College of Water Sciences, Beijing Normal University, Beijing, 100875, China; State Key Laboratory of Environmental Criteria and Risk Assessment, Chinese Research Academy of Environmental Sciences, Beijing, 100012, China.
Technical Center for Soil, Agricultural and Rural Ecology and Environment, Ministry of Ecology and Environment of the People's Republic China, Beijing, 100012, China.
Chemosphere. 2021 Dec;284:131166. doi: 10.1016/j.chemosphere.2021.131166. Epub 2021 Jun 13.
Tetrabromobisphenol A (TBBPA) greatly impacts on ecosystems and human health due to its high environmental toxicity and persistence. Persulfate (PS) advanced oxidation technology to remove organic pollutants in soils has received intense attention. In this study, nanoscale zero-valent iron (nZVI) was synthesized through the borohydride reduction method to explore its activating potential towards PS to accelerate the degradation of TBBPA in soils. The degradation behaviors of TBBPA in soils were investigated by batch experiments. The degradation efficiency of TBBPA (5 mg kg) was 78.32% within 12 h under the following reaction conditions: 3 g kg nZVI, 25 mM PS, and pH 5.5 at 25 °C. Notably, PS can be used effectively, and the pH changed slightly in the reaction system. Oxidative degradation of TBBPA is favored at higher temperatures and lower pH values, while it is inhibited when the amount of catalyst increases significantly. The coexisting heavy metal ions such as Zn(II) and Ni(II) inhibit TBBPA degradation, while Cu(II) accelerates the degradation. Radical scavenging and electron spin resonance (ESR) tests further confirmed the generation of SO, ·OH, and O in nZVI activated PS. The intermediates identified by gas chromatograph-mass spectrometry analysis indicated that TBBPA via debromination and the cleavage between the isopropyl group and one of the benzene rings complete degradation. These findings provide new insight into the mechanism of nZVI activation of PS and will promote its application in the degradation of refractory organic compounds.
四溴双酚 A(TBBPA)由于其高环境毒性和持久性,对生态系统和人类健康有很大影响。过硫酸盐(PS)高级氧化技术用于去除土壤中的有机污染物受到了广泛关注。本研究通过硼氢化还原法合成了纳米零价铁(nZVI),探索其对 PS 的活化潜力,以加速土壤中 TBBPA 的降解。通过批实验研究了 TBBPA 在土壤中的降解行为。在以下反应条件下,土壤中 TBBPA(5mgkg)在 12h 内的降解效率为 78.32%:3gkg nZVI、25mM PS 和 25°C 时 pH 值为 5.5。值得注意的是,反应体系中 PS 可以有效利用,且 pH 值变化较小。TBBPA 的氧化降解在较高温度和较低 pH 值下有利,而当催化剂用量显著增加时则受到抑制。共存的重金属离子如 Zn(II)和 Ni(II)抑制 TBBPA 的降解,而 Cu(II)则加速降解。自由基捕获和电子自旋共振(ESR)测试进一步证实了 nZVI 活化 PS 生成 SO4·-、·OH 和 O2的过程。气相色谱-质谱分析鉴定的中间产物表明,TBBPA 通过脱溴和异丙基与苯环之一之间的断裂完成降解。这些发现为 nZVI 活化 PS 的机制提供了新的见解,并将促进其在难降解有机化合物降解中的应用。