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通过铁电极对过硫酸盐反应性进行电解调控以降解地下水中的三氯乙烯

Electrolytic manipulation of persulfate reactivity by iron electrodes for trichloroethylene degradation in groundwater.

作者信息

Yuan Songhu, Liao Peng, Alshawabkeh Akram N

机构信息

State Key Lab of Biogeology and Environmental Geology, China University of Geosciences , 388 Lumo Road, Wuhan, Hubei 430074, P. R. China.

出版信息

Environ Sci Technol. 2014;48(1):656-63. doi: 10.1021/es404535q. Epub 2013 Dec 19.

Abstract

Activated persulfate oxidation is an effective in situ chemical oxidation process for groundwater remediation. However, reactivity of persulfate is difficult to manipulate or control in the subsurface causing activation before reaching the contaminated zone and leading to a loss of chemicals. Furthermore, mobilization of heavy metals by the process is a potential risk. An effective approach using iron electrodes is thus developed to manipulate the reactivity of persulfate in situ for trichloroethylene (TCE) degradation in groundwater and to limit heavy metals mobilization. TCE degradation is quantitatively accelerated or inhibited by adjusting the current applied to the iron electrode, following k1 = 0.00053·Iv + 0.059 (-122 A/m(3) ≤ Iv ≤ 244 A/m(3)) where k1 and Iv are the pseudo first-order rate constant (min(-1)) and volume normalized current (A/m(3)), respectively. Persulfate is mainly decomposed by Fe(2+) produced from the electrochemical and chemical corrosion of iron followed by the regeneration via Fe(3+) reduction on the cathode. SO4(•-) and ·OH cocontribute to TCE degradation, but ·OH contribution is more significant. Groundwater pH and oxidation-reduction potential can be restored to natural levels by the continuation of electrolysis after the disappearance of contaminants and persulfate, thus decreasing adverse impacts such as the mobility of heavy metals in the subsurface.

摘要

活化过硫酸盐氧化法是一种用于地下水修复的有效原位化学氧化工艺。然而,过硫酸盐在地下的反应活性难以操控或控制,会在到达污染区之前就发生活化,导致化学药剂损失。此外,该工艺使重金属迁移是一个潜在风险。因此,开发了一种使用铁电极的有效方法,以原位操控过硫酸盐的反应活性,用于降解地下水中的三氯乙烯(TCE)并限制重金属迁移。通过调节施加到铁电极上的电流,TCE的降解会定量加速或受到抑制,遵循k1 = 0.00053·Iv + 0.059(-122 A/m³ ≤ Iv ≤ 244 A/m³),其中k1和Iv分别是伪一级反应速率常数(min⁻¹)和体积归一化电流(A/m³)。过硫酸盐主要由铁的电化学和化学腐蚀产生的Fe²⁺分解,随后通过阴极上Fe³⁺的还原实现再生。SO₄•⁻和·OH共同促进TCE的降解,但·OH的贡献更为显著。在污染物和过硫酸盐消失后,通过持续电解可将地下水的pH值和氧化还原电位恢复到自然水平,从而减少诸如地下重金属迁移等不利影响。

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