP and tetrathiofulvalene (TTF) units encircled by CBPQT4+ rings was studied, which shows reversible bistability controlled by electrochemical redox processes. The poly[ n]rotaxane was incorporated into solid-state devices by means of spin-coating, which exhibit switching behavior depending on electrode choices. In order to extend the exploration to the area of MOFs, rigid organic dicarboxylic acids containing crown ethers were synthesized. These novel compounds retain the characteristics of their parent crown ethers since they can bind cationic guests and serve as templates for making MIMs. The binding behavior of BPP34C10DA with the paraquat dication (PQT2+) has been investigated, and the BPP34C10DA-based [2]catenane (H2BPP34C10DC-CAT) were prepared. The former was used to synthesize MOF-1001, which adopts the primitive cubic structure and is capable of docking PQT2+ guests within the macrocycles in a stereoelectronically controlled fashion. The latter was used to construct MOF-1011, whose two-dimensional layered structure contains [2]catenanes in an extremely dense and highly ordered fashion. These studies not only represent efficient approaches to the preparation of polymers and metal-organic frameworks with previously undescribed functionalities, but also set the stage for the development of next-generation solid-state materials with unprecedented complex functions.
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