Teel A L, Warberg C R, Atkinson D A, Watts R J
Department of Civil & Environmental Engineering, Washington State University, Pullman 99164-2910, USA.
Water Res. 2001 Mar;35(4):977-84. doi: 10.1016/s0043-1354(00)00332-8.
Contaminant degradation, stoichiometry, and role of hydroxyl radicals (OH*) in four Fenton's systems were investigated using trichloroethylene (TCE) as a model contaminant. A standard Fenton's system, a modified soluble iron system with a pulse input of hydrogen peroxide, and two modified mineral-catalyzed systems (pH 3 and 7) were studied. In the standard Fenton's system, which had the most efficient reaction stoichiometry, 78% of the TCE was degraded; however, chloride analysis indicated that no more than two of the three chlorines were displaced per TCE molecule degraded. Although the modified soluble iron system was characterized by 91% TCE degradation, chloride analysis also indicated that no more than two of the chlorines were lost from the TCE. In the goethite system of pH 3, > 99% of the TCE was degraded. Near-complete release of chloride suggested that the TCE may have been mineralized. Only 22% degradation of TCE was achieved in the pH 7 goethite system. and there was minimal release of chloride. The mineral-catalyzed reactions exhibited the least efficient reaction stoichiometry of the four systems. Experiments using hydroxyl radical scavengers showed that the standard Fenton's system degraded TCE entirely by hydroxyl radical mechanisms, while approximately 10-15% of the degradation achieved in the modified soluble iron and goethite-catalyzed systems at pH 3 was mediated by non-hydroxyl radical mechanisms. In the goethite system at pH 7, only non-hydroxyl radical mechanisms were found. The goethite-catalyzed system at pH 3 effectively degraded the parent compound and may have the potential to mineralize contaminants when used for in situ soil and groundwater remediation and ex situ waste stream treatment in packed-bed reactors.
以三氯乙烯(TCE)作为模型污染物,研究了四种芬顿体系中污染物的降解、化学计量关系以及羟基自由基(OH*)的作用。研究了标准芬顿体系、过氧化氢脉冲输入的改良可溶性铁体系以及两种改良的矿物催化体系(pH值分别为3和7)。在具有最有效反应化学计量关系的标准芬顿体系中,78%的TCE被降解;然而,氯分析表明,每降解一个TCE分子,三个氯原子中最多只有两个被取代。尽管改良可溶性铁体系的TCE降解率为91%,但氯分析也表明,TCE中最多只有两个氯原子损失。在pH值为3的针铁矿体系中,>99%的TCE被降解。氯的近乎完全释放表明TCE可能已被矿化。在pH值为7的针铁矿体系中,TCE的降解率仅为22%,且氯的释放量极少。矿物催化反应在四个体系中表现出最低效的反应化学计量关系。使用羟基自由基清除剂的实验表明,标准芬顿体系完全通过羟基自由基机制降解TCE,而在改良可溶性铁体系和pH值为3的针铁矿催化体系中,约10-15%的降解是由非羟基自由基机制介导的。在pH值为7的针铁矿体系中,仅发现非羟基自由基机制。pH值为3的针铁矿催化体系能有效降解母体化合物,在用于原位土壤和地下水修复以及填充床反应器中的异位废水处理时,可能具有矿化污染物的潜力。