铁-多羧基有机酸光化学体系研究进展  

Research Progress on the Photochemistry System of the Fe-organic Acids with Multi-carboxyls: A Review

作　　者：兰青 莫家乐[1] 曹美苑 LAN Qing;MO Jiale;CAO Meiyuan(Environment Monitoring Department,Guangdong Polytechnic of Environmental Protection Engineering,Foshan 528216,China;Guangdong Engineering and Technology Research Center of Solid Waste Resource Recovery and Heavy Metal Pollution Control,Foshan 528216,China;School of Chemistry and Chemical Engineering,Sun Yat-sen University,Guangzhou 510275,China)

机构地区：[1]广东环境保护工程职业学院环境监测系,广东佛山528216 [2]广东省固体废弃物资源化与重金属污染控制工程技术研究中心,广东佛山528216 [3]中山大学化学与化学工程学院,广东广州510275

出　　处：《生态环境学报》2018年第10期1972-1980,共9页Ecology and Environmental Sciences

基　　金：国家自然科学基金项目(41201503);高等学校博士学科点专项科研基金资助课题(20110171120025);广东省高等职业教育品牌专业建设项目(室内环境检测与控制技术)(2016gzpp036);广东高校省级重点平台和重大科研项目(2017GKTSCX039)

摘　　要：铁-多羧基有机酸光化学体系在自然界中广泛存在,该体系可以由内源生成过氧化氢和羟基自由基,对研究有机污染物的归趋和治理具有重要意义。通过梳理近30年来有关该体系研究的代表性文献,从机理概述、均相体系研究进展、异相体系研究进展以及研究展望4个方面,系统总结了一些重要研究成果。从反应机理来看,吸附反应、光诱导反应、光链反应和有机物降解是该体系的重要反应过程,主要涉及配体和自由基的生成反应,以及铁的氧化还原循环反应。体系活性高低主要取决于多羧基有机酸铁配体的光化学活性大小。异相体系中,吸附态铁配体与溶解态铁配体共同参与光催化过程,对污染物的降解均有贡献。影响体系降解目标物的重要因素包括铁氧化物的种类和剂量、多羧基有机酸的种类和浓度、pH、光源波长和强度、氧气、金属离子、目标物的中间产物以及体系内活性物种的竞争反应等。其中,有机酸存在最佳浓度,铁氧化物存在最佳剂量,而有机酸最佳浓度与其在铁氧化物表面上的饱和吸附浓度密切相关。今后,基础研究方面需联合应用同位素示踪技术、穆斯堡尔谱、薄膜扩散梯度-荧光分析等先进实验技术,结合表面络合模型等才能取得重要突破;应用研究方面,构建适于实际工程运用的高效光化学反应器和废水处理集成工艺、重金属脱毒技术,扩展铁氧化物在土壤有机物降解及微生物燃料电池中的应用范围,是重要的扩展研究方向。Fe-carboxylic acids with multi-carboxyls are ubiquitous in nature and often lead to the formation of H2O2 and·OH,which can facilitate the removal of many organic pollutants and thus affect their environment fate.In the past 30 years,many advances on their reaction mechanisms,both in homogeneous and heterogeneous systems,have been made and are reviewed in this paper.The main reactions in the system of Fe-carboxylic acids include adsorption,light induced reactions,light chain reactions.The degradation of organic pollutants are achieved mainly through the formation of Fe-organic acid complexes and radicals,and the iron redox reactions,where the removal efficiency mainly depends on the photochemical activity of Fe-organic acid complexes.In heterogeneous system,the adsorbed complexes and the dissolved complexes involve the whole photocatalysis process and contribute to the degradation of pollutants.Many factors affect the degradation of pollutants,such as type and dose of iron oxides,speciation and concentration of carboxylic acids,pH,wavelength and intensity of light,oxygen,metal ion,intermediates and competing reactions among the active species.Optimal concentrations or doses have been observed for organic acids and iron oxides,where the optimal concentration of organic acids are often closely related to their saturated adsorption on the surface of iron oxides.Further research on the reaction mechanisms requires cutting edge experimental technologies such as isotopic tracing,Mossbauer Spectroscopy,DGT-PO technology,as well as surface complexation chemical modeling.Application researches in the area include constructions of high efficient photochemical reactors,integrated industrial treatment of wastewater,detoxification of heavy metals,and application of iron oxides in degradation of soil organic pollutants and in microbiological fuel cells.

关 键 词：光化学 铁 多羧基有机酸 污染物 

分 类 号：X13[环境科学与工程—环境科学]