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环境科学  2010 

Degradation Mechanism of Phenol with Electrogenerated Hydrogen Peroxide on a Pd/C Gas-diffusion Electrode
Pd/C气体扩散电极用于电生成H2O2降解苯酚的研究

Keywords: electrochemical oxidation,gas-diffusion cathode,Pd/C catalyst,hydrogen peroxide,phenol
电化学氧化
,气体扩散电极,Pd/C催化剂,过氧化氢,苯酚

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Abstract:

Using a self-made Pd/C gas-diffusion electrode as the cathode and Ti/IrO2/RuO2 as the anode, the degradation of phenol was investigated in an undivided electrolysis device by the electrochemical oxidation process. Hydroxyl radical (·OH) was determined in the reaction mixture by the electron spin resonance spectrum (ESR). The result indicated that the Pd/C catalyst in Pd/C gas-diffusion electrode system accelerated the two-electron reduction of O2 to H2O2 when feeding air, which is in favor of producing ·OH. After 120 min electrolysis in Pd/C gas-diffusion electrode system, the steady concentration of H2O2 was 7.5 mg/L. The removal efficiency of phenol and COD reached about 97.2% and 50% after 120 min electrolysis, respectively, which suggested that most of phenol were oxidized to intermediates using the Pd/C gas-diffusion electrode. Furthermore, the ratio of BOD5/COD of the solutions was 9.1 times larger than the initial ones. Hence the electrochemical oxidation can enhance the biodegradation character of the phenol solution. The degradation of phenol was supposed to be cooperative oxidation by direct and/or indirect electrochemical oxidation at the anode and H2O2, ·OH produced by oxygen reduction at the cathode. UV-Vis and GC-MS identified catechol, hydroquinone, and benzoquinone as the main aromatic intermediates, and adipic, maleic, fumaric, succinic, malonic, and oxalic acids as the main aliphatic carboxylic intermediates. A reaction scheme involving all these intermediates was proposed.

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