School of Chemistry and Chemical Engineering, Xi'an University of Architecture and Technology, Xi'an, Shaanxi, 710055, China.
School of Chemistry and Chemical Engineering, Xi'an University of Architecture and Technology, Xi'an, Shaanxi, 710055, China.
Chemosphere. 2023 Sep;335:139074. doi: 10.1016/j.chemosphere.2023.139074. Epub 2023 May 30.
To solve the challenges facing the low-cost and high-efficiency purification of water pollution caused by the production and metabolism of biodegradable hydroxychloroquine (HCQ), electrooxidation treatment with a Ti-based PbO anode is the most promising technical solution for engineering applications. However, Ti-based PbO anodes have apparent disadvantages, such as poor stability and insufficient electrocatalytic activity. To overcome these shortcomings, a novel Ti/(Ti,Zr)N/PbO anode was prepared by introducing an arc-sprayed (Ti,Zr)N conductive composite interlayer together with a PbO surface layer anodically deposited at different times on a Ti substrate. The electrocatalytic activity, anode stability, optimized parameters and degradation mechanism of the HCQ electrooxidation treatment were experimentally studied. As a result, compared to the Ti/PbO anode without an interlayer, the Ti/(Ti,Zr)N/PbO anode not only showed obviously excellent stability but could also effectively electrocatalytically degrade HCQ. The optimal Ti/(Ti,Zr)N/PbO-2.0 anode prepared using the arc-sprayed (Ti,Zr)N interlayer and electrodepositing PbO for 2 h can remove 95.85% of 200 mg L HCQ at 20 °C and pH 7 after electrolysis at 20 mA cm for 3 h, and possesses a longer accelerated life with 11.8 times the lifetime of the Ti/PbO anode. Furthermore, after five consecutive periodic electrooxidation treatments, its degradation rate was retained at 86.3% and its Pb dissolution concentration (0.0036 mg L) met the requirements of the Chinese standard for drinking water. This long-acting PbO coated anode reveals promising application potential for the electrocatalytic degradation of refractory organic sewage, such as HCQ, which will help to promote the practical popularization of electrooxidation water treatment technology.
为了解决因羟氯喹(HCQ)生产和代谢而导致的水污染的低成本、高效率净化所面临的挑战,采用钛基 PbO 阳极进行电氧化处理是最有前途的工程应用技术解决方案。然而,钛基 PbO 阳极存在明显的缺点,如稳定性差和电催化活性不足。为了克服这些缺点,通过在 Ti 基体上依次弧喷涂(Ti,Zr)N 导电复合中间层和阳极电沉积不同时间的 PbO 表面层,制备了一种新型 Ti/(Ti,Zr)N/PbO 阳极。实验研究了 HCQ 电氧化处理的电催化活性、阳极稳定性、优化参数和降解机制。结果表明,与没有中间层的 Ti/PbO 阳极相比,Ti/(Ti,Zr)N/PbO 阳极不仅表现出明显优异的稳定性,而且能够有效地电催化降解 HCQ。采用弧喷涂(Ti,Zr)N 中间层和电沉积 PbO 2 h 制备的最佳 Ti/(Ti,Zr)N/PbO-2.0 阳极在 20 mA cm、20°C 和 pH 7 条件下,电解 3 h 可去除 200 mg L 的 200 mg L HCQ 的 95.85%,其加速寿命是 Ti/PbO 阳极的 11.8 倍。此外,在连续五次周期性电氧化处理后,其降解率仍保持在 86.3%,Pb 溶解浓度(0.0036 mg L)满足中国饮用水标准要求。这种长效 PbO 涂层阳极在电催化降解难处理有机污水(如 HCQ)方面具有广阔的应用前景,将有助于推动电氧化水处理技术的实际推广。