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Year:: 2015
Contributor:: Zhu, Huiyuan (creator); Sun, Shouheng (Director); Kim, Eunsuk (Reader); Wang, Lai-Sheng (Reader); Brown University. Chemistry (sponsor)
Genre:: theses
Subject:: Nanoparticles; Catalysts; Fuel cells; Nanowires
Extent:: xxxiii, 187 p.

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Abstract:: Controlled synthesis of nanoparticles (NPs) is the key to developing highly efficient and stable catalysts for various reactions, including those involved in energy conversion systems, such as the proton exchange membrane fuel cell, and those used for catalytic bio-detections. The organic-solution based chemical synthesis provides a robust approach to obtaining well-defined NPs with monodisperse morphologies and assuring precise control over NP physicochemical parameters (size, shape, composition and crystal structure). It thus allows for a better understanding of the parameter-property correlation and the optimization rules of advanced NP catalysts. This dissertation covers the synthesis of 1-dimensional (1-D) binary FePt, CoPt and ternary FePtCu, FePtNi nanowires (NWs), face centered tetragonal (fct) FePt nanoparticles (NPs), Au-MnO nanocomposites and etc., as well as their applications in energy conversion and bio-detection systems. One-dimensional FePt, CoPt and FePtM (M = Cu, Ni) nanowires (NWs) are synthesized and converted to FePtM/Pt core/shell structure. These FePtM/Pt NWs show superior performance in catalyzing oxygen reduction reaction (ORR) in acidic solution. Furthermore, seed-mediated approach is applied to produce FeNiPt/Pt core/shell NWs. Tailoring the NW thickness and the surface structure (Pt-skeleton and Pt-skin) leads to an optimized catalytic performance towards ORR. Monodisperse FePt NPs are synthetically controlled from chemically disordered face centered cubic (fcc) structure to ordered face centered tetragonal (fct) structure. The NP’s electrocatalytic efficiency in oxygen reduction reaction (ORR) can be drastically increased by the fcc-fct structural transition. The relevant theoretical calculations of the structure-induced catalytic enhancement will also be discussed to provide a predictable model for future design and optimization of ORR nanocatalysts. My thesis also includes some other NPs, such as Au-MnO nanocomposites used for the electrochemical detection of H2O2, sub-10 nm M (II)-substituted magnetite MxFe3-xO4 (M=Fe, Cu, Co, Mn) NPs as the alternatives for Pt to catalyze ORR in alkaline solution and structure-controlled NPs FePtAu as electrocatalysts for formic acid oxidation reaction (FAOR).
Notes:: Thesis (Ph.D. -- Brown University (2015)

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Zhu, Huiyuan, "Rational Synthesis of Monodisperse Nanoparticles for Catalytic Applications" (2015). Chemistry Theses and Dissertations. Brown Digital Repository. Brown University Library. https://repository.library.brown.edu/studio/item/bdr:svr5zuvg/

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Chemistry Theses and Dissertations

Theses and Dissertations for the Chemistry department.
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Rational Synthesis of Monodisperse Nanoparticles for Catalytic Applications