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.
J Environ Sci (China). 2020 Apr;90:87-97. doi: 10.1016/j.jes.2019.11.014. Epub 2019 Dec 9.
A novel insight on the role of interactions between target pollutants and the catalyst in the copper-containing layered double oxide (LDO)-catalyzed persulfate (PS) system was elucidated in the present study. 4-Chlorophenol (4-CP), as a representative benzene derivative with a hydroxyl group, was completely removed within 5 min, which was much faster than the reaction of monochlorobenzene (MCB) without a hydroxyl group, with the degradation efficiency of 31.7% in 240 min. Through the use of radical quenching and surface inhibition experiments, it could be concluded that the interaction between 4-CP and CuMgFe-LDO, rather than free radicals, played a key role in the decomposition of 4-CP, while only the free radicals participated in the MCB degradation process. According to electron paramagnetic resonance and X-ray photoelectron spectroscopy data, the formation of a Cu(II)-complex between phenolic hydroxyl groups and surface Cu(II) was primarily responsible for the degradation of phenolic compounds, in which PS accepted one electron from the complex and generated sulfate radicals and chelated radical cations. The chelated radical cations transferred one electron to Cu(II) followed by Cu(I) generation and pollutant degradation successively.
本研究阐明了目标污染物与催化剂之间相互作用在含铜层状双氧化物(LDO)催化过硫酸盐(PS)体系中的作用的新见解。以具有羟基的代表性苯衍生物 4-氯苯酚(4-CP)为例,它在 5 分钟内完全去除,这比没有羟基的一氯苯(MCB)的反应快得多,在 240 分钟内的降解效率为 31.7%。通过使用自由基猝灭和表面抑制实验,可以得出结论,4-CP 与 CuMgFe-LDO 之间的相互作用,而不是自由基,在 4-CP 的分解中起着关键作用,而只有自由基参与了 MCB 的降解过程。根据电子顺磁共振和 X 射线光电子能谱数据,酚羟基与表面 Cu(II) 之间形成 Cu(II)-配合物是酚类化合物降解的主要原因,其中 PS 从配合物中接受一个电子,生成硫酸根自由基和螯合自由基阳离子。螯合自由基阳离子将一个电子转移到 Cu(II),随后依次生成 Cu(I)并降解污染物。