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電流密度對(duì)BDD電極電化學(xué)礦化吲哚的影響與機(jī)制

發(fā)布時(shí)間:2018-02-25 22:04

  本文關(guān)鍵詞: 摻硼金剛石膜電極 吲哚 礦化 氣體逸出 碳守恒 氮形態(tài) 出處:《環(huán)境科學(xué)》2017年09期  論文類型:期刊論文


【摘要】:摻硼金剛石膜(BDD)電極電化學(xué)氧化法是去除難降解有機(jī)污染物的有效手段.與總有機(jī)碳(TOC)等的測定相比,氣態(tài)中間產(chǎn)物的逸出量能夠更直觀有效地反映有機(jī)物的礦化程度與去除效果.本研究以吲哚為代表性污染物,通過對(duì)比不同電流密度(10、20和30 m A·cm-2)下BDD電極對(duì)吲哚的去除率與礦化率,結(jié)合降解過程中碳和氮形態(tài)的變化與守恒情況,分析吲哚的降解機(jī)制.結(jié)果表明,BDD電極對(duì)吲哚有良好的去除效果,電流密度為10、20、30 m A·cm-2時(shí),吲哚達(dá)到100%去除的時(shí)間分別為8、5和4 h;TOC去除率、CO_2產(chǎn)生量均隨電流密度的增加而增大,證明礦化率與電流密度成正相關(guān);電解產(chǎn)生的CO_2氣體與TOC、無機(jī)碳(TIC)構(gòu)成了碳守恒體系.4~5 h時(shí),體系TOC、TON和CO_2產(chǎn)生量均沒有變化,表明電解產(chǎn)生的靛紅具有較高的穩(wěn)定性,此時(shí)為中間產(chǎn)物積累階段;XPS表征進(jìn)一步證實(shí)了中間產(chǎn)物靛紅、苯醌等在電極表面的吸附,隨著電解時(shí)間的延長,這些吸附的中間產(chǎn)物可進(jìn)一步被降解.本研究從氣態(tài)產(chǎn)物檢測及碳氮形態(tài)分析與守恒的角度闡釋吲哚礦化過程,對(duì)于輔助揭示有機(jī)物的電解過程有重要意義.
[Abstract]:The electrochemical oxidation of boron doped diamond (BDD) electrode is an effective method to remove refractory organic pollutants, compared with the determination of total organic carbon (TOC), etc. The emission of gaseous intermediate products can reflect the mineralization degree and removal efficiency of organic compounds more directly and effectively. In this study, indole was used as the representative pollutant. By comparing the removal rate and mineralization rate of indole at BDD electrode at different current densities of 10 ~ (20) and 30 Ma 路cm ~ (-2), the change and conservation of carbon and nitrogen forms in the degradation process were combined. The degradation mechanism of indole was analyzed. The results showed that the removal efficiency of indole was good. When the current density was 10 ~ 20 ~ 30 Ma 路cm-2, the removal time of indole to 100% was 8 ~ 5 and 4 h respectively. The yield of indoles increased with the increase of current density. It is proved that the mineralization rate is positively correlated with the current density, and that the CO_2 gas produced by electrolysis has no change in the production of both TOCITon and CO_2, and that the CO_2 gas produced by electrolysis has a high stability with respect to the formation of the conserved carbon system for 5 h, and the amount of CO_2 produced by the system does not change, which indicates that the indirubin produced by electrolysis is of high stability. XPS characterization at this stage of intermediate product accumulation further confirmed the adsorption of indirubin and benzoquinone on the electrode surface with the prolongation of electrolysis time. These adsorbed intermediates can be further degraded. In this study, the indole-mineralization process was explained from the point of view of gaseous product detection, carbon and nitrogen speciation analysis and conservation, which is of great significance in assisting to reveal the electrolytic process of organic matter.
【作者單位】: 北京大學(xué)環(huán)境工程系水沙科學(xué)教育部重點(diǎn)實(shí)驗(yàn)室;
【基金】:國家重點(diǎn)研發(fā)計(jì)劃項(xiàng)目(2016YFC0402102)
【分類號(hào)】:X592

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