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Effects of dissolved oxygen and iron aging on the reduction of trichloronitromethane, trichloracetonitrile, and trichloropropanone

机译:溶解氧和铁的老化对三氯硝基甲烷,三氯乙腈和三氯丙烷的还原的影响

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Iron metal (Fe(0)) is a potent reductant capable of reducing a wide variety of halogenated organic compounds including disinfection byproducts (DBPs). These reduction reactions may play a role in DBP fate in iron water mains and potentially could be exploited to remove DBPs from drinking water or wastewater in a packed-bed configuration. Oxidants (i.e., dissolved oxygen (DO) and chlorine) present in the water, however, may decrease the DBP degradation rate by competing for reactive sites and rapidly aging or corroding the iron surface. Thus, batch experiments were performed to investigate the effect of DO on the degradation rates of selected DBPs by Fe(0). Experiments were performed under anaerobic conditions, in initially oxygen saturated buffer without DO control, and under controlled DO (approximately 4.0 or 8.0 mg l~(-1)) conditions. The effect of short-term (25-105 min) iron aging in DO-containing buffer on DBP degradation rate also was investigated in separate experiments. For fresh Fe(0), the degradation rates of trichloronitromethane (TCNM) and trichloroacetonitrile (TCAN) in initially oxygen saturated buffer were similar to their respective rates under anaerobic conditions. The degradation rate of 1,1,1-trichloropropanone (1,1,1-TCP), however, decreased significantly in the presence of DO and the effect was proportional to DO concentration in the controlled DO experiments. For a DO concentration of 4 mg l~(-1), the degradation rate of the three DBPs was greater for longer aging times as compared to their respective rates after 25 min, suggesting the formation of a mineral phase that increased reactivity. For a DO concentration of 8 mg l~(-1), the effects of increasing aging time were mixed. TCNM degradation rates were stable for all aging times and comparable to that under anaerobic conditions. The TCAN and 1,1,1-TCP degradation rates, however, tended to decrease with increasing aging time. These results suggest that the reduction of highly reactive DBFs by Fe(0) will not be affected by the presence of DO but that the reaction rates will be slowed by DO for DBFs with slower degradation kinetics.
机译:铁金属(Fe(0))是一种有效的还原剂,能够还原多种卤化有机化合物,包括消毒副产物(DBP)。这些还原反应可能会在铁水总管中的DBP命运中发挥作用,并且有可能被利用来从填充床配置中从饮用水或废水中去除DBP。然而,水中存在的氧化剂(即溶解氧(DO)和氯)可能会竞争反应性位点并迅速老化或腐蚀铁表面,从而降低DBP降解速率。因此,进行了批处理实验以研究DO对Fe(0)对所选DBP降解速率的影响。实验是在厌氧条件下,在最初没有DO控制的氧饱和缓冲液中,以及在受控的DO(约4.0或8.0 mg l〜(-1))条件下进行的。还在单独的实验中研究了含DO的缓冲液中短期(25-105分钟)铁老化对DBP降解速率的影响。对于新鲜的Fe(0),三氯硝基甲烷(TCNM)和三氯乙腈(TCAN)在最初的氧饱和缓冲液中的降解速率与它们在厌氧条件下的降解速率相似。但是,在有DO的情况下,1,1,1-三氯丙烷(1,1,1-TCP)的降解速率显着降低,并且在受控的DO实验中,其效果与DO浓度成正比。对于溶解度为4 mg l〜(-1)的溶解氧,三个DBP在更长的老化时间下的降解速率与其在25分钟后的降解速率相比更大,表明形成了增加反应性的矿物相。当溶解氧浓度为8 mg l〜(-1)时,混合了增加老化时间的效果。 TCNM的降解速率在所有老化时间内均保持稳定,并且与厌氧条件下的降解速率相当。然而,随着老化时间的增加,TCAN和1,1,1-TCP降解率趋于降低。这些结果表明,Fe(0)对高反应性DBF的还原不会受到DO的存在的影响,但是对于降解动力学较慢的DBF,DO会降低反应速率。

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