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Metal-Organic Framework Platforms: Diversity-Oriented Synthesis and Application-Directed Custom Design

Luo, Tianyi (2020) Metal-Organic Framework Platforms: Diversity-Oriented Synthesis and Application-Directed Custom Design. Doctoral Dissertation, University of Pittsburgh. (Unpublished)

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This dissertation describes diversity-oriented development of metal-organic framework (MOF) platforms and their custom design for specific applications. The three aims of this dissertation include: 1) construct MOF material platforms with exceptional amenability to systematic variations via de novo design; 2) develop new strategies to further increase the diversity and complexity of established MOF platforms; 3) custom-design MOF materials for target applications based on judiciously adjustment on structural parameters of established MOF platforms.
The work in Chapter 2 describes the de novo design of a diverse series of rare earth MOF materials amenable to rational and systematic control of topology, structural metrics, functionalization and inorganic compositions. The optical properties of these MOFs can be customized for potential near infrared (NIR) biological imaging. Chapter 3 describes the custom-design of lanthanide MOF materials as luminescence “turn-on” sensors for gossypol, a natural toxin concerning the cotton industry. The ability to judiciously control the inorganic composition, structural metrics as well as functionalities with the employed lanthanide MOF platform allows for the observed sensing performance and insight into the sensing mechanism. Chapter 4 introduces the concept of domain building blocks (DBBs) as an effective approach to create additional levels of diversity and complexity in MOF platforms. DBBs are defined as distinct structural or compositional regions within a MOF material. I demonstrate that the DBB strategy can be used in conjunction with post-synthetic modification and nanoparticle encapsulation to construct a rich library of UiO-67 stratified MOF (sMOF) particles consisting of multiple concentric DBBs. I further discuss the negative consequences of linker exchange reactions during sMOFs synthesis on the compositional integrity of DBBs in the UiO-67 sMOFs and propose mitigation strategies. In Chapter 5, the application of MOFs as adsorbent materials for chemical warfare agents (CWAs) is explored. A combined experimental and computational study shows that tailoring the functional groups of UiO-67 MOFs can influence their binding energy for dimethyl methylphosphonate (DMMP), a CWA adsorption simulant.


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Item Type: University of Pittsburgh ETD
Status: Unpublished
CreatorsEmailPitt UsernameORCID
Luo, Tianyitil27@pitt.edutil270000-0002-9973-9328
ETD Committee:
TitleMemberEmail AddressPitt UsernameORCID
Committee ChairRosi,
Committee MemberMillstone,
Committee MemberLiu,
Committee MemberWilmer,
Date: 16 January 2020
Date Type: Publication
Defense Date: 28 October 2019
Approval Date: 16 January 2020
Submission Date: 18 October 2019
Access Restriction: 2 year -- Restrict access to University of Pittsburgh for a period of 2 years.
Number of Pages: 338
Institution: University of Pittsburgh
Schools and Programs: Dietrich School of Arts and Sciences > Chemistry
Degree: PhD - Doctor of Philosophy
Thesis Type: Doctoral Dissertation
Refereed: Yes
Uncontrolled Keywords: Metal-Organic Frameworks
Date Deposited: 16 Jan 2021 06:00
Last Modified: 16 Jan 2022 06:15

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