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Characteristics of Poly-aminoanthraquinone Modified Electrode as Oxygen Reduction Cathode and Its Application in Electro-Fenton

Author: GaoMingMing
Tutor: YangFengLin
School: Dalian University of Technology
Course: Water Science and Technology
Keywords: Poly 1,5 - diamino anthraquinone Stability Electrochemical behavior Oxygen reduction Electro-Fenton
CLC: O631.3
Type: PhD thesis
Year: 2009
Downloads: 371
Quote: 1
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Abstract


Polyethylene 1,5 - diamino-anthraquinone the (P1 ,5-DAAQ) is a new kind of conductive polymer materials, the course of the electrochemical reaction corresponding to the like polyaniline conductive skeleton doping / de-doping process and anthraquinone group of the pros and cons of the electronic process. These two processes in the same molecular unit in the conjugated system, and not only makes the the aminoanthraquinone polymer structure has been optimized, further it has high electrical activity, and to exhibit in the energy storage and electrocatalytic excellent performance. Electrocatalytic oxygen reduction technology is a chemically modified electrode electrocatalytic research in the field of hot issues. The quinone compounds modified electrode has obvious electrocatalytic activity for oxygen reduction, caused extensive study of the electrochemical workers. This thesis study aminoanthraquinone polymer modified electrode, and other methods (such as adsorption, doping, etc.) to obtain a quinone modified electrode having a stable, simple preparation process, the advantages of higher concentrations of the active point, and also has long chain structure and characteristics of the functional groups of the anthraquinone like polyaniline is prepared with high oxygen reduction catalytic activity of anthraquinone modified electrode provides a new way of thinking. In this thesis, the electrochemical anodization prepared poly 1,5 - diamino anthraquinone the (P1 ,5-DAAQ) modified Pt electrode. And electrochemical detection techniques using cyclic voltammetry, chronoamperometry, electrochemical impedance spectroscopy, and scanning electron microscopy, Fourier transform infrared spectroscopy and other characterization methods to study the electrochemical properties of Pt P1 ,5-DAAQ modified, stable , of oxygen 2 electronic revert to the electrocatalytic activity of hydrogen peroxide, to explore the feasibility of its application in the electro-Fenton technology. By cyclic voltammetry allows the 1,5-DAAQ monomer polymerization to form a thin layer of black polymer film in the surface of the Pt electrode electrochemical oxidation occurs. The polymerization process is significantly affected by the temperature, the optimal polymerization results can be obtained when the control of the polymerization reaction is carried out at 10 ℃. Using scanning electron microscopy, Fourier transform infrared spectroscopy and electrochemical analysis method to study a the P1 ,5-DAAQ polymerization process. Found the P1 ,5-DAAQ polymerization process nucleation stage is divided into two phases: the polymer forming the core of the aggregation point bit, i.e. in the initial polymerization, the monomer oxidation; including a two-dimensional growth phase and three-dimensional growth phase polymerization was the growth stage. Electrochemical detection method and Fourier transform infrared spectroscopy study the Pt/P1 ,5-DAAQ electrode in acidic solution redox behavior and stability. The study found that the oxidation process and the reduction process, the the ,5-DAAQ film P1 of the ion transport process is different, and is close to the ionic radius. H transmission non-diffusion-controlled process; the anion entering and exclude polymer film process controlled by diffusion. And the establishment of a model used to describe this process. P1 ,5-DAAQ membrane hydrated anion diffusion coefficient in line Cl - gt; the SO 4 2 - gt; NO 3 < / sub> - gt; the PO 4 3 - relationship. Investigated not only in the study of the process of degradation of the polymer P1 ,5-DAAQ reversible potential range of degradation, but also studied a P1 ,5-DAAQ anode peroxidation. The study found that the reversible potential region, P1 ,5-DAAQ 0.5 mol / LHCl H 2 SO 4 the HNO 3 H < sub> 3 PO degradation rate constant were 2.46,4.93,2.46 and 2.85 × 10 -4 s -1 . In the potential range than the reversible potential corrections, P1 ,5-DAAQ occurred phenomenon of anode peroxide. Peroxidation process P1 ,5-DAAQ occurs is not completely degraded, class quinone structure is destroyed, π-bond conjugated length is reduced, the long-chain structure of the polymer is destroyed, while the anion binding to the polymer which. Pt/P1 ,5-DAAQ electrodes in 0.1 mol / LH 2 SO 4 obvious electrocatalytic activity for oxygen reduction reaction in 0.1 mol / LH 2 SO 4 in the oxygen reduction peak potential of 0.39 V, the oxygen reduction reaction to the two-electron reduction. Cyclic voltammetry, chronoamperometry and electrochemical impedance spectroscopy study found that the electrode Pt/P1 ,5-DAAQ electrocatalytic activity for oxygen reduction by the thickness of the film, the influence of the pH of the solution is obvious. Different thickness the P1 ,5-DAAQ membrane surface exists different oxygen transmission process. According to the comparison of the data of the oxygen diffusion coefficient the different thickness the P1 ,5-DAAQ of Modified Pt electrode surface, an electron transport resistance, an oxygen-reduction reaction rate constants, etc., to prove Although a thicker provide P1 ,5-DAAQ, the true electrode area and a higher concentration of active point, a short time is more conducive to the electro-catalytic oxygen reduction reaction, but the thinner the P1 ,5-DAAQ, modified Pt electrode formed surface morphology is more conducive to the oxygen mass transfer it showed better electrocatalytic oxygen reduction performance. Activity of the electrocatalytic activity Pt/P1 ,5-DAAQ oxygen reduction decreases with increasing pH value. In addition, Degradation as P1 ,5-DAAQ the, the oxygen reducing catalytic activity is gradually reduced. Of Pt/P1 ,5-DAAQ electrode as oxygen reduction cathode electro-Fenton system. Its used for the electrocatalytic O 2 H 2 O 2 rate and current efficiency is generated and its influencing factors. Moreover, this electrode Fe 3 restore also showed significant electrocatalytic activity. And electrochemical impedance spectroscopy to study the competition between this electrode surface reduction reaction. When this electrode as an oxygen reduction cathode for electrically Fenton reaction, it is possible within a potential range of -0.2 to 0.1 V, pH value of the acidic solution of 2-3, decolorizing bromamine. And through degradation kinetics analysis bromamine, to examine the impact of this electric Fenton oxidation ability of different reaction conditions.

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CLC: > Mathematical sciences and chemical > Chemistry > Polymer chemistry ( polymer ) > Polymer physics and physical chemistry of polymers > The chemical nature of polymers
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