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题名: Fenton体系氧化吸附机理研究及在采油污水处理中的应用
作者: 高迎新
学位类别: 博士
答辩日期: 2003
授予单位: 中国科学院研究生院
授予地点: 北京
导师: 杨敏
关键词: Fenton试剂 ; Fenton's Reagent ; 类Fenton反应 ; Fenton-like's Reaction ; 采油污水 ; Produced Water ; 经基自由基 ; Hydroxyl Radicals ; 氧化 ; Oxidation ; 吸附 ; Absorption ; 水解 ; Hydrolysis
其他题名: Study on Oxidation and Absorption Aspects of Fenton's Process and Its Application to Produced Water Treatment
中文摘要:
      Fento可类Fenton体系在处理生物难降解有机污染物方面已成为得到广泛应用的高级氧化技术之一。本文从理论和应用两个方面对Fent。可类Fenton体系中过氧化氢的分解规律、铁的水解形态特征、自由基产生速度、ORP变化规律及Fenton体系在处理采油污水方面的应用进行了系统研究,并取得了如下研究成果。1)类Fenton反应中凡02的分解是假一级动力学反应,分解速率在pH2.8-3.0之间达到最大,分解速率常数与[H 202〕0/[Fe3+]0的摩尔比的指数成正比;该反应的活化能为4083J/mol;其H2O2分解速率及反应中亚铁离子浓度都明显地低于Fenton反应过程。2)在Fenion反应和类Fenton反应两种反应体系中,起始反应的轻基自由基生成速率高,并都随投加的HZoZ浓度和Fe2+/Fe3+浓度的增大而升高,但在同样条件下类Fenton反应自由基的生成速率要显著地低于Fenton反应。初始反应完成后Fenton体系中自由基的生成速率仍然高于类Fenton反应。3)在水解度B”相同时,Fenton反应中Fe(III)的水解速度明显快于类Fenton体系中Fe(III)和铁盐体系,Fe(III)水解速率随H202浓度增加而呈下降趋势。4)在没有有机物存在的Fenton体系中,oRP随HZOZ的加入而迅速升高,直至H2O2/Fe2+摩尔比达到0.72-0.76。在有机物存在的条件下,ORP值随着反应时间出现最大值,而Fe2+浓度出现最小值,ORP最大值与Fe2+最小值相对应,极值的出现与有机自由基的作用有关。5)实验室小试和现场中试结果均表明,采油污水经混凝-Fenton工艺处理后,出水有机物可以满足国家外排标准;处理过程中,石油烃类物质通过自由基反应形成了二酯类化合物,其含量随着氧化的进行而逐渐降低。
英文摘要:       The reaction of hydrogen peroxide with ferrous ions (known as Fenton's reaction) or ferric ions (known as Fenton-like reaction), as a technology of advanced oxidation process, is widely used for the removal of bio-refractory organic substrates from wastewater. In this paper, a study on H2O2 decomposition rates, Fe(III) hydrolyzing characteristics, formation rates of hydroxyl radicals in both Fenton's and Fenton-like's processes, was conducted systematically for the purpose of better understanding pollutant removal mechanisms of the Fenton's process. On the basis of the above studies, the Fenton's process was employed to treat produced water from oilfield. The following innovative results were obtained. The decomposition of H2O2 in a Fenton-like's process was found to obey the pseudo-first-order reaction. The rate constant of H2O2 decomposition was an index function of [H2O2]0/[Fe3+]0, and the optimum pH range for H2O2 decomposition was 2.8-3.0. The activation energy for H2O2 decomposition was 4083J/mol. Compared with the Fenton's process, both the rate constant of H2O2 decomposition and the residual Fe2+ were significantly low. Under similar conditions, the production rate of hydroxyl radicals in the Fenton's system was significantly higher than that in a Fenton-like's system, indicating that the Fenton's system is not equal to the Fenton-like's system following the end of the initial reaction. In both systems, however, the amount of hydroxyl radicals increased with the increase of H2O2 and Fe2+/ Fe3+ concentration. The hydrolysis rate of Fe(III) in the Fenton's system was markedly higher than that in the Fenton-like's system or ferric solution system at the same hydrolysity The hydrolysis of Fe(III) in the Fenton's system was retarded to some extent by the increase of H2O2 dose. In a Fenton's system without input of organics, the ORP values increased with the increase of H2O2 dose until the molar ratio of [H2O2]o/[Fe2+]0 arrived at 0.72-0.76. In the presence of organics, there appeared a maximum point of ORP corresponding with the minimum point of Fe2+ with the progress of reactions. ORP can be utilized as an important parameter for process control. 5) The lab and field tests demonstrated that the Fenton's process was effective for the removal of organics from produced water. GC-MS chromatographic analysis indicated that the formation of esters during Fenton's reaction was attributed to the oxidation of hydrocarbon by hydroxyl radical.
内容类型: 学位论文
URI标识: http://ir.rcees.ac.cn/handle/311016/34942
Appears in Collections:环境水质学国家重点实验室_学位论文

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Recommended Citation:
高迎新. Fenton体系氧化吸附机理研究及在采油污水处理中的应用[D]. 北京. 中国科学院研究生院. 2003.
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