炭基材料催化過(guò)氧化物降解水中有機(jī)污染物:表面作用機(jī)制
發(fā)布時(shí)間:2018-04-09 05:29
本文選題:表面作用機(jī)制 切入點(diǎn):炭基材料 出處:《化學(xué)進(jìn)展》2017年05期
【摘要】:近幾年來(lái),利用傳統(tǒng)炭材料(如活性炭(AC)、生物炭(BC)、活性炭纖維(ACF)與活性炭布(ACC))以及納米碳材料(如碳納米管(CNT)、石墨烯(GE)、有序介孔碳(OMC)),或其表面改性后的炭基材料,代替金屬催化劑,來(lái)催化活化過(guò)氧化物(包括過(guò)氧化氫(H_2O_2)、過(guò)一硫酸氫鹽(HSO_5~-,PMS)、過(guò)二硫酸鹽(S_2O_8~(2-),PS))產(chǎn)生高活性羥基自由基(·OH)或硫酸根自由基(SO_4~(·-)),從而氧化去除水中難生物降解有機(jī)污染物,成為水處理領(lǐng)域研究熱點(diǎn)。在炭表面富含很多起催化作用的官能團(tuán),如羥基、羧基、酮基、吡啶、吡咯等,同時(shí)具有豐富多樣的缺陷形狀、離域π電子、雜化C軌道等,能共同協(xié)作表現(xiàn)出非金屬炭基催化劑的優(yōu)良特性。因此,不同類(lèi)型材料及其表面官能團(tuán)、表面結(jié)構(gòu)、電子密度等因素對(duì)炭基材料催化過(guò)氧化物的機(jī)理發(fā)揮顯著作用。本文深入分析了上述炭基材料在吸附、絡(luò)合中間體、電子轉(zhuǎn)移過(guò)程中催化過(guò)氧化物產(chǎn)生強(qiáng)氧化性的自由基,并高效降解水中有機(jī)污染物的作用機(jī)理,綜述了2010年以來(lái)該類(lèi)高級(jí)氧化技術(shù)在水處理領(lǐng)域的研究進(jìn)展,特別是通過(guò)總結(jié)炭基材料的氧化改性作用、氮化改性作用、多原子原位摻雜作用以及還原改性作用,系統(tǒng)闡述了表面物理化學(xué)性質(zhì)對(duì)炭基材料催化過(guò)氧化物的表面作用機(jī)制的影響,并歸納了氧化劑對(duì)炭基材料的表面作用機(jī)制,對(duì)存在的問(wèn)題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.
【作者單位】: 海洋環(huán)境與生態(tài)教育部重點(diǎn)實(shí)驗(yàn)室;山東省海洋環(huán)境地質(zhì)工程重點(diǎn)實(shí)驗(yàn)室;中國(guó)海洋大學(xué)環(huán)境科學(xué)與工程學(xué)院;
【基金】:國(guó)家自然科學(xué)基金項(xiàng)目(No.21107101,21677135)資助~~
【分類(lèi)號(hào)】:O643.32;X52
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