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Enzyme-Containing Liquid Crystal Pol...

Velasco Abadia, Albert.

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Enzyme-Containing Liquid Crystal Polymer Networks and Elastomers as Biomolecular-Responsive Actuators.

紀錄類型:	書目-電子資源 : Monograph/item
正題名/作者:	Enzyme-Containing Liquid Crystal Polymer Networks and Elastomers as Biomolecular-Responsive Actuators./
作者:	Velasco Abadia, Albert.
出版者:	Ann Arbor : ProQuest Dissertations & Theses, : 2023,
面頁冊數:	199 p.
附註:	Source: Dissertations Abstracts International, Volume: 85-03, Section: B.
Contained By:	Dissertations Abstracts International85-03B.
標題:	Bioengineering. -
電子資源:	https://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=30574291
ISBN:	9798380167956

Enzyme-Containing Liquid Crystal Polymer Networks and Elastomers as Biomolecular-Responsive Actuators.
Velasco Abadia, Albert.

Enzyme-Containing Liquid Crystal Polymer Networks and Elastomers as Biomolecular-Responsive Actuators. - Ann Arbor : ProQuest Dissertations & Theses, 2023 - 199 p.

Source: Dissertations Abstracts International, Volume: 85-03, Section: B.

Thesis (Ph.D.)--University of Colorado at Boulder, 2023.

Stimuli-responsive materials, which readily respond to a plethora of signals such as heat, light, electrical fields or chemical triggers are at the forefront of modern material science, finding applicability in fields as disparate as tunable textiles or autonomous robots. In particular, liquid crystal polymer networks (LCNs) and elastomers (LCEs) have emerged as powerful smart materials by virtue of their ability to display anisotropic responses given their intrinsic tendency to form ordered phases. LCNs and LCEs can change shape, stiffness or color on demand, which makes them potential candidates for biological applications that require materials that continuously adapt to their surroundings, such as anti-fouling surfaces or shape-changing medical implants. While there is a plethora of examples of LC materials that respond to broad chemical stimuli (e.g., pH or humidity), it is of interest to develop LCNs and LCEs that can sense and actuate upon the detection of specific biochemical stimuli, which may open the door to the use of such materials in new and exciting applications.In this work, we proposed the incorporation of enzymes into chemically responsive LCNs and LCEs as a way to impart them with sensitivity to specific biochemical stimuli. We hypothesized that the immobilized enzyme would effectively act as a molecular transducer, sensitizing the material to a chemical signal by converting the original signal to a stimulus to which the polymer responds. Upon detection of the enzymatic substrate, the films would then undergo a shape reconfiguration, with the final shape controlled either by the orientation of the liquid crystal director field or the localization of the chemical response via enzyme patterning. First, tailor-made enzyme immobilization chemical strategies were devised, implemented and optimized. Fluorination of carboxylic acids, attachment via a bismaleimide homobifunctional linker or glutaraldehyde-mediated crosslinking were used depending on the LCN/LCE chemistry and the characteristics of the immobilized enzyme. Then, the loading, activity and stability of attached enzymes were thoroughly characterized, which was critical to ensure that films would respond in a reproducible and predictable manner. This was performed using a diverse set of techniques such as FTIR, confocal laser scanning microscopy or biochemical assays. Finally, the mechanical response of the films to the detection of the biochemical substrates was studied, including how the concentration and the exposure time (among other factors) influence the magnitude of the response. More specifically, urease-containing flat films transformed into curls, arches or accordions upon exposure to urea. Moreover, 3D printing was used to make yellow disks that simultaneously changed color and shape to red cones upon exposure to stimuli as diverse as lipids, carbohydrates or peptides. Lastly, the use of an enzyme-containing LCE as a field-deployable pesticide biosensor was studied. Ultimately, this work constitutes the establishment of a versatile platform of biochemically responsive actuators for use in biological applications.

ISBN: 9798380167956Subjects--Topical Terms:

657580
Bioengineering.
Subjects--Index Terms:

Liquid crystal polymer networks

Enzyme-Containing Liquid Crystal Polymer Networks and Elastomers as Biomolecular-Responsive Actuators.
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300 $a 199 p.
500 $a Source: Dissertations Abstracts International, Volume: 85-03, Section: B.
500 $a Includes supplementary digital materials.
500 $a Advisor: Kaar, Joel L.;Schwartz, Daniel K.
502 $a Thesis (Ph.D.)--University of Colorado at Boulder, 2023.
520 $a Stimuli-responsive materials, which readily respond to a plethora of signals such as heat, light, electrical fields or chemical triggers are at the forefront of modern material science, finding applicability in fields as disparate as tunable textiles or autonomous robots. In particular, liquid crystal polymer networks (LCNs) and elastomers (LCEs) have emerged as powerful smart materials by virtue of their ability to display anisotropic responses given their intrinsic tendency to form ordered phases. LCNs and LCEs can change shape, stiffness or color on demand, which makes them potential candidates for biological applications that require materials that continuously adapt to their surroundings, such as anti-fouling surfaces or shape-changing medical implants. While there is a plethora of examples of LC materials that respond to broad chemical stimuli (e.g., pH or humidity), it is of interest to develop LCNs and LCEs that can sense and actuate upon the detection of specific biochemical stimuli, which may open the door to the use of such materials in new and exciting applications.In this work, we proposed the incorporation of enzymes into chemically responsive LCNs and LCEs as a way to impart them with sensitivity to specific biochemical stimuli. We hypothesized that the immobilized enzyme would effectively act as a molecular transducer, sensitizing the material to a chemical signal by converting the original signal to a stimulus to which the polymer responds. Upon detection of the enzymatic substrate, the films would then undergo a shape reconfiguration, with the final shape controlled either by the orientation of the liquid crystal director field or the localization of the chemical response via enzyme patterning. First, tailor-made enzyme immobilization chemical strategies were devised, implemented and optimized. Fluorination of carboxylic acids, attachment via a bismaleimide homobifunctional linker or glutaraldehyde-mediated crosslinking were used depending on the LCN/LCE chemistry and the characteristics of the immobilized enzyme. Then, the loading, activity and stability of attached enzymes were thoroughly characterized, which was critical to ensure that films would respond in a reproducible and predictable manner. This was performed using a diverse set of techniques such as FTIR, confocal laser scanning microscopy or biochemical assays. Finally, the mechanical response of the films to the detection of the biochemical substrates was studied, including how the concentration and the exposure time (among other factors) influence the magnitude of the response. More specifically, urease-containing flat films transformed into curls, arches or accordions upon exposure to urea. Moreover, 3D printing was used to make yellow disks that simultaneously changed color and shape to red cones upon exposure to stimuli as diverse as lipids, carbohydrates or peptides. Lastly, the use of an enzyme-containing LCE as a field-deployable pesticide biosensor was studied. Ultimately, this work constitutes the establishment of a versatile platform of biochemically responsive actuators for use in biological applications.
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650 4 $a Polymer chemistry. $3 3173488
650 4 $a Materials science. $3 543314
653 $a Liquid crystal polymer networks
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653 $a Biochemically responsive actuators
653 $a Stimuli-responsive materials
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