Zhang Zhen, Zhang Junya, Ye Xiaokun, Hu Yongyou, Chen Yuancai
The Key Laboratory of Pollution Control and Ecosystem Restoration in Industry Clusters, Ministry of Education, State Key Laboratory of Pulp and Paper Engineering, College of Environment and Energy, South China University of Technology, Guangzhou Higher Education Mega Centre, Guangzhou 510006, China E-mail:
Water Sci Technol. 2016;74(3):639-46. doi: 10.2166/wst.2016.215.
Ethylenediaminetetraacetic acid (EDTA) forms stable complexes with toxic metals such as nickel due to its strong chelation. The electro-Fenton (EF) process using a cathode made from palladium (Pd), reduced graphene oxide (RGO) and carbon felt, fed with air, exhibited high activities and stability for the removal of 10 mg L(-1) EDTA-Ni solution. Pd/RGO catalyst was prepared by one-pot synthesis; the scanning electron microscopy and X-ray diffraction analysis indicated nanoparticles and RGO were well distributed on carbon felt, forming three dimensional architecture with both large macropores and a mesoporous structure. The cyclic voltammetric results showed that the presence of RGO in Pd/RGO/carbon felt significantly increased the current response of two-electron reduction of O2 (0.45 V). The key factors influencing the removal efficiency of EDTA-Ni, such as pH, current and Fe(2+) concentration, were investigated. Under the optimum conditions, the removal efficiency of EDTA-Ni reached 83.8% after 100 min EF treatment. Mechanism analysis indicated that the introduction of RGO in Pd/RGO/carbon felt significantly enhanced the electrocatalytic activities by inducing •OH in the EF process; direct H2O2 oxidation still accounted for a large amount of EDTA-Ni removal efficiency.
乙二胺四乙酸(EDTA)由于其强大的螯合作用,能与镍等有毒金属形成稳定的络合物。使用由钯(Pd)、还原氧化石墨烯(RGO)和碳毡制成的阴极,并通入空气的电芬顿(EF)工艺,对10 mg L(-1) 的EDTA-Ni溶液具有高活性和稳定性。通过一锅法合成制备了Pd/RGO催化剂;扫描电子显微镜和X射线衍射分析表明,纳米颗粒和RGO在碳毡上分布良好,形成了具有大孔和介孔结构的三维结构。循环伏安结果表明,Pd/RGO/碳毡中RGO的存在显著增加了O2两电子还原的电流响应(0.45 V)。研究了影响EDTA-Ni去除效率的关键因素,如pH值、电流和Fe(2+)浓度。在最佳条件下,经100分钟的EF处理后,EDTA-Ni的去除效率达到83.8%。机理分析表明,在Pd/RGO/碳毡中引入RGO通过在EF过程中诱导•OH显著增强了电催化活性;直接H2O2氧化仍占大量的EDTA-Ni去除效率。