Publication Date

2013-04-11

Availability

Open access

Embargo Period

2013-04-11

Degree Type

Dissertation

Degree Name

Doctor of Philosophy (PHD)

Department

Chemistry (Arts and Sciences)

Date of Defense

2013-03-28

First Committee Member

Marc R. Knecht

Second Committee Member

Roger M. Leblanc

Third Committee Member

Rajeev Prabhakar

Fourth Committee Member

Onur Tigli

Abstract

Bio-inspired nanoparticle catalysis offers the opportunity to improve on current catalytic standards with respect to turnover efficiency, organic solvent use, and thermal activation. Unfortunately, projected energy demands will soon outweigh our fuel supplies. The task of creating multifunctional catalysts that both lower thermal activation and possess a number of functions in aqueous conditions is daunting. Similar to these needs, nature has evolved to create a wide range of highly specialized catalytic processes, which incorporate inorganic materials, take place in ambient temperatures, and in an aqueous environment. These specialized biological systems provide inspiration, but are not applicable to current needs. Exploitation of these biotic-abiotic systems could allow for green, multifunctional catalysts. In the resulting works, a peptide sequence has been isolated via phage display with affinity for Pd surfaces, that forms stable, peptide-capped nanoparticles. Substitution of residues results in the tuning of both nanocatalyst activity and nanoparticle size, such that a peptide surface-controlling effect can be noted. These characteristics can be exploited to ultimately understand the binding interactions among bio-inorganic interfaces, such that a rational design of biomolecules can be realized for the synthesis of highly active, green, multifunctional nanomaterials.

Keywords

Biomimetic; Peptides; Nanoparticles; Sequence Effects; Binding Affinity

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