Development of Novel Electrode Materials for the Electrocatalysis of Oxygen-Transfer and Hydrogen-Transfer Reactions

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Throughout this thesis, the fundamental aspects involved in the electrocatalysis of anodic O-transfer reactions and cathodic H-transfer reactions have been studied. The investigation into anodic O-transfer reactions at undoped and Fe(III)[doped MnO{sub 2} films] revealed that MnO{sub 2} film electrodes prepared by a cycling voltammetry deposition show improved response for DMSO oxidation at the film electrodes vs. the Au substrate. Doping of the MnO{sub 2} films with Fe(III) further enhanced electrode activity. Reasons for this increase are believed to involve the adsorption of DMSO by the Fe(III) sites. The investigation into anodic O-transfer reactions at undoped and Fe(III)-doped RuO{sub 2} ... continued below

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2779 Kilobytes pages

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Simpson, Brett Kimball August 27, 2002.

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  • Ames Laboratory
    Publisher Info: Ames Lab., IA (United States)
    Place of Publication: Iowa

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Throughout this thesis, the fundamental aspects involved in the electrocatalysis of anodic O-transfer reactions and cathodic H-transfer reactions have been studied. The investigation into anodic O-transfer reactions at undoped and Fe(III)[doped MnO{sub 2} films] revealed that MnO{sub 2} film electrodes prepared by a cycling voltammetry deposition show improved response for DMSO oxidation at the film electrodes vs. the Au substrate. Doping of the MnO{sub 2} films with Fe(III) further enhanced electrode activity. Reasons for this increase are believed to involve the adsorption of DMSO by the Fe(III) sites. The investigation into anodic O-transfer reactions at undoped and Fe(III)-doped RuO{sub 2} films showed that the Fe(III)-doped RuO{sub 2}-film electrodes are applicable for anodic detection of sulfur compounds. The Fe(III) sites in the Fe-RuO{sub 2} films are speculated to act as adsorption sites for the sulfur species while the Ru(IV) sites function for anodic discharge of H{sub 2}O to generate the adsorbed OH species. The investigation into cathodic H-transfer reactions, specifically nitrate reduction, at various pure metals and their alloys demonstrated that the incorporation of metals into alloy materials can create a material that exhibits bifunctional properties for the various steps involved in the overall nitrate reduction reaction. The Sb{sub 10}Sn{sub 20}Ti{sub 70}, Cu{sub 63}Ni{sub 37} and Cu{sub 25}Ni{sub 75} alloy electrodes exhibited improved activity for nitrate reduction as compared to their pure component metals. The Cu{sub 63}Ni{sub 37} alloy displayed the highest activity for nitrate reduction. The final investigation was a detailed study of the electrocatalytic activity of cathodic H-transfer reactions (nitrate reduction) at various compositions of Cu-Ni alloy electrodes. Voltammetric response for NO{sub 3}{sup -} at the Cu-Ni alloy electrode is superior to the response at the pure Cu and Ni electrodes. This is explained on the basis of the synergism of the two different metal sites at these binary alloy electrodes acting within the proposed response mechanism. Accordingly, adsorbed H-atoms are generated by cathodic discharge of H{sup +} at the Ni-sites whereas adsorption of NO{sub 3}{sup -} occurs at the Cu-sites.

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2779 Kilobytes pages

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OSTI as DE00804542

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  • Other Information: TH: Thesis (Ph.D.); Submitted to Iowa State Univ., Ames, IA (US)

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  • Report No.: IS-T 1970
  • Grant Number: W-7405-Eng-82
  • Office of Scientific & Technical Information Report Number: 804542
  • Archival Resource Key: ark:/67531/metadc734056

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  • August 27, 2002

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  • Oct. 19, 2015, 7:39 p.m.

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  • Nov. 11, 2015, 6:06 p.m.

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Simpson, Brett Kimball. Development of Novel Electrode Materials for the Electrocatalysis of Oxygen-Transfer and Hydrogen-Transfer Reactions, thesis or dissertation, August 27, 2002; Iowa. (digital.library.unt.edu/ark:/67531/metadc734056/: accessed December 19, 2018), University of North Texas Libraries, Digital Library, digital.library.unt.edu; crediting UNT Libraries Government Documents Department.