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Cu Nitrides and Cu Phosphides for Hydrogen Evolution, Oxygen Evolution and Oxygen Reduction Reaction

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Cu Nitrides and Cu Phosphides for Hydrogen Evolution, Oxygen Evolution and Oxygen Reduction Reaction
Ma, Xiao
One way to alleviate some environmental issues related to the global use of fossil fuels is to develop efficient non-platinum group metal (non-PGM) electrocatalysts that can be used for electrochemical energy conversion reactions including hydrogen evolution reaction (HER), oxygen evolution reaction (OER), and oxygen reduction reaction (ORR). For their broader adoption, high activity and durability of the electrocatalysts is crucial. The incorporation of nitrogen and phosphorus could downshift the d-band center and alleviate the overly strong intermediates binding, thus promotes the ability to dissociate molecular oxygen and further proton-electron transfer of *O intermediates. It’s also beneficial for increasing the stability compared with Cu nanoparticles. In this dissertation, the synthesis of copper-based materials including Cu phosphides and Cu nitrides, and the study of their electrochemical properties and potential electrochemical applications were performed. In this dissertation, the following projects were completed: (1) Colloidal synthesis of Cu and Ag-Cu nanocrystals and their phosphidation products (Cu3P and Ag-Cu3P). (2) Direct synthesis of CuP2 and Cu3P with red phosphorus in solution-phase without annealing, trioctylphosphine oxide was found to help control the morphology and form CuP2 nanowires. (3) Using Cu nanocrystal as seeds for hot-injected during the synthesis of Cu3N synthesis, and lattice-strained Cu@Cu3N nanocrystals. (4) Exploration of Cu-based MOF materials, including mixed-metal Cu (II) BDC, Cu (II) BTC and their derivatives for hydrogen evolution reaction. These materials were structurally characterized using techniques such as Powder X-ray diffraction, electron microscopy, energy dispersive X-ray Spectroscopy and X-ray Photoelectron Spectroscopy. Their electrochemical performance and stability towards HER, OER and ORR were investigated with techniques including voltammetry (polarization curve, Tafel analysis, etc.) and electrochemical impedance spectroscopy (for charge transfer resistance). Rotating disk electrode set-up was used additionally for oxygen reduction reaction to investigate the intrinsic electrocatalytic performance from the mass transport. In summary, Cu-based materials have cost-effectiveness advantages in alkaline medium and their surface strain, composition and morphology are important to study for HER, OER and ORR. By incorporating N and P, the activity and stability can be improved and used as efficient non-Platinum based electrocatalyst.
Copper nitride
Copper phosphides
Energy conversion
Lachgar, Abdessadek (advisor)
Holzwarth, Natalie (committee member)
Ghadiri, Elham (committee member)
Ding, Wendu (committee member)
King, Bruce (committee member)
2024-02-13T09:36:06Z (accessioned)
2023 (issued)
Chemistry (discipline)
2029-01-01 (terms)
2029-01-01 (liftdate)
http://hdl.handle.net/10339/102908 (uri)
en (iso)
Wake Forest University

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