高级氧化体系中活性氧化物质的定性和半定量分析方法研究进展
Advances in Qualitative and Semi-quantitative Analysis of Reactive Oxygen Species in Advanced Oxidation Processes
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摘要: 由于人为活动和环境因素的影响,有机污染物迁移进入水、土壤和大气生态环境,进而危害粮食安全和人体健康,阻碍社会可持续发展. 高级氧化技术作为一类降解有机污染的重要手段,可以通过产生羟基自由基、硫酸根自由基、超氧自由基、单线态氧、高价态金属氧化物和表面活性中间体等具有不同氧化活性和反应特性的活性氧化物质(ROS)分解或转化各类有机污染物. 因此,对高级氧化反应体系中ROS的类型、贡献占比和反应途径的定性与半定量分析对于探究有机污染物的降解过程与具体机制至关重要. 基于文献调研,该文总结了高级氧化体系中多种ROS的氧化还原电位、反应机制等主要特点,综述了ROS的定性和半定量分析方法,包括电子顺磁性共振技术、ROS选择性淬灭方法、化学探针法、电化学法、原位拉曼法、穆斯堡尔光谱法、同步辐射法和定量构效关系分析法,分析了其优缺点和应用场景. 同时,对未来ROS的定性和半定量分析方法可能的发展趋势进行了思考,为今后更加科学合理地开展有机污染降解机理探究和应用技术开发工作提供基础.Abstract: Due to the influence of anthropogenic activities and environmental conditions, organic contaminants can migrate into water, soil and atmospheric ecological environment, which endanger food security and human health, and hinder the sustainable development of society. As a kind of crucial technique for degrading organic pollutants, advanced oxidation technologies can decompose or transform organic contaminants by producing reactive oxygen species (ROS) with different oxidation activities and reaction characteristics, such as hydroxyl radical, sulfate radical, superoxide radical, singlet oxygen, high-valent metal species as well as surface active intermediates. The qualitative and semi-quantitative analysis of the type, contribution and reaction pathway of ROS is crucial to explore mechanism of contaminant degradation. Based on previous literatures, this study summarized the main characteristics of ROS (redox potentials and reaction mechanisms) and reviewed the qualitative and semi-quantitative analysis methods of ROS, including electron paramagnetic resonance, quenching, chemical probe, electrochemical method, in situ Raman, Mossbauer spectroscopy, synchrotron radiation and quantitative structure-activity relationship analysis method. Their advantages, shortcoming and application scenarios were discussed. For providing a basis for more scientific and reasonable exploration of organic degradation mechanism and the exploitation of technology application exploitation, the possible development trend of qualitative and semi-quantitative analysis methods for ROS in the future was also proposed.
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