Li Shuilian, Zhang Lishan, Zhong Shan, Zhu Jiayan, Wei Zengxian
School of Life and Environment Sciences, Guilin University of Electronic Technology, Guilin, Guangxi 541004, China; Geological Resources and Environmental Testing Laboratory, Pengzhou, Sichuan 611930, China.
School of Life and Environment Sciences, Guilin University of Electronic Technology, Guilin, Guangxi 541004, China; Key Laboratory of Ecology of Rare and Endangered Species and Environmental Protection, Guangxi Normal University, Guilin, Guangxi 541001, China E-mail:
Water Sci Technol. 2025 Mar;91(5):609-625. doi: 10.2166/wst.2025.033. Epub 2025 Feb 28.
This study reports the preparation of granular ternary micro-electrolysis materials and their effectiveness in removing the emerging contaminant PFOA. Al/nZVI/C@F granules were synthesized using a liquid-phase reduction method combined with high-temperature calcination. By comparing the removal of methylene blue dye by granules, the optimum preparation conditions were determined as follows: Fe:C = 5:1, fly ash = 50%, calcination temperature = 800 °C, and holding time = 1 h. Static batch experiments revealed that under optimal conditions (PFOA concentration = 25 mg/L, solid-liquid ratio = 30 g/L, pH = 3, reaction temperature = 15 °C), Al/nZVI/C@F achieved a PFOA removal rate of 97.83%. The removal efficiency of Al/nZVI/C@F (93.90%) was significantly higher than that of commercial iron-carbon (12.75%). After 45 days of dynamic column experiments, the removal efficiency of nZVI/C@F and Al/nZVI/C@F for PFOA (50 mg/L) remained above 60%, demonstrating strong practical application potential. Further adsorption-desorption experiments revealed that nZVI/C@F and Al/nZVI/C@F primarily removed 50 mg/L PFOA through adsorption. For a lower PFOA concentration of 0.5 mg/L, the defluorination rates were 53.2% for nZVI/C@F and 68.9% for Al/nZVI/C@F. High-performance liquid chromatography-tandem mass spectrometry was used to analyze the intermediates formed during PFOA removal, leading to a proposed degradation pathway.
本研究报道了颗粒状三元微电解材料的制备及其对新兴污染物全氟辛酸（PFOA）的去除效果。采用液相还原法结合高温煅烧合成了Al/nZVI/C@F颗粒。通过比较颗粒对亚甲基蓝染料的去除效果，确定了最佳制备条件如下：铁与碳的比例为5:1，粉煤灰含量为50%，煅烧温度为800℃，保温时间为1小时。静态间歇实验表明，在最佳条件下（PFOA浓度为25mg/L，固液比为30g/L，pH值为3，反应温度为15℃），Al/nZVI/C@F对PFOA的去除率达到97.83%。Al/nZVI/C@F的去除效率（93.90%）显著高于商业铁碳材料（12.75%）。经过45天的动态柱实验，nZVI/C@F和Al/nZVI/C@F对50mg/L PFOA的去除效率保持在60%以上，显示出很强的实际应用潜力。进一步的吸附-解吸实验表明，nZVI/C@F和Al/nZVI/C@F主要通过吸附去除50mg/L的PFOA。对于较低浓度的0.5mg/L PFOA，nZVI/C@F的脱氟率为53.2%，Al/nZVI/C@F的脱氟率为68.9%。采用高效液相色谱-串联质谱法分析了PFOA去除过程中形成的中间产物，提出了降解途径。
