Li Changyu, Shen Cong, Gao Bin, Liang Wenxu, Zhu Yifan, Shi Weijie, Ai Shiyun, Xu Hongxia, Wu Jichun, Sun Yuanyuan
State Key Laboratory of Pollution Control and Resource Reuse, Key Laboratory of Surficial Geochemistry, Ministry of Education, School of Earth Sciences and Engineering, Hydrosciences Department, Nanjing University, Nanjing, 210023, China.
College of Chemistry and Material Science, Shandong Agricultural University, Taian, 271018, Shandong, China.
Chemosphere. 2024 Mar;351:141209. doi: 10.1016/j.chemosphere.2024.141209. Epub 2024 Jan 13.
Perfluorooctanoic acid (PFOA) is an emerging pollutant that is non-biodegradable and presents severe environmental and human health risks. In this study, we present an effective and mild approach for PFOA degradation that involves the use of nitrogen-doped carbon foam anchored with nanoscale zero-valent iron (nZVI@NCF) to activate low concentration peroxymonosulfate (PMS) for the treatment. The nZVI@NCF/PMS system efficiently removed 84.4% of PFOA (2.4 μM). The active sites of nZVI@NCF including Fe (110) and graphitic nitrogen played crucial roles in the degradation. Electrochemical analyses and density functional theory calculations revealed that nZVI@NCF acted as an electronic donor, transferring electrons to both PMS and PFOA during the reaction. By further analyzing the electron paramagnetic resonance and byproducts, it was determined that electron transfer and singlet oxygen were responsible for PFOA degradation. Three degradation pathways involving decarboxylation and surface reduction of PFOA in the nZVI@NCF/PMS system were determined. Finding from this study indicate that nZVI@NCF/PMS systems are effective in degrading PFOA and thus present a promising persulfate-advanced oxidation process technology for PFAS treatment.
全氟辛酸(PFOA)是一种新兴污染物,不可生物降解,对环境和人类健康构成严重风险。在本研究中,我们提出了一种有效且温和的PFOA降解方法,该方法涉及使用锚定纳米级零价铁的氮掺杂碳泡沫(nZVI@NCF)来激活低浓度过一硫酸盐(PMS)进行处理。nZVI@NCF/PMS系统有效去除了84.4%的PFOA(2.4 μM)。nZVI@NCF的活性位点包括Fe(110)和石墨氮在降解过程中起关键作用。电化学分析和密度泛函理论计算表明,nZVI@NCF作为电子供体,在反应过程中将电子转移给PMS和PFOA。通过进一步分析电子顺磁共振和副产物,确定电子转移和单线态氧是PFOA降解的原因。确定了nZVI@NCF/PMS系统中涉及PFOA脱羧和表面还原的三条降解途径。本研究结果表明,nZVI@NCF/PMS系统对PFOA降解有效,因此是一种有前景的用于全氟和多氟烷基物质(PFAS)处理的过硫酸盐高级氧化工艺技术。