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Photocatalytic synthesis of metallic nanoparticles and their applications

Simon, Zoe Carolyn (2024) Photocatalytic synthesis of metallic nanoparticles and their applications. Doctoral Dissertation, University of Pittsburgh. (Unpublished)

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Abstract

Photo-driven nanoparticle syntheses have remained relatively limited in scope compared to traditional synthetic methods, such as chemical reduction, thermal decomposition, laser-based syntheses, and nanolithography techniques. However, a photo-driven pathway offers numerous advantages, as light is highly tunable in its wavelength, intensity, timing, and duration of irradiation. The majority of light-driven syntheses which have been reported use either the localized surface plasmon resonance of existing or developing seed particles, or a photoexcited reagent which is depleted as the reaction proceeds, analogous to chemical reduction. Here, I introduce a photocatalytic reduction method for the synthesis of metallic nanoparticles, a novel synthetic technique which produces nanoparticles via a continuous nucleation pathway. In Chapter 2, I discuss this nucleation pathway and how light can be used to effectively “turn on” nanoparticle synthesis without impacting final nanoparticle morphology. Chapter 3 investigates the effects of reagent identity and the ratio of reagents on nanoparticle outcomes. Chapter 4 extends this photocatalytic reduction approach to the synthesis of bimetallic nanoparticles, and compares reaction outcomes to those of traditional chemical reduction based syntheses. In Chapter 5, the evolution of stoichiometry and chemical ordering in bimetallic nanoparticles synthesized via photocatalytic reduction is discussed, focusing on the gold/copper system. Finally, in Chapter 6 I apply this synthetic approach to the production of hydrogen through a photocatalytic water splitting reaction, and demonstrate the necessity of stable nanoparticles to catalyze the reaction. Taken together, this new approach to the synthesis of metallic nanoparticles via a photocatalytic reduction mechanism and the application of particles synthesized through this pathway offers insight into how light can be utilized as a reagent in nanochemistry, and lays the foundation for future studies to elucidate the underlying mechanism to further control nanoparticle outcomes.

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Details

Item Type: University of Pittsburgh ETD
Status: Unpublished
Creators/Authors:
CreatorsEmailPitt UsernameORCID
Simon, Zoe Carolynzcs12@pitt.eduzcs120000-0003-2302-1165
ETD Committee:
TitleMemberEmail AddressPitt UsernameORCID
Committee ChairMillstone, Jilljem210@pitt.edu
Committee MemberRosi, Nathanielnrosi@pitt.edu
Committee MemberMeyer, Taratara.meyer@pitt.edu
Committee MemberBernhard, Stefanbern@cmu.edu
Date: 10 January 2024
Date Type: Publication
Defense Date: 26 June 2023
Approval Date: 10 January 2024
Submission Date: 12 December 2023
Access Restriction: 2 year -- Restrict access to University of Pittsburgh for a period of 2 years.
Number of Pages: 217
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: photocatalytic reduction, nanoparticle synthesis, metal nanoparticles, hydrogen evolution
Date Deposited: 10 Jan 2024 14:21
Last Modified: 10 Jan 2024 14:21
URI: http://d-scholarship.pitt.edu/id/eprint/45661

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