炭基材料催化过氧化物降解水中有机污染物:表面作用机制

发布时间：2018-04-09 05:29

本文选题：表面作用机制　切入点：炭基材料　出处：《化学进展》2017年05期

【摘要】：近几年来,利用传统炭材料(如活性炭(AC)、生物炭(BC)、活性炭纤维(ACF)与活性炭布(ACC))以及纳米碳材料(如碳纳米管(CNT)、石墨烯(GE)、有序介孔碳(OMC)),或其表面改性后的炭基材料,代替金属催化剂,来催化活化过氧化物(包括过氧化氢(H_2O_2)、过一硫酸氢盐(HSO_5~-,PMS)、过二硫酸盐(S_2O_8~(2-),PS))产生高活性羟基自由基(·OH)或硫酸根自由基(SO_4~(·-)),从而氧化去除水中难生物降解有机污染物,成为水处理领域研究热点。在炭表面富含很多起催化作用的官能团,如羟基、羧基、酮基、吡啶、吡咯等,同时具有丰富多样的缺陷形状、离域π电子、杂化C轨道等,能共同协作表现出非金属炭基催化剂的优良特性。因此,不同类型材料及其表面官能团、表面结构、电子密度等因素对炭基材料催化过氧化物的机理发挥显著作用。本文深入分析了上述炭基材料在吸附、络合中间体、电子转移过程中催化过氧化物产生强氧化性的自由基,并高效降解水中有机污染物的作用机理,综述了2010年以来该类高级氧化技术在水处理领域的研究进展,特别是通过总结炭基材料的氧化改性作用、氮化改性作用、多原子原位掺杂作用以及还原改性作用,系统阐述了表面物理化学性质对炭基材料催化过氧化物的表面作用机制的影响,并归纳了氧化剂对炭基材料的表面作用机制,对存在的问题提出了新的研究展望。
[Abstract]:In recent years, conventional carbon materials (such as activated carbon (AAC), biochar (BCC), activated carbon fiber (ACFC) and activated carbon cloth (ACC)), as well as nano-carbon materials (such as carbon nanotubes (CNT), graphene gels, ordered mesoporous carbon (OMC), or their surface modified carbon-based materials) have been used in recent years.Instead of metal catalysts, to catalyze the activation of peroxides (including hydrogen peroxide / H _ 2O _ 2H _ 2O _ 2H _ 2O _ 2H _ 2SO _ 4 / S _ so _ 5- / PMSS, P / S _ 2O _ 2O _ 8 / S _ 2O _ 8 / S _ 2O _ 2-PSN) to produce highly active hydroxyl radicals (OHs) or sulphate radical radical (-SO _ 4), thereby oxidizing and removing non-biodegradable organic pollutants in the water,It has become a research hotspot in the field of water treatment.The carbon surface is rich in many catalytic functional groups, such as hydroxyl group, carboxyl group, ketone group, pyridine, pyrrole, etc.The excellent properties of non-metallic carbon-based catalysts can be demonstrated by co-operation.Therefore, different types of materials and their surface functional groups, surface structure, electron density and other factors play a significant role in the catalytic mechanism of peroxide.In this paper, the mechanism of catalytic production of strongly oxidized free radicals by peroxides in adsorption, complexation intermediates and electron transfer of carbon based materials is analyzed, and the mechanism of degradation of organic pollutants in water is also discussed.The research progress of this advanced oxidation technology in the field of water treatment since 2010 was reviewed, especially by summarizing the oxidation modification, nitridation modification, polyatomic in-situ doping and reduction modification of carbon based materials.The effects of surface physicochemical properties on the surface action mechanism of peroxide catalyzed by carbon based materials are systematically expounded, and the surface action mechanisms of oxidants on carbon based materials are summarized, and new research prospects for the existing problems are put forward.
【作者单位】：海洋环境与生态教育部重点实验室;山东省海洋环境地质工程重点实验室;中国海洋大学环境科学与工程学院;
【基金】：国家自然科学基金项目(No.21107101,21677135)资助~~
【分类号】：O643.32;X52

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