Effect of nitrogen doping on the electronic and catalytic properties of carbon nanotube electrode materials



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This dissertation discusses the influence of nitrogen doping (N-doping) on the electronic and catalytic properties of carbon nanotubes (CNTs). These properties have been studied using a variety of techniques, in order to both qualitatively and quantitatively analyze the relationship between the nitrogen concentration and observed properties. Chapter 1 provides a general overview of CNTs and N-doping and details some of the previous research from our group. Chapter 2 discusses the assembly and characterization of free-standing electrode mats, which are used in order to understand the intrinsic physicochemical properties of the material without relying on the secondary influence of another conductive support. Raman microscopy, X-Ray photoelectron spectroscopy, scanning and scanning-tunneling electron microscopy, as well as electrochemical methods were all used to demonstrate the viability of the mat electrodes for further experiments. Chapter 3 addresses the examination of a range of nitrogen concentrations in order to better understand the effects of nitrogen concentration on the electrochemical and electrical properties such as the differential capacitance, density of states at the Fermi level (D(E[subscript F])), bulk conductivity and work function. These properties were studied using a variety of techniques, including UV-photoelectron spectroscopy, electrochemical impedance spectroscopy and conductive four point probe. Chapter 4 investigates the inherent catalysis of the nitrogen doped CNTs (N-CNTs) with respect to O2 reduction, and a complex mechanism is proposed. Electrochemical methods such as cyclic and linear sweep voltammetries as well as thermo-gravimetric analysis and gasometric analysis were all employed to determine heterogeneous decomposition rates as well as to detect intermediates of the O₂ reduction reaction. Chapter 5 discusses the electrocatalytic degradation of free cyanide (CN⁻) at the N-CNT mat electrodes. These results both provide further support for the mechanism discussed in Chapter 4, and present the opportunity for a potential application of N-CNTs for environmental purposes. Specifically, spectroscopic and electrochemical methods, in conjunction with theoretical models show both that the presence of CN⁻ does not inhibit O2 reduction, and that it can be effectively converted to cyanate (OCN⁻) at the N-CNT electrodes. Future work involving the assembly and characterization of transparent N-CNT films is discussed in Chapter 6.