納米零價(jià)鐵芬頓體系降解三氯乙烯實(shí)驗(yàn)研究
本文選題:納米零價(jià)鐵 + 殼-核結(jié)構(gòu) ; 參考:《中國地質(zhì)大學(xué)(北京)》2015年碩士論文
【摘要】:隨著經(jīng)濟(jì)的快速發(fā)展和人口的急劇增長,人類生活和生產(chǎn)過程中對地下水資源的需求量也不斷增長。與此同時(shí),在地下水的大量開發(fā)和利用過程中不可避免會(huì)遇到污染問題,其中三氯乙烯作為典型氯代有機(jī)污染受到人們的特別關(guān)注。近年來,研究者發(fā)現(xiàn)納米零價(jià)鐵可以應(yīng)用于原位環(huán)境修復(fù),由于納米零價(jià)鐵較大的比表面積和較高的反應(yīng)活性,相比于傳統(tǒng)的零價(jià)鐵顆粒,納米顆粒表現(xiàn)出更高的降解速率和更少的反應(yīng)副產(chǎn)物。納米零價(jià)鐵顆粒在接觸空氣、水后會(huì)快速形成鐵氧化物、鐵氫氧化物的外殼,這種天然的殼-核結(jié)構(gòu)在一定程度上降低了納米零價(jià)鐵的活性,但是其外殼可以提供Fenton氧化法所需要的二價(jià)鐵和三價(jià)鐵來源,因此殼-核結(jié)構(gòu)的納米零價(jià)鐵作為Fenton體系的多相催化劑進(jìn)行原位環(huán)境修復(fù)具有一定的潛力。本論文使用殼-核結(jié)構(gòu)納米零價(jià)鐵作為Fenton體系的催化劑,在中酸性條件下,進(jìn)行高濃度三氯乙烯降解實(shí)驗(yàn),同時(shí)選擇苯甲酸作為化學(xué)探針捕獲Fenton體系產(chǎn)生的羥基自由基,通過XRD、TEM、XPS等表征手段,考慮到初始p H值對Fenton體系的影響,對比納米磁鐵礦的Fenton體系,探討殼-核結(jié)構(gòu)納米零價(jià)鐵的Fenton體系氧化降解TCE的反應(yīng)機(jī)理,為納米零價(jià)鐵的Fenton體系應(yīng)用于原位環(huán)境修復(fù)的場地試驗(yàn)以及實(shí)際污染修復(fù)提供了重要的理論基礎(chǔ)和實(shí)際應(yīng)用參考。本論文主要研究成果如下:(1)在中酸性條件下,殼-核結(jié)構(gòu)納米零價(jià)鐵的Fenton體系可以對高濃度TCE進(jìn)行高效、完全的氧化降解。(2)以苯甲酸作為化學(xué)探針,發(fā)現(xiàn)殼-核結(jié)構(gòu)納米零價(jià)鐵的Fenton體系主要以產(chǎn)生強(qiáng)氧化性的羥基自由基對TCE進(jìn)行氧化降解。(3)初始p H條件影響Fenton體系的氧化能力,酸性p H條件強(qiáng)于中性p H條件,且殼-核結(jié)構(gòu)納米零價(jià)鐵有利用擴(kuò)展Fenton體系的p H值適用范圍。(4)殼-核結(jié)構(gòu)納米零價(jià)鐵在Fenton體系中主要作為固體催化劑進(jìn)行多相催化反應(yīng),外殼Fe3O4提供Fenton催化反應(yīng)必需的Fe2+和Fe3+來源,內(nèi)核Fe0提供電子加速Fenton鏈?zhǔn)酱呋磻?yīng)的循環(huán)。相比于納米磁鐵礦,殼-核結(jié)構(gòu)納米零價(jià)鐵的Fenton體系更適用于原位環(huán)境修復(fù)。
[Abstract]:With the rapid development of economy and the rapid growth of population, the demand for groundwater resources in human life and production process is also increasing. At the same time, pollution problems will inevitably be encountered in the development and utilization of groundwater, especially trichloroethylene as a typical chlorinated organic pollution. In recent years, researchers have found that nanocrystalline zero-valent iron can be used for in-situ environmental remediation. Due to its larger specific surface area and higher reactive activity, nano-zero-valent iron particles are more efficient than traditional zero-valent iron particles. Nanoparticles exhibit higher degradation rates and less byproducts. Nanocrystalline zero-valent iron particles will quickly form iron oxides, ferric hydroxide shells after contact with air, and this natural shell-core structure reduces the activity of nanoscale zero-valent iron to a certain extent. However, the shell can provide the bivalent and trivalent iron sources for the Fenton oxidation process. Therefore, the nano-zero-valent iron with shell-core structure can be used as a heterogeneous catalyst for the Fenton system for in situ environmental remediation. In this paper, the chi-core nanosized zero-valent iron was used as the catalyst for the Fenton system. The degradation of trichloroethylene was carried out under the medium acid condition. Benzoic acid was used as the chemical probe to capture the hydroxyl radical produced by the Fenton system. Considering the effect of initial pH value on Fenton system, compared with the Fenton system of nano-magnetite, the mechanism of oxidative degradation of TCE by Fenton system with shell core structure nano-zero valence iron was discussed. It provides an important theoretical basis and practical reference for the application of nano-zero-valent iron Fenton system in site tests of in-situ environmental remediation and the actual remediation of pollution. The main results of this paper are as follows: (1) in the presence of intermediate-acid conditions, the high concentration of TCE can be effectively degraded by Fenton system with zero-valence iron nanostructure, and benzoic acid is used as a chemical probe. It was found that the oxidation ability of TCE was affected by the initial pH condition of the Fenton system, which produced strongly oxidized hydroxyl radicals. The acidic pH condition was stronger than the neutral pH condition. In addition, nanocrystalline zero-valent iron with shell / core structure is mainly used as a solid catalyst for heterogeneous catalytic reaction in Fenton system by extending the pH value of Fenton system. The shell Fe3O4 provides the necessary Fe2 and Fe3 sources for the Fenton catalytic reaction, and the kernel Fe0 provides the electron accelerated Fenton chain reaction cycle. Compared with nanomagnetite, the Fenton system is more suitable for in situ environmental remediation.
【學(xué)位授予單位】:中國地質(zhì)大學(xué)(北京)
【學(xué)位級(jí)別】:碩士
【學(xué)位授予年份】:2015
【分類號(hào)】:X523
【共引文獻(xiàn)】
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