Material Type  

 학위논문

 

0017162456

Date and Time of Latest Transaction  

20250211152014

ISBN  

9798384049104

DDC  

540

Author  

Mandel, Ruth Michelle.

Title/Author  

Controlling Toxic Gas Capture and Delivery in Metal-Organic Frameworks: From Chlorine to Hydrogen Sulfide.

Publish Info  

[S.l.] : Cornell University., 2024

Publish Info  

Ann Arbor : ProQuest Dissertations & Theses, 2024

Material Info  

458 p.

General Note  

Source: Dissertations Abstracts International, Volume: 86-03, Section: B.

General Note  

Advisor: Milner, Phillip.

학위논문주기  

Thesis (Ph.D.)--Cornell University, 2024.

Abstracts/Etc  

요약The development of materials for the efficient capture and delivery of toxic gases is crucial in both mitigating harmful emissions streams and enabling the safe storage and delivery of these gases for use in industry and medicine. Porous materials, specifically metal-organic frameworks (MOFs), represent a better alternative to molecular systems in attaining this goal through their structural tunability and precisely controlled gas-adsorbent interactions. Here, we describe efforts to design MOF-based systems for the irreversible capture of toxic chlorine (Cl2) gas and the reversible adsorption of hydrogen sulfide (H2S) gas for therapeutic delivery.We begin by reporting the first examples of irreversible Cl2 capture via the dichlorination of alkene linkages in zirconium-based MOFs. As a toxic and corrosive gas that is both an essential reagent in industry and a potent chemical warfare agent, Cl2 mitigation is needed for industrial and civilian personal protective equipment (PPE). MOFs constructed from alkene linkers were found to retain long-range order and accessible porosity after alkene dichlorination and could capture Cl2 at low partial pressures. Our results ultimately support that alkene dichlorination represents a new pathway for reactive Cl2 capture, introducing new opportunities for binding this gas irreversibly in PPE. We then proceed to review the emerging use of porous materials to deliver gases relevant to medicine, biomedical imaging, and pharmaceutical synthesis. Specific topics include MOFs and zeolites as solid-state sources of the gasotransmitter H2S, xenon-129 for magnetic resonance imaging, oxygen gas for the treatment of cancer and hypoxia, and various synthetically relevant gases prevalent in organic synthesis.We focus next on therapeutic H2S delivery in MOFs. H2S is an endogenous gasotransmitter with potential therapeutic value for treating a range of disorders, such as ischemia-reperfusion injury (IRI) resulting from a myocardial infarction or stroke. However, the medicinal delivery of H2S is hindered by its corrosive and toxic nature. In addition, small-molecule H2S donors often generate other reactive species upon H2S release, leading to unwanted side effects. We demonstrate that H2S release from biocompatible MOFs is a promising alternative strategy for H2S delivery under physiologically relevant conditions. These zirconium-based MOFs retain crystallinity and porosity after H2S adsorption and can deliver the gas to mitigate IRI-related injuries in rat cardiomyoblast cells using an in vitro model. Finally, we expand beyond zirconium-based MOFs and consider other framework materials that can bind H2S more strongly for transdermal delivery through porcine skin as a treatment of skin pathologies and wound healing. These studies intend to highlight the advantages of a MOF-based approach to harnessing toxic gases and demonstrate the potential for further adoption of these systems into the industrial and medicinal communities.

Subject Added Entry-Topical Term  

Chemistry.

Subject Added Entry-Topical Term  

Biomedical engineering.

Subject Added Entry-Topical Term  

Medical imaging.

Subject Added Entry-Topical Term  

Biochemistry.

Index Term-Uncontrolled  

Chlorine

Index Term-Uncontrolled  

Hydrogen sulfide

Index Term-Uncontrolled  

Metal-organic frameworks

Index Term-Uncontrolled  

Toxic gases

Index Term-Uncontrolled  

Ischemia-reperfusion injury

Added Entry-Corporate Name  

Cornell University Chemistry and Chemical Biology

Host Item Entry  

Dissertations Abstracts International. 86-03B.

Electronic Location and Access  

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Control Number  

joongbu:654675