Publication Date

2015-08-06

Availability

Open access

Embargo Period

2015-08-06

Degree Type

Dissertation

Degree Name

Doctor of Philosophy (PHD)

Department

Chemistry (Arts and Sciences)

Date of Defense

2015-07-21

First Committee Member

Marc R. Knecht

Second Committee Member

Roger LeBlanc

Third Committee Member

Angel Kaifer

Fourth Committee Member

Onur Tigli

Abstract

Nature possesses methods for the formation and manipulation of inorganic materials with controlled size, shape, and compositions. Biomolecules, such as peptides, are known to be responsible for the generation of such inorganic materials on the nanoscale, where the enhanced properties can be exploited for various applications. Pd nanoparticles, capped with the Pd-specific Pd4 peptide (TSNAVHPTLRHL), were found to be active catalysts for Stille coupling, where the debated mechanism of oxidative addition was explored. Furthermore, the same Pd4-capped nanoparticles were found to be active in Suzuki coupling, another C-C coupling reaction that undergoes catalysis following a similar mechanism. Other considerations with peptide-capped metal catalysis involved the role of the reductant and the subsequent effects on morphology and reactivity, as seen by use of Au nanoparticles capped with a library of peptides. The role of the reductant was studied using varied reductants and was found to directly affect the catalytic activity. Additionally, such Au and Ag materials-binding peptides were expanded to generate multi-domain biomolecules capable of metal-specific binding and nanoparticle assembly. Such in-depth studies of peptide-capped nanomaterials and their uses in catalysis and assembly is important for optimized functionality and application.

Keywords

Nanoparticles; peptides; biomimetic; C-C coupling; leaching; bionanocombinatorics

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