Separation and Purification Technology ( IF 8.1 ) Pub Date : 2023-10-04 , DOI: 10.1016/j.seppur.2023.125271 Miao Lu , Siyuan Zhang , Zhongmei Song , Liang Ma , Haining Liu , Ming Fang , Huifang Zhang , Xiushen Ye , Zhijian Wu
Increased levels of octadecylamine (ODA) and 4-dodecylmorpholine (DMP) in the aqueous, primarily utilized as flotation agents in the worldwide production of potash fertilizer, imperil the stability of ecosystems and the downstream production of high-end chemicals. Nevertheless, there is a dearth of exhaustive studies pertaining to the elimination of ODA and DMP. Herein, the Ti/SnO2-Sb/β-PbO2 anode was fabricated by a thermal decomposition-electrodeposition technique for the electrocatalytic degradation of ODA and DMP. The degradation efficiency of ODA and DMP can achieve complete degradation, reaching 100%, after treatment periods of 10 min and 120 min, respectively. Meanwhile, the TOC removal efficiency of ODA and DMP is up to 85% and 61% at 30 min and 120 min, respectively. In particular, sulphate exhibits inhibitory degradation activity of ODA and DMP in comparison to chloride salt. The recycling and accelerated lifetime tests indicate excellent stability and recyclability of the Ti/SnO2-Sb/β-PbO2 electrode. The mechanism of electrocatalytic degradation involves indirect electrochemical oxidation mediated by free radicals. The primary reactive species responsible for the degradation of DMP and ODA, as determined through scavenger quenching experiments and ESR, are ·OH and Cl·. The degradation of the ODA and DMP commences with the elimination of N element, leading to the formation of the . The carbon chain subsequently undergoes the breakdown. The degradation pathways of ODA and DMP were also proposed based on the GC–MS and H-NMR analyses, respectively. Moreover, the Ti/SnO2-Sb/β-PbO2 anode performed excellently in the removal of ODA and DMP in real samples, TOC removal from ODA and DMP in natural samples was 56% and 52%, respectively, within 180 min. This study provides the first exploration of electrocatalytic degradation mechanisms and pathways of ODA and DMP based on the Ti/SnO2-Sb/β-PbO2 anode.
中文翻译:
Ti/SnO2-Sb/β-PbO2 阳极在高盐度条件下电催化降解十八胺和 4-十二烷基吗啉:活性和机制见解
水中十八胺 (ODA) 和 4-十二烷基吗啉 (DMP) 的含量增加,主要用作全球钾肥生产中的浮选剂,危及生态系统的稳定性和高端化学品的下游生产。然而,缺乏关于取消官方发展援助和官方发展计划的详尽研究。本文通过热分解-电沉积技术制备了Ti/SnO 2 -Sb/β-PbO 2阳极,用于电催化降解ODA和DMP。ODA和DMP的降解效率分别在10 min和120 min后即可实现完全降解,达到100%。同时,ODA和DMP的TOC去除率在30分钟和120分钟时分别高达85%和61%。特别地,与氯化物盐相比,硫酸盐表现出ODA和DMP的抑制降解活性。回收和加速寿命测试表明Ti/SnO 2 -Sb/β-PbO 2电极具有优异的稳定性和可回收性。电催化降解的机制涉及自由基介导的间接电化学氧化。通过清除剂猝灭实验和 ESR 确定,负责 DMP 和 ODA 降解的主要活性物质是·OH 和 Cl·。ODA 和 DMP 的降解从 N 元素的消除开始,导致形成。碳链随后发生断裂。还分别根据 GC-MS 和 H-NMR 分析提出了 ODA 和 DMP 的降解途径。此外,Ti/SnO 2 -Sb/β-PbO 2阳极在实际样品中ODA和DMP的去除方面表现出色,在180 min内对自然样品中ODA和DMP的TOC去除率分别为56%和52%。本研究首次探索了基于Ti/SnO 2 -Sb/β-PbO 2阳极的ODA和DMP的电催化降解机制和途径。