Graduation Term

Summer 2026

Degree Name

Master of Science (MS)

Department

Department of Chemistry

Committee Chair

Jun-Hyun Kim

Committee Member

Christopher Hamaker

Committee Member

Christopher Mulligan

Abstract

The development of efficient and sustainable catalytic systems is a major focus in modern chemistry, particularly as industries seek greener and more energy-efficient chemical processes. Nanoparticle (NP)-based colloidal catalysts have emerged as powerful materials for catalytic applications due to their large surface areas, tunable structural changes, and easy recyclability. Among various metallic elements, palladium nanoparticles (PdNPs) have gained particular attention due to their outstanding catalytic versatility and ability to facilitate important reactions used in organic synthesis, pharmaceutical production, and materials chemistry. However, colloidal PdNPs possess high surface energy and are thermodynamically unstable, which can lead to aggregation and loss of catalytic performance. To maintain catalytic efficiency, appropriate support materials are required to effectively stabilize the NPs while preserving accessibility to active catalytic sites. Carbon-based supports have been extensively studied due to their exceptional combination of structural, chemical, and electronic properties. These materials provide a stable support platform for dispersing metallic NPs while maintaining accessibility of active sites for catalytic reactions. Among carbon-based supports, carbon black (CB) has been widely utilized materials in both industrial and academic catalytic systems typically produced through the incomplete combustion or thermal decomposition of hydrocarbon feedstocks. The defect-rich surface and intrinsic electrical conductivity of CB facilitate strong interactions with metallic NPs and enhance electron transfer processes between the catalyst and reactants during chemical reactions. These features make CB an effective support material for PdNPs in reactions such as hydrogenation and Pd-catalyzed cross-coupling. We prepared surfactant-free and physically incorporated PdNPs within CB-based materials in situ via a deposition–precipitation (D–P) method, a widely used approach for immobilizing metal NPs onto solid supports. In this method, metal precursor species are deposited from solution and subsequently precipitated directly onto the surface of the support material, allowing ionic species to nucleate and grow to form NPs at the interface of the support. As a result, the NPs become strongly anchored to the CB surface, promoting strong metal–support interactions that enhance catalyst stability during catalytic reactions. These catalysts were evaluated as quasi-homogeneous systems in carbon–carbon bond forming reactions using alcohol-rich solvents under ambient aerobic conditions. The D-P method using Pd ions in the presence of the carbon-based materials in situ provided an effective strategy for preparing highly dispersed and stable metal PdNPs as catalysts since it does not require additional stabilizing agents or surfactants. This process allows the NPs to retain clean, bare surfaces that remain fully accessible to catalytic sites. The absence of stabilizers also minimizes the possibility of surface blockage that could otherwise reduce the number of active catalytic sites supported on carbon-based materials. The resulting composite particles were then employed as quasi-heterogeneous catalysts in C-C forming reactions. Furthermore, optimum reaction conditions were established by screening various bases, temperatures, and recyclability using these composite particles. By investigating carbon-based catalytic substrates capable of stabilizing PdNPs for other C-C bond-forming reactions such as Ullmann, Suzuki, Sonogashira, and hydrogenation transformations, this study aims to elucidate how support structure and surface chemistry influence catalytic activity and stability.

Access Type

Thesis-Open Access

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Available for download on Saturday, October 12, 2030

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