State Key Laboratory of Water Environment Simulation, School of Environment, Beijing Normal University, Beijing 100875, PR China.
Chemosphere. 2010 May;79(10):987-96. doi: 10.1016/j.chemosphere.2010.03.029. Epub 2010 Apr 14.
The erbium (Er)-chitosan-fluorine (F) modified PbO(2) electrode was prepared by electrodeposition method, and its use for adsorption and electrochemical degradation of 2,4-dichlorophenol (2,4-DCP) in aqueous solution was compared with F-PbO(2) and Er-F-PbO(2) electrodes in a batch experiment. The electrodes were characterized by scanning electron microscopy, X-ray diffraction and cyclic voltammetry. Degradation of 2,4-DCP depending on Er and chitosan contents was discussed. The results showed that Er(2)O(3) and chitosan were scattered between the prevailing crystal structure of beta-PbO(2) and thus decreased the internal stress of PbO(2) film. Prior to each electrolysis, the modified PbO(2) anode was first pre-saturated with 2,4-DCP solution for 360 min to preclude the 2,4-DCP decrease due to adsorption. Among the electrodes examined in our study, the highest adsorption and electrochemical degradation for 2,4-DCP and TOC removals that are due to oxidation and adsorption of the organic products onto the chitosan was observed on Er-chitosan-F-PbO(2) electrode. At an applied current density of 5 mAcm(-2), the removal percentages of 2,4-DCP and TOC (solution volume: 180 mL, initial 2,4-DCP concentration: 90 mgL(-1)) were 95% after 120 min and 53% after 360 min, respectively. At Er amount of 10mM in the precursor coating solution, the degradation and mineralization removal for 2,4-DCP on the Er-F-PbO(2) electrode reached a maximum. At chitosan amount of 5 gL(-1), the highest TOC removal on the Er-chitosan-F-PbO(2) electrode was observed. Intermediates mainly including aliphatic carboxylic acids were examined and a possible degradation pathway for 2,4-DCP in aqueous solution involving dechlorination and hydroxylation reactions was proposed.
采用电化学沉积法制备了铒(Er)-壳聚糖-氟(F)修饰的 PbO2 电极,并将其用于吸附和电化学降解水溶液中的 2,4-二氯苯酚(2,4-DCP),与 F-PbO2 和 Er-F-PbO2 电极在批处理实验中进行了比较。通过扫描电子显微镜、X 射线衍射和循环伏安法对电极进行了表征。讨论了 Er 和壳聚糖含量对 2,4-DCP 降解的影响。结果表明,Er2O3 和壳聚糖分散在β-PbO2 的主要晶体结构之间,从而降低了 PbO2 薄膜的内应力。在每次电解之前,先将改性 PbO2 阳极用 2,4-DCP 溶液预饱和 360 min,以排除因吸附而导致的 2,4-DCP 减少。在所研究的电极中,观察到 Er-壳聚糖-F-PbO2 电极对 2,4-DCP 和 TOC 的去除具有最高的吸附和电化学降解效果,这归因于有机产物的氧化和吸附到壳聚糖上。在 5 mAcm(-2)的施加电流密度下,在 120 min 后去除率为 95%,在 360 min 后去除率为 53%,去除率为 95%,溶液体积为 180 mL,初始 2,4-DCP 浓度为 90 mgL(-1)。在前驱体涂层溶液中 Er 量为 10mM 时,Er-F-PbO2 电极上 2,4-DCP 的降解和矿化去除达到最大值。在壳聚糖量为 5 gL(-1)时,在 Er-壳聚糖-F-PbO2 电极上观察到最高的 TOC 去除率。检测到的中间产物主要包括脂肪族羧酸,并提出了水溶液中 2,4-DCP 的可能降解途径,涉及脱氯和羟化反应。