State Key Laboratory of Urban Water Resources Center, Department of Municipal and Environmental Engineering, Harbin Institute of Technology, Harbin, 150090, PR China; Centre for Water Research, Department of Civil and Environmental Engineering, National University of Singapore, 1 Engineering Dr. 2, Singapore, 117576, Singapore.
Centre for Water Research, Department of Civil and Environmental Engineering, National University of Singapore, 1 Engineering Dr. 2, Singapore, 117576, Singapore.
Chemosphere. 2018 Jun;201:687-696. doi: 10.1016/j.chemosphere.2018.02.186. Epub 2018 Mar 5.
A composite nickel-iron-foam (Ni-Fe-F) electrode was used as a cathode in the electro-Fenton (EF) process at circum-neutral pH in the presence of sodium tripolyphosphate (TPP) as supporting electrolyte. It was found that phenol degradation was dramatically improved by the synergistic effect of Ni-Fe-F and TPP, reaching 100% removal in 40 min, with k = (8.90 ± 0.12) × 10 min, which was about 18 times higher than that of Ni-Fe-F with sulfate as conventional electrolyte at pH 3.00 (k = (5.00 ± 0.14) × 10 min). A (75.00 ± 1.67)% mineralization yield was attained after 4-h treatment time. Ni-Fe-F proved capable of providing the Fe ions necessary to catalyze the Fenton's reaction via a controlled chemical/electrochemical redox process. In addition, Ni-Fe-F promoted the chemical and electrochemical generation of HO. With respect to TPP, its chelation with Fe ions prevented iron precipitation at neutral and higher pH values, extending the pH range of the Fenton's reaction. Furthermore, the TPP ligand promoted the activation of molecular O for the chemical production of OH, enhancing the process efficiency. By overcoming these common limitations of conventional EF in KSO electrolyte, the Ni-Fe-F/TPP system represents a more sustainable alternative for practical application of EF. A degradation pathway for phenol mineralization with homogeneous and heterogeneous OH produced by the EF Ni-Fe-F/TPP system is proposed based on the identification of the oxidation by-products.
一种复合镍铁泡沫(Ni-Fe-F)电极在中性 pH 条件下,以三聚磷酸钠(TPP)作为支持电解质,在电芬顿(EF)过程中用作阴极。研究发现,Ni-Fe-F 和 TPP 的协同作用显著提高了苯酚的降解效率,在 40 分钟内达到 100%去除,k 值为(8.90±0.12)×10 min,约为 pH 3.00 时以硫酸盐为常规电解质的 Ni-Fe-F 的 18 倍(k 值为(5.00±0.14)×10 min)。经过 4 小时处理时间,达到了(75.00±1.67)%的矿化率。Ni-Fe-F 能够通过控制化学/电化学氧化还原过程提供催化 Fenton 反应所需的 Fe 离子。此外,Ni-Fe-F 促进了 HO 的化学和电化学生成。对于 TPP,它与 Fe 离子的螯合作用防止了在中性和更高 pH 值下铁的沉淀,从而扩展了 Fenton 反应的 pH 范围。此外,TPP 配体促进了分子 O 的活化,用于 OH 的化学生成,提高了处理效率。通过克服 KSO 电解质中传统 EF 的这些常见限制,Ni-Fe-F/TPP 系统代表了一种更可持续的替代方案,适用于 EF 的实际应用。基于氧化产物的鉴定,提出了 EF Ni-Fe-F/TPP 系统产生的均相和非均相 OH 对苯酚矿化的降解途径。