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CNT/Nafion functionalized Ti/SnO2-Sb/β-PbO2-CNT/Nafion composite electrode toward highly active and robust degradation of octadecylamine and 4-dodecylmorpholine in real high-salinity system
Chemical Engineering Journal ( IF 13.3 ) Pub Date : 2024-05-31 , DOI: 10.1016/j.cej.2024.152716 Miao Lu , Siyuan Zhang , Liang Ma , Zhongmei Song , Xiushen Ye , Huifang Zhang , Haining Liu , Zhijian Wu
Chemical Engineering Journal ( IF 13.3 ) Pub Date : 2024-05-31 , DOI: 10.1016/j.cej.2024.152716 Miao Lu , Siyuan Zhang , Liang Ma , Zhongmei Song , Xiushen Ye , Huifang Zhang , Haining Liu , Zhijian Wu
The efficient removal of recalcitrant organics in high-salinity systems, specifically brine, poses a significant challenge for electrochemically advanced oxidation processes in terms of both activity and stability. Herein, a composite electrode comprising of CNT/Nafion functionalized Ti/SnO2 -Sb/β-PbO2 -CNT/Nafion was developed for efficient and stable removal of octadecylamine (ODA) and 4-dodecylmorpholine (DMP) in a real high-salinity environment. The degradation efficiencies of ODA and DMP on the composite electrode can reach 100 % within 60 min, respectively. The total organic carbon (TOC) removal efficiency of ODA and DMP was significantly improved to 78 % and 66 % with remarkably low energy consumption (0.414 and 1.402 kWh/g TOC), respectively. The electrochemical characterizations demonstrate that the composite electrode exhibits improved electrochemical activity (oxygen evolution potentials = 1.791 V) and electrode surface area (ECSA = 20 cm2 ), while maintaining reduced charge transfer resistance (Rct = 18.21 Ω/cm2 ) and enhanced corrosion-resistant capacity (corrosion potential = 1.115 V). Based on recycling and accelerated lifespan testing, the composite electrode demonstrates exceptional stability and recyclability. Additionally revealed was the linked stability mechanism. The electrocatalytic degradation of ODA and DMP begins with the removal of amino and morpholine rings, and then the decomposition of the carbon chains. Gas chromatography-mass spectrometry (GC–MS) and theoretical calculations were used to identify intermediate products generated during the degradation of ODA and DMP, and possible degradation pathways were provided in high-salinity systems, respectively. This work offered a fresh perspective on electrocatalytic oxidation for a real high-salinity system that is more efficient and stable.
中文翻译:
CNT/Nafion 功能化的 Ti/SnO2-Sb/β-PbO2-CNT/Nafion 复合电极在真正的高盐度体系中对十八烷胺和 4-十二烷基吗啉进行高活性和稳健降解
在高盐度系统中有效去除顽固有机物,特别是盐水,在活性和稳定性方面对电化学高级氧化过程构成了重大挑战。在此,开发了一种由 CNT/Nafion 官能化的 Ti/SnO2-Sb/β-PbO2-CNT/Nafion 组成的复合电极,用于在真正的高盐度环境中高效稳定地去除十八烷胺 (ODA) 和 4-十二烷基吗啉 (DMP)。ODA 和 DMP 在复合电极上的降解效率可在 60 min 内分别达到 100 %。ODA 和 DMP 的总有机碳 (TOC) 去除效率显著提高至 78 % 和 66 %,能耗极低(0.414 和 1.402 kWh/g TOC)。电化学特性表明,复合电极表现出更好的电化学活性(析氧电位 = 1.791 V)和电极表面积 (ECSA = 20 cm2),同时保持较低的电荷转移电阻 (Rct = 18.21 Ω/cm2) 和增强的耐腐蚀能力 (腐蚀电位 = 1.115 V)。基于回收和加速使用寿命测试,复合电极表现出卓越的稳定性和可回收性。此外,还揭示了相关的稳定性机制。ODA 和 DMP 的电催化降解从去除氨基和吗啉环开始,然后分解碳链。采用气相色谱-质谱 (GC-MS) 和理论计算鉴定 ODA 和 DMP 降解过程中产生的中间产物,并分别提供了高盐度系统中可能的降解途径。 这项工作为电催化氧化提供了新的视角,以实现更高效、更稳定的真正高盐度系统。
更新日期:2024-05-31
中文翻译:
CNT/Nafion 功能化的 Ti/SnO2-Sb/β-PbO2-CNT/Nafion 复合电极在真正的高盐度体系中对十八烷胺和 4-十二烷基吗啉进行高活性和稳健降解
在高盐度系统中有效去除顽固有机物,特别是盐水,在活性和稳定性方面对电化学高级氧化过程构成了重大挑战。在此,开发了一种由 CNT/Nafion 官能化的 Ti/SnO2-Sb/β-PbO2-CNT/Nafion 组成的复合电极,用于在真正的高盐度环境中高效稳定地去除十八烷胺 (ODA) 和 4-十二烷基吗啉 (DMP)。ODA 和 DMP 在复合电极上的降解效率可在 60 min 内分别达到 100 %。ODA 和 DMP 的总有机碳 (TOC) 去除效率显著提高至 78 % 和 66 %,能耗极低(0.414 和 1.402 kWh/g TOC)。电化学特性表明,复合电极表现出更好的电化学活性(析氧电位 = 1.791 V)和电极表面积 (ECSA = 20 cm2),同时保持较低的电荷转移电阻 (Rct = 18.21 Ω/cm2) 和增强的耐腐蚀能力 (腐蚀电位 = 1.115 V)。基于回收和加速使用寿命测试,复合电极表现出卓越的稳定性和可回收性。此外,还揭示了相关的稳定性机制。ODA 和 DMP 的电催化降解从去除氨基和吗啉环开始,然后分解碳链。采用气相色谱-质谱 (GC-MS) 和理论计算鉴定 ODA 和 DMP 降解过程中产生的中间产物,并分别提供了高盐度系统中可能的降解途径。 这项工作为电催化氧化提供了新的视角,以实现更高效、更稳定的真正高盐度系统。