Publication Date

2017-04-17

Availability

Open access

Embargo Period

2017-04-17

Degree Type

Dissertation

Degree Name

Doctor of Philosophy (PHD)

Department

Chemistry (Arts and Sciences)

Date of Defense

2017-04-06

First Committee Member

Marc R. Knecht

Second Committee Member

James N. Wilson

Third Committee Member

Rajeev Prabhakar

Fourth Committee Member

Kevin M. Collins

Abstract

The rational design of nanomaterials has yielded new technologies that have revolutionized numerous diverse fields. The work detailed herein first describes the application of photocatalytic nanomaterials towards the environmental remediation of harmful toxins. Specifically, a low-temperature solution-phase synthetic route for size- controlled Cu2O octahedra particles was developed, and these materials were evaluated as catalysts for the photocatalytic degradation of aromatic organic compounds. Moreover, cubic Cu2O/Pd composite structures were fabricated and demonstrated to be effective photocatalysts for the generation of H2 and the reductive dehalogenation of polychlorinated biphenyls, well-known carcinogens present at many contaminated sites around the world. This photocatalytic approach to environmental remediation exemplifies the adaptation of light-driven technologies and sustainable practices to energy-intensive catalytic systems. In addition, this work also investigates the organic/inorganic interface of peptide-mediated Au nanoparticles as a means to identify rational design principles for materials binding peptide sequences for the advancement of stimuli-responsive bionanoassemblies. Factors inherent to peptide sequences that can promote strong materials-binding affinity and/or effective nanoparticle stabilization capability were identified in order to progress biomimetic technologies. These findings were elucidated using a combinational approach of peptide binding experiments to Au in partnership with molecular dynamics simulations. Overall, this work demonstrates the growing applications of nanomaterials in remediation technologies and aids in the understanding of the origins of peptide material affinity and nanoparticle stabilization.

Keywords

Cu2O; photodegradation; tandem catalysis; polychlorinated biphenyls; reductive dehalogenation; bionanocombinatorics; peptides; Au nanoparticles; binding affinity; binding thermodynamics

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