Enhanced degradation of tetracycline by gas-liquid discharge plasma coupled with g-C3N4/TiO2

Zhenhai Wang, Zikai Zhou, Sen Wang, Zhi Fang
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Abstract

Plasma-catalysis is considered as one of the most promising technologies for antibiotic degradation in water. In the plasma-catalytic system, one of the factors affecting the degradation effect is the performance of the photocatalyst, which is usually restricted by the rapid recombination of electrons and holes as well as narrow light absorption range. In this research, a photocatalyst g-C3N4/TiO2 was prepared and coupled with gas-liquid discharge (GLD) to degrade tetracycline (TC). The performance was examined, and the degradation pathways and mechanisms were studied. Results show that a 90% degradation rate is achieved in the GLD with g-C3N4/TiO2 over a 10 min treatment. Increasing the pulse voltage is conducive to increasing the degradation rate, whereas the addition of excessive g-C3N4/TiO2 tends to precipitate agglomerates, resulting in a poor degradation efficiency. The redox properties of the g-C3N4/TiO2 surface promote the generation of oxidizing active species (H2O2, O3) in solution. Radical quenching experiments showed that ·OH, hole (h+), play important roles in the TC degradation by the discharge with g-C3N4/TiO2. Two potential degradation pathways were proposed based on the intermediates. The toxicity of tetracycline was reduced by treatment in the system. Furthermore, the g-C3N4/TiO2 composites exhibited excellent recoverability and stability. Keywords: Gas-liquid discharge; Plasma-catalysis; g-C3N4/TiO2; TC degradation
气液放电等离子体与 g-C3N4/TiO2 相结合增强四环素的降解能力
等离子催化被认为是最有前途的水中抗生素降解技术之一。在等离子催化系统中,影响降解效果的因素之一是光催化剂的性能,而光催化剂的性能通常受到电子和空穴快速重组以及光吸收范围狭窄的限制。本研究制备了一种光催化剂 g-C3N4/TiO2,并将其与气液放电(GLD)耦合用于降解四环素(TC)。该研究考察了其性能,并研究了降解途径和机制。结果表明,使用 g-C3N4/TiO2 的 GLD 在 10 分钟的处理时间内实现了 90% 的降解率。增加脉冲电压有利于提高降解率,而过量添加 g-C3N4/TiO2 则容易析出团聚体,导致降解效率低下。g-C3N4/TiO2 表面的氧化还原特性促进了溶液中氧化活性物种(H2O2、O3)的生成。自由基淬灭实验表明,-OH、空穴(h+)在 g-C3N4/TiO2 放电降解 TC 的过程中发挥了重要作用。根据中间产物提出了两种潜在的降解途径。在该系统中处理四环素可降低其毒性。此外,g-C3N4/TiO2复合材料还表现出优异的可回收性和稳定性。关键词气液放电;等离子催化;g-CN4/TiO2;四环素降解
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