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铁和硫矿物组分对模拟厌氧土壤和沉积物中四氯化碳转化的影响。

The influence of iron and sulfur mineral fractions on carbon tetrachloride transformation in model anaerobic soils and sediments.

作者信息

Shao Hongbo, Butler Elizabeth C

机构信息

School of Civil Engineering and Environmental Science, University of Oklahoma, Norman, OK 73019, USA.

出版信息

Chemosphere. 2007 Aug;68(10):1807-13. doi: 10.1016/j.chemosphere.2007.04.048. Epub 2007 May 29.

Abstract

The objective of this research was to identify the dissolved species or solid phase mineral fraction(s) best correlated with rates of carbon tetrachloride (CT) reductive transformation in systems modeling sulfate-reducing and iron oxide-rich soils and sediments. We used sulfide (S(-II))-treated goethite as our model system, but also studied Fe(II) and S(-II)-treated goethite, Fe(II)-treated goethite, pure FeS, and Fe(II)-treated FeS in order to isolate and evaluate the influence of different mineral fractions on reaction rates. Initial rates of CT transformation were measured for different pH values and concentrations of added Fe(II), as well as different aging times and conditions. The following dissolved species and iron and sulfur mineral fractions were quantified and compared with CT transformation rates: aqueous Fe(2+) and S(-II), surface associated Fe(II) (including weakly and strongly bound Fe(II)), FeS(s), and Cr(II) reducible solid phase S. Over the pH range of 6-10, CT transformation rates were correlated with surface associated Fe(II), while at pH 8, rates were correlated with weakly bound Fe(II). Aging of S(-II)-treated goethite led to oxidation of surface sulfur and a change in the concentration of weakly bound Fe(II), but did not change the relationship between initial rates and weakly bound Fe(II). The results of this research suggest that surface associated Fe(II) and weakly bound Fe(II) could serve as indicators of the potential for abiotic CT dechlorination in natural soils under sulfate-reducing conditions.

摘要

本研究的目的是在模拟硫酸盐还原和富含氧化铁的土壤及沉积物的体系中,确定与四氯化碳(CT)还原转化速率相关性最佳的溶解态物种或固相矿物组分。我们使用硫化物(S(-II))处理过的针铁矿作为模型体系,但也研究了Fe(II)和S(-II)处理过的针铁矿、Fe(II)处理过的针铁矿、纯FeS以及Fe(II)处理过的FeS,以便分离和评估不同矿物组分对反应速率的影响。针对不同的pH值、添加的Fe(II)浓度、不同的老化时间和条件,测量了CT转化的初始速率。对以下溶解态物种以及铁和硫矿物组分进行了定量分析,并与CT转化速率进行了比较:水相Fe(2+)和S(-II)、表面结合的Fe(II)(包括弱结合和强结合的Fe(II))、FeS(s)以及可被Cr(II)还原的固相S。在pH值为6 - 10的范围内,CT转化速率与表面结合的Fe(II)相关,而在pH值为8时,速率与弱结合的Fe(II)相关。S(-II)处理过的针铁矿的老化导致表面硫的氧化以及弱结合的Fe(II)浓度的变化,但并未改变初始速率与弱结合的Fe(II)之间的关系。本研究结果表明,在硫酸盐还原条件下,表面结合的Fe(II)和弱结合的Fe(II)可作为天然土壤中非生物CT脱氯潜力的指标。

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