反应性炭膜电催化净化水中氟喹诺酮类抗生素的构效和调控机制

This proposal is attempted to develop a SnO2-Bi doped carbon membrane filter anode, and applied to construct a novel Reactive Electrochemical Carbon Membrane Filter (RECMF), which could minimize the transfer limitation of the electrochemical reactor, and remove typical Fluroquinolones (FQs) by the synergetic effect of adsorption, filtration and electrochemical oxidation. This hybrid of technology is a new attempt to remove FQs fast with high efficiency. We attempt to prepare the carbon membrane from coal using MnCO3 as template to control pore structure and in-situ grow nano size bismuth-antimony oxidized layer on the surface of the carbon membrane, which is referred as SnO2/Bi - carbon membrane filter anode. The goal of this research is to investigate the change of electrochemical reactivity and anti-corrosion properties of the carbon membrane after growing SnO2/Bi layer; Besides, this research also aims to reveal the relationship between the anode pore structure (average pore size, porosity) and FQs mineralization efficiency in RECMF, so as to determine the optimal pore structure; Then the filter anode with optimal pore structure will be used to construct a RECMF system to remove FQs, the mechanism and kinetics of FQs degradation in RECMF system will be carefully studied to find out the key control factor of FQs degradation in RECMF; Finally, we will optimize the control factor in RECMF according to its energy efficiency in FQs degradation and evaluate its stability. The findings of this research will have important theoretical significance and application value for developing efficient RECMF with low cost for water purification.

本课题针对传统电化学体系的传质局限，提出以纳米SnO2-Bi改性的多孔炭膜作为过滤性阳极，构建新型反应性炭膜电催化过滤体系（RECMF）。以典型的氟喹诺酮类抗生素（FQs）为处理对象，通过耦合SnO2-Bi炭膜电极的吸附、过滤和电化学氧化作用实现对FQs高效、快速降解。主要研究内容：①分析制备工艺参数对SnO2-Bi炭膜电极电催化活性和耐腐蚀性等电化学性能的影响规律，优化制备方法；②构建RECMF体系，探明SnO2-Bi炭膜电极孔结构和FQs处理效率之间的构-效关系，为高性能的RECMF孔结构设计奠定基础；③研究RECMF体系吸附、过滤和电催化协同降解FQs的机理并建立反应动力学模型，识别关键控制因子，提出调控FQs处理效率的方法，并评价RECMF体系的稳定性。研究结果将为炭膜电催化过滤技术在水体净化领域的应用提供理论依据。

针对电化学氧化技术处理难降解有机废水工程应用面临的瓶颈，如电极性能不够完善，电极反应速率受污染物传质限制导致整体电流效率低下等问题，本项目以抗生素（环丙沙星）为研究对象，研制新型多孔炭膜电极的优化制备工艺，制备酸洗改性炭膜作为阳极用于构建电化学体系，通过在电化学体系中引入过硫酸盐，构建炭膜阳极-过硫酸盐电化学体系，利用强化传质和发挥阴阳极协同作用提高体系的氧化性能，实现了抗生素废水的高效净化。发展了基于锡铋（SnO2-Bi）的钛基电极的可控制备方法，利用铁改性炭膜作为阴极，通过引入过硫酸盐，构建炭膜阴极-过硫酸盐电化学体系，强化阴阳极耦合作用，研究环丙沙星在该体系中的电化学氧化降解行为、效能和体系的稳定性。优化关键影响因子，阐明降解机理和降解路径，并探索应用于实际医院污水处理的适应性，为电化学高级氧化技术在医院污水治理中的应用提供理论依据。