Li, Tao
(2014)
DESIGN AND MODULATION OF ADENINE BASED METAL-ORGANIC FRAMEWORKS AND EXPLORATION OF THEIR NEW PROPERTIES.
Doctoral Dissertation, University of Pittsburgh.
(Unpublished)
Abstract
This dissertation describes the development of adenine-based biomolecular metal-organic frameworks (Bio-MOFs). Four specific topics are presented: 1) design of new bio-MOFs for CO2 capture; 2) preparation of core-shell bio-MOFs with enhanced properties; 3) development of new synthetic strategies for increasing bio-MOF porosity; and 4) exploration of new applications of mesoporous bio-MOFs.
Specifically, Chapter 2 reports the preparation of an isoreticular series of cobalt-adeninate bio-MOFs (bio-MOFs-11-14). The pores of bio-MOFs-11-14 are decorated with linear aliphatic pendant groups (acetate, propionate, butyrate, and valerate). The new materials exhibit higher CO2/N2 selectivity and greatly improved water stability. Based on the findings in Chapter 2, Chapter 3 describes the design of a core-shell material comprising a porous bio-MOF-11/14 mixed core and a less porous bio-MOF-14 shell. The resulting core-shell material successfully combined the merits of bio-MOF-11 and 14 and exhibits higher CO2 capacity, the ability to exclude N2, and improved water stability. Chapter 4 demonstrates the use of in situ ligand exchange as a synthetic strategy for the preparation of an isoreticular series of zinc-adeninate bio-MOFs (bio-MOFs-100-103) exhibiting exclusive mesoporosity. Following the work in Chapter 4, Chapter 5 presents the use of these exclusively mesoporous bio-MOFs for the separation of thiolated gold nanoclusters. This is the first demonstration of large species separation using MOFs.
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| Item Type: |
University of Pittsburgh ETD
|
| Status: |
Unpublished |
| Creators/Authors: |
|
| ETD Committee: |
|
| Date: |
31 January 2014 |
| Date Type: |
Publication |
| Defense Date: |
15 October 2013 |
| Approval Date: |
31 January 2014 |
| Submission Date: |
27 November 2013 |
| Access Restriction: |
No restriction; Release the ETD for access worldwide immediately. |
| Number of Pages: |
272 |
| 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 framework, bio-MOF, ligand exchange, core-shell, CO2 capture |
| Date Deposited: |
31 Jan 2015 06:00 |
| Last Modified: |
15 Nov 2016 14:16 |
| URI: |
http://d-scholarship.pitt.edu/id/eprint/20116 |
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