Singlet Oxygen-Mediated Electrochemical Filter for Selective and Rapid Degradation of Organic Compounds,Industrial & Engineering Chemistry Research

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Singlet Oxygen-Mediated Electrochemical Filter for Selective and Rapid Degradation of Organic Compounds
Industrial & Engineering Chemistry Research ( IF 3.8 ) Pub Date : 2020-07-08 , DOI: 10.1021/acs.iecr.0c02223
Dongli Guo ₁ , Yanbiao Liu _{1,

2}

Affiliation

Singlet oxygen (¹O₂)-based homogeneous oxidation processes have been extensively investigated for selective degradation of organic substrates. Herein, to address the existing limitations of these homogeneous systems, we rationally designed a heterogeneous ¹O₂-mediated flow-through electrochemical system based on a functional carbon nanotubes cathode filter. We showed that hydrogen peroxide (H₂O₂), which was produced in situ with the application of an electric field, reacted with the hypochlorous ion (ClO^–) electrolyte to produce ¹O₂. Electrochemical filtration of 0.03 mM Methylene Blue (MB) at −2.5 V and a flow rate of 1.0 mL/min resulted in an oxidation flux of 2.62 ± 0.04 mmol/(h m²). The flow-through design introduced more convection, which lead to enhanced mass transport and, in turn, faster oxidation kinetics of organic compounds. Moreover, the oxidation of a mixed solution of cationic MB, cationic Rhodamine 6G (R6G), and anionic Methyl Orange (MO) yielded the selective oxidation of only MB and R6G, where the oxidation flux of MB and R6G was 3.7 and 3.0 times, respectively, greater than that of MO. In particular, the flow-through system exhibited a remarkable 20-times-higher MB oxidation efficiency, when compared with a conventional batch configuration (95.8% vs 4.9%). Electron paramagnetic resonance (EPR) techniques and quenching experiments verified the essential role of ¹O₂. The proposed flow-through system may provide a highly potent, efficient, and rapid approach for selective environmental remediation.

中文翻译：

单线态氧介导的电化学过滤器，用于有机化合物的选择性和快速降解

基于单线态氧（¹ O ₂）的均相氧化过程已被广泛研究用于有机底物的选择性降解。在本文中，为了解决这些均相系统的现有局限性，我们合理地设计了基于功能性碳纳米管阴极过滤器的异质¹ O ₂介导的流通式电化学系统。我们发现，过氧化氢（H ₂ ö ₂），将其产生的原位与电场的应用，与次氯酸离子（CLO反应^-）电解质中产生¹ Ò ₂。在-2.5 V和1.0 mL / min的流速下进行0.03 mM亚甲蓝（MB）的电化学过滤，氧化通量为2.62±0.04 mmol /（hm ²）。流通设计引入了更多的对流，从而提高了质量传递，进而加快了有机化合物的氧化动力学。此外，阳离子MB，阳离子罗丹明6G（R6G）和阴离子甲基橙（MO）的混合溶液的氧化仅产生MB和R6G的选择性氧化，其中MB和R6G的氧化通量分别是3.7和3.0倍，分别大于MO。特别是，与传统的批处理配置相比，流通系统的MB氧化效率高出20倍（95.8％对4.9％）。电子顺磁共振（EPR）技术和淬灭实验证实了¹ O ₂的重要作用。所提出的流通系统可以提供用于选择环境修复的高效，高效和快速的方法。

更新日期：2020-08-05

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