State key Laboratory of Environmental Aquatic Chemistry, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China.
State key Laboratory of Environmental Aquatic Chemistry, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China; China Academy of Urban Planning and Design, Beijing 100044, China.
Water Res. 2014 Mar 15;51:134-43. doi: 10.1016/j.watres.2013.12.028. Epub 2014 Jan 2.
The reductive removal of haloacetic acids (HAAs) in a three-dimensional electrochemical continuous reactor with Pd-granular activated carbon (Pd-GAC) particles as fixed filler and Pd-modified carbon paper (Pd-C) as cathode was studied in this research. Pd-C electrode was prepared from PdCl2 via electrodeposition onto carbon paper. Pd-GAC particles were prepared by the impregnation of Pd(2+) ions onto GAC. Efficient electrocatalytic reduction of HAAs in this reactor was exhibited. Effects of current density, initial HHAs concentration, and hydraulic retention time on the HHAs removal were investigated. Under the current density of 0.3 mA/cm(2), HAAs with initial concentration of 120 μg/L were reduced to be less than 60 μg/L with hydraulic retention time of 20 min. Electron transfer and HAAs diffusion both played an important role in controlling the electro-reduction process under the conditions of current density less than 0.6 mA/cm(2) with an initial HAAs concentration ranging from 120 to 600 μg/L. However, the HAAs diffusion became the primary rate-limiting step when the current density was higher than 0.6 mA/cm(2). The Pd(0) and Pd(2+) species were detected by X-ray photoelectron spectroscopy. The stability of the electrochemical reactor in the reduction removal of HAAs was also exhibited.
本研究采用 Pd-颗粒状活性炭(Pd-GAC)颗粒作为固定填充物和 Pd 修饰碳纸(Pd-C)作为阴极的三维电化学连续反应器,研究了卤乙酸(HAAs)的还原去除。Pd-C 电极是通过将 PdCl2 电沉积到碳纸上制备的。Pd-GAC 颗粒是通过将 Pd(2+)离子浸渍到 GAC 上制备的。该反应器表现出对 HAAs 的高效电催化还原。考察了电流密度、初始 HHAs 浓度和水力停留时间对 HHAs 去除的影响。在电流密度为 0.3 mA/cm2 的条件下,初始浓度为 120 μg/L 的 HAAs 在水力停留时间为 20 min 时被还原至低于 60 μg/L。在电流密度小于 0.6 mA/cm2 且初始 HAAs 浓度范围为 120 至 600 μg/L 的条件下,电子转移和 HAAs 扩散都对控制电还原过程起着重要作用。然而,当电流密度高于 0.6 mA/cm2 时,HAAs 扩散成为主要的限速步骤。通过 X 射线光电子能谱检测到 Pd(0)和 Pd(2+)物种。还展示了电化学反应器在还原去除 HAAs 中的稳定性。