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Electrocatalytic Oxidation of Some Alcohols on the Platinum Electrode Modified with Ordered Cyanide-Bridged Mixed Complexes

Author: LiuZuo
Tutor: MaYongJun
School: Northwest Normal University
Course: Analytical Chemistry
Keywords: nanomaterials soft template chemically modified electrode electrocatalytic oxidation methanol ethylene glycol glycerol
CLC: O643.32
Type: Master's thesis
Year: 2012
Downloads: 25
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Abstract


In this thesis, an ordered cyanide-bridged mixed complexes (Nd-Fe-MoO42-)modified platinum electrode is prepared by electrodeposition methods which rely onassistance of the lyotropic liquid crystal soft template. The soft template is constructedthrough component ratio of lecithin, AOT, Triton X-100and other compounds.Furthermore, the electrocatalytic oxidation process of three kinds of alcohols on thismodified electrode has been studied, it infers that the novel ordered cyanide-bridgedmixed complexes material possesses effectively cooperative catalytic action onplatinum substrate.There were four chapters in this paper:Chapter one: The characteristics and the preparation of nanomaterial aresummarized, with emphasis on the synthesis method of the lyotropic liquid crystalsoft template and the related nanomaterials in the field of electroanalysis. In addition,the developments and the problems of fuel cell anode materials using three kinds ofsmall organic molecules（methanol, ethylene glycol, glycerol）as fuels are reviewed.Chapter two: An ordered Nd-Fe-MoO42-cyanide-bridged mixed complexesmodified platinum electrode is prepared by the lyotropic liquid crystal soft templatemethods in which lecithin-AOT-Triton X-100system is accepted for the first time.Scanning electron microscopy （SEM） is employed to characterize morphology of themodified film. The electrocatalytic oxidation behavior of methanol on this modifiedelectrode is studied by means of cyclic voltammetry and chronoamperometry. Theordered cyanide-bridged mixed complexes film can be obtained by firstelectrodeposition on pre-coated soft template platinum substrate, and then removal ofsoft template with hydrogen bubble method. On the highly ordered cyanide-bridgedmixed complexes modified platinum electrode (Nd-Fe-MoO42-/Pt), the electrocatalyticoxidation peak current density of methanol has increased about50percent more thanthat on the disordered similar materials modified platinum electrode. In addition, theapparent activation energy of methanol on the ordered modified electrode is obviouslydecreased. Meanwhile, the electrocatalytic stability experiments and chronoampero-metry also demonstrate that the novel ordered Nd-Fe-MoO42-cyanide-bridged mixed complexes possesses much better and steady cooperative catalytic action toelectro-oxidation process of methanol on metal platinum.Chapter three: The electrocatalytic oxidation behavior of ethylene glycol on theordered cyanide-bridged mixed complexes modified platinum electrode(Nd-Fe-MoO42-/Pt) is studied by means of cyclic voltammetry and chronoampero-metry. The results indicate that the electrocatalytic oxidation current density ofethylene glycol on modified electrode is about10times more than that on bareplatinum electrode. Moreover, the influence of H+and SO42-concentration inelectrolyte solution on the voltammetric characteristics of ethylene glycolelectrocatalytic oxidation is also studied. It shows that the peak potential shiftsnegatively with increasing SO42-/HSO4-concentration. The effect of H+plays adominant role when H+and SO42-coexist in the system. Meanwhile, the relationshipbetween the oxidation peak current density of ethylene glycol and the temperaturedemonstrates that the apparent activation energy of ethylene glycol on the orderedmodified electrode is obviously decreased. Furthermore, the electrocatalytic stabilityexperiments and chronoamperometry also demonstrate that the newly developedmodified electrode possesses much better electrocatalytic activity and tolerance totoxic intermediate contamination.Chapter four: The electrocatalytic oxidation behavior of glycerol on the orderedmodified platinum electrode is studied, and the influence of supporting electrolyte,concentration of glycerol, scan rate and other factor are discussed. It shows that thesefactors have significant effect on electrocatalytic oxidation of glycerol. The resultsdemonstrate that the electrocatalytic oxidation current density of glycerol on themodified electrode is about4times more than that on the bare platinum electrode, andthe apparent activation energy of glycerol is significantly decreased. The good linearrelationship between the oxidation peak current of glycerol and the square root of thescan rate indicates that the electrode reaction of glycerol is controlled by diffusionprocess. Meanwhile, the electrocatalytic stability experiments and Chronoampero-metry for electrooxidation reaction of glycerol on metal platinum demonstrate that thenovel ordered cyanide-bridged mixed complexes material possesses much better andsteady cooperative catalytic action.

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CLC: > Mathematical sciences and chemical > Chemistry > Physical Chemistry ( theoretical chemistry ),chemical physics > Chemical kinetics,catalysis > Catalytic > Catalytic reaction
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