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Mechanism and Kinetics of the Catalytic Oxidation of Aqueous Ammonia to Molecular Nitrogen

机译:Mechanism and Kinetics of the Catalytic Oxidation of Aqueous Ammonia to Molecular Nitrogen

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摘要

Aqueous phase catalytic oxidation of ammonia has been studied over Ru/TiO{sub}2 catalyst in a batch reactor by changing the solution pH, concentration of catalyst in the solution, temperature, and reaction time. The oxidation reaction of ammonia over Ru/TiO{sub}2 catalyst has been found to take place exclusively for the aqueous NH{sub}3 with a preferred mode in strong alkaline pH region. An oxidation reaction pathway has been proposed as follows: Oxidation of ammonia is initiated by the reaction of aqueous ammonia with catalytically activated oxygen. After undergoing further successive oxidation reactions with activated oxygen, ammonia is finally oxidized to a molecule of nitrous acid. Nitrous acid dissociates into a nitrite ion and a proton. The solution pH is decreased with the protons from the dissociation of HNO{sub}2 so that the solution concentration of (NH{sub}4){sup}+ is increased. Molecular nitrogen as a final product is produced from the homogeneous aqueous phase reaction between nitrous ion and ammonium ion. Further reaction of nitrous ion with the activated oxygen leads to the formation of nitrate ion. The reaction pathway proposed has been validated with the changes of solution pH along with the ammonia conversions, and the formation of N{sub}2 from the solution containing (NO{sub}2){sup}- and (NH{sub}4){sup}+ ions in equimolar amounts of nitrogen has been confirmed in a separate experiment. The kinetics of aqueous ammonia oxidation reaction has been well represented as a first-order reaction with respect to the concentration of aqueous ammonia, and an apparent rate constant has been obtained as a function of catalyst concentration in solution, oxygen pressure, and reaction temperature.

著录项

  • 来源
    《Environmental Science & Technology: ES&T》 |2003年第24期|5745-5749|共5页
  • 作者

    DEUK KI LEE;

  • 作者单位
  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
  • 原文格式 PDF
  • 正文语种 英语
  • 中图分类 环境化学;
  • 关键词

  • 入库时间 2024-01-25 20:34:07
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