relation: http://d-scholarship-dev.library.pitt.edu/19565/ title: CARBON NANOMATERIALS AND THEIR ELECTROCHEMICAL APPLICATIONS creator: Tang, Yifan description: Recent years have witnessed the continuously growing interest in the area of nanotechnology. Among the innumerable novel compounds and materials, carbon nanomaterials, especially carbon nanotubes (CNTs) and graphene, are undeniably two of the most glorious shining stars due to their unique structures and promising physical, chemical, and electrical properties. Numerous research projects have been focused on the synthesis, characterization, and functionalization of carbon nanomaterials, as well as their enormous possible applications in energy generation/storage, sensors, electronics, reinforcement of composite materials, and drug delivery. Of particular interest in this dissertation are the functionalization of carbon nanomaterials − either by decorating with Pt nanoparticles (NPs) or by doping with nitrogen atoms − and their electrochemical applications for both fuel cell catalysts (and supports) and electrochemical sensors/biosensors. I have successfully synthesized and characterized hybrid structures of Pt NP-CNTs or Pt NP-graphene, and also a novel carbon nanomaterial − nitrogen doped carbon nanotube cups (NCNCs). The electrochemical properties and applications of these nanomaterials were also investigated. Pt NP decorated CNTs or graphene were studied and compared for their electrochemical sensor performance in order to obtain further understanding on the structure-property relationship between 1-dimensional and 2-dimensional nanomaterials as the sensing platform. Both Pt-CNTs and NCNCs were investigated as fuel cell catalysts with the aim of improving the performance and stability, decreasing the amount of expensive Pt, and most importantly, understanding and optimizing NCNCs as non-precious-metal catalysts to ultimately replace expensive Pt-based catalysts. Pt-CNTs demonstrated extraordinary stability with less material used compared to commercial Pt/C catalysts in long term stability testing. NCNCs also exhibited good catalytic activity towards oxygen reduction reaction (ORR) which makes them promising alternatives to Pt-based catalysts. Further look into the ORR mechanism suggested that the presence of both nitrogen and iron from catalyst of NCNCs synthesis process is crucial for the improved ORR catalytic activity. From the materials point of view, a novel simple sonication method was studied to separate stacked NCNCs into individual nanocups structures, with the long-term objective of drug delivery or nano-reactor applications. Both the separation mechanism and the structure-property relationship of the stacked and separated NCNCs were investigated. date: 2013-10-17 type: University of Pittsburgh ETD type: PeerReviewed format: application/pdf language: en identifier: http://d-scholarship-dev.library.pitt.edu/19565/1/Yifan_Dissertation_-_D-scholar_revision.pdf identifier: Tang, Yifan (2013) CARBON NANOMATERIALS AND THEIR ELECTROCHEMICAL APPLICATIONS. Doctoral Dissertation, University of Pittsburgh. (Unpublished)