Ministry of Education Key Laboratory of Pollution Control and Ecological Remediation for Industrial Agglomeration Area, State Key Laboratory of Pulp and Paper Engineering, College of Environment and Energy, South China University of Technology, Guangzhou, 510006, PR China.
Ministry of Education Key Laboratory of Pollution Control and Ecological Remediation for Industrial Agglomeration Area, State Key Laboratory of Pulp and Paper Engineering, College of Environment and Energy, South China University of Technology, Guangzhou, 510006, PR China.
J Hazard Mater. 2018 Jan 5;341:128-137. doi: 10.1016/j.jhazmat.2017.07.014. Epub 2017 Jul 8.
Ethylenediaminetetraacetic acid (EDTA) could form stable complexes with toxic metals such as nickel due to its strong chelation. The three-dimensional (3D) macroporous graphene aerogels (GA), which was in-situ assembled by reduced graphene oxide (rGO) sheets on titanium wire as binder-free electrode, was presented as cathode for the degradation of EDTA-Ni in Electro-Fenton process. The X-ray diffraction (XRD), Scanning Electron Microscopy (SEM), Transmission Electron Microscope (TEM) and Brunauer-Emmett-Teller (BET) results indicated 3D GA formed three dimensional architecture with large and homogenous macropore structure and surface area. Cyclic Voltammetry (CV), Linear Sweep Voltammetry (LSV) and Rotating Ring-disk Electrode (RRDE) results showed that the 3D GA cathode at pH 3 displayed the highest current density and electrochemical active surface area (ECSA), and better two-electron selectivity for ORR than other pH value, confirming the 3D-GA cathode at pH 3 has the highest electrocatalytic activity and generates more HO. The factors such as pH, applied current density, concentration of Fe, NaSO and aeration rates of air were also investigated. Under the optimum conditions, 73.5% of EDTA-Ni was degraded after reaction for 2h. Mechanism analysis indicated that the production of OH on the 3D GA cathode played an important role in the removal of EDTA-Ni in the 3D GA-EF process, where the direct regeneration of Fe on the cathode would greatly reduce the consumption of HO. Therefore, it is of great promise for 3D-GA catalyst to be developed as highly efficient, cost-effective and durable cathode for the removal of EDTA-Ni.
乙二胺四乙酸(EDTA)因其强螯合作用,可与镍等有毒金属形成稳定的配合物。三维(3D)大孔石墨烯气凝胶(GA)是由还原氧化石墨烯(rGO)片在钛丝上原位组装而成的无粘结剂电极,作为电芬顿过程中 EDTA-Ni 降解的阴极。X 射线衍射(XRD)、扫描电子显微镜(SEM)、透射电子显微镜(TEM)和 Brunauer-Emmett-Teller(BET)结果表明,3DGA 形成了具有大而均匀的大孔结构和表面积的三维结构。循环伏安法(CV)、线性扫描伏安法(LSV)和旋转环盘电极(RRDE)结果表明,在 pH 3 下,3DGA 阴极具有最高的电流密度和电化学活性表面积(ECSA),对 ORR 的双电子选择性也优于其他 pH 值,这表明 3D-GA 阴极在 pH 3 时具有最高的电催化活性,并产生更多的 HO。还研究了 pH、施加电流密度、Fe、NaSO 浓度和空气曝气速率等因素。在最佳条件下,反应 2h 后,73.5%的 EDTA-Ni 被降解。机理分析表明,3DGA 阴极上 OH 的产生在 3DGA-EF 过程中 EDTA-Ni 的去除中起着重要作用,其中阴极上 Fe 的直接再生会大大减少 HO 的消耗。因此,3D-GA 催化剂作为高效、经济、耐用的阴极,用于去除 EDTA-Ni,具有很大的应用前景。