pH值对纳米零价铁吸附降解2,4-二氯苯酚的影响

在不同pH条件下,对纳米铁(颗粒粒径为30～40 nm)及其降解2,4-二氯苯酚反应体系进行取样,并进行透射电子显微镜(TEM)、扫描电子显微镜-能谱联用(SEM-EDX)以及电感耦合等离子体发射光谱(ICP-OES)等形貌观测与分析表征,以考察pH值在纳米零价铁降解氯酚反应过程中的影响和作用.结果表明,在降解2,4-二氯苯酚的过程中纳米铁由分散的颗粒逐渐团聚,其表面逐渐氧化,并最终被呈针状结晶的碱式氧化亚铁(FeOOH)覆盖,从而阻碍了降解反应的进一步进行.在酸性体系中,纳米零价铁的氧化和团聚现象有所缓解,尽管会造成一部分铁量的损失,但反应产生大量的亚铁离子参与并促进了脱氯降解反应的进行,反应过程中溶液pH值有逐渐升高的趋势.不同pH条件下,纳米铁对氯酚的去除率随pH值的降低而升高,酸性条件有利于提高氯酚的还原降解速率,当pH=3时,24 h内氯酚的去除率可达到90%以上.

Effects of pH Value on the Adsorption and Degradation of 2,4-DCP by Nanoscale Zero-Valent Iron

To evaluate the effect of pH on the degradation of 2,4-DCP by zero-valent iron nanoparticles (with the particle size of 30-40 nm in diameter) samples were taken for TEM, SEM-EDX, and ICP-OES analysis and investigated on the particle morphology changes and 2,4-DCP removal under different pH conditions. It is shown that iron nanoparticles agglomerate from individual particles and tiny clusters into massive aggregate assemblies with their surfaces oxidized and coated by the needle-like rotten iron oxide products (FeOOH) in the degradation process, which will block up a further reaction of 2,4-DCP dechlorination, while the low pH value condition in acidic system can effectively suppress particles aggregation and the surface oxidation, although iron loss in the solid phase is somehow inevitable. Large quantity of Fe²⁺ ions soaked out from iron nanoparticles significantly promote 2,4-DCP removal by reduction, and the solution pH tends to go up in the reaction process. Acidic conditions facilitate 2,4-DCP dechlorination, and the removal efficiency became higher with the pH reduced, in which 90% of 2,4-DCP removal is reached in 24 h under the pH value of 3.