Key Laboratory of Soil Environment and Pollution Remediation, Institute of Soil Science, Chinese Academy of Sciences, Nanjing, 210008, China; University of Chinese Academy of Sciences, Beijing, 100049, China.
Key Laboratory of Soil Environment and Pollution Remediation, Institute of Soil Science, Chinese Academy of Sciences, Nanjing, 210008, China; University of Chinese Academy of Sciences, Beijing, 100049, China.
Chemosphere. 2020 May;246:125849. doi: 10.1016/j.chemosphere.2020.125849. Epub 2020 Jan 6.
The sodium pyrophosphate (SP)-enhanced Fenton reaction has been proven to have promising potential in remediation of polychlorinated biphenyls in soils by keeping iron ions soluble at high pH and minimizing the useless decomposition of HO. However, little information can be obtained about the effect of environmental factors on its remediation performance. Thus, the effect of environmental factors on the degradation of 2,2',5-trichlorodiphenyl (PCB18), one of the main PCB congeners in Chinese sites, was investigated in this study. PCB18 degradation was sensitive to pH, which ranged from 39.8% to 99.5% as increased pH from 3.0 to 9.0. ·OH was responsible for PCB18 degradation at pH 5.0, while both ·OH and O resulted in PCB 18 degradation at pH 7.0 with the calculated reaction activation energy of 73.5 kJ mol. Bivalent cations and transition metal ions decreased PCB18 degradation markedly as their concentrations increased. The addition of humic acid had an inhibitory on PCB18 degradation, but no obvious inhibition of PCB18 removal was observed when the same concentration of fulvic acid was added. The addition of 1 and 10 μM model humic constituents (MHCs) promoted PCB18 degradation, but the addition of 100 μM MHCs decreased PCB18 removal. Biphenyl, two dichlorobiphenyl, and two hydroxy trichlorobiphenyl derivatives were identified as the major degradation products of PCB18 in the Fe/SP/HO system at pH 7.0. Thus, an oxidative pathway contributed by OH and a reductive pathway induced by O were proposed as the main mechanisms for PCB18 degradation in the SP-enhanced Fenton reaction.
焦磷酸钠(SP)增强的芬顿反应已被证明在修复土壤中的多氯联苯方面具有很大的潜力,因为它可以在高 pH 值下保持铁离子的可溶性,并最大限度地减少 HO 的无用分解。然而,关于环境因素对其修复性能的影响,我们了解甚少。因此,本研究考察了环境因素对 2,2',5-三氯二苯(PCB18)降解的影响,PCB18 是中国污染场地中主要的多氯联苯同系物之一。PCB18 的降解对 pH 敏感,当 pH 值从 3.0 增加到 9.0 时,降解率从 39.8%增加到 99.5%。在 pH 5.0 时,·OH 负责 PCB18 的降解,而在 pH 7.0 时,·OH 和 O 共同导致 PCB18 的降解,计算得到的反应活化能为 73.5 kJ/mol。二价阳离子和过渡金属离子的浓度增加会显著降低 PCB18 的降解。腐殖酸的添加对 PCB18 的降解有抑制作用,但当添加相同浓度的富里酸时,对 PCB18 的去除没有明显的抑制作用。1 和 10 μM 模型腐殖质组分(MHCs)的添加促进了 PCB18 的降解,但添加 100 μM MHCs 降低了 PCB18 的去除率。在 pH 7.0 时,Fe/SP/HO 体系中鉴定出 PCB18 的主要降解产物为联苯、两种二氯联苯和两种羟基三氯联苯衍生物。因此,提出了 OH 引发的氧化途径和 O 诱导的还原途径作为 SP 增强的芬顿反应中 PCB18 降解的主要机制。