【摘要】：納米零價(jià)鐵具有較大的比表面積和較強(qiáng)的反應(yīng)活性,能夠有效地去除環(huán)境中的有機(jī)污染物,是目前最具有應(yīng)用潛力的高效還原劑之一;但由于其在處理污染物時(shí)表現(xiàn)出易團(tuán)聚的缺陷,限制了其工程應(yīng)用。為了克服此缺陷,本研究以生物炭為載體,使用液相還原法制備生物炭負(fù)載納米零價(jià)鐵材料,并使用制備的生物炭負(fù)載納米零價(jià)鐵材料對(duì)甲基橙、三氯乙烯以及1,2,4-三氯苯進(jìn)行降解研究。最后,為了拓寬材料的應(yīng)用范圍,使用生物炭負(fù)載納米零價(jià)鐵活化過(guò)硫酸鹽,并研究了其對(duì)三氯乙烯的去除效果。主要研究?jī)?nèi)容與結(jié)果如下:(1)利用液相還原沉積法制備了生物炭負(fù)載納米零價(jià)鐵材料。材料的表征結(jié)果表明,生物炭的微觀形態(tài)呈片狀形態(tài),且生物炭上出現(xiàn)的羥基、羧基、羰基等電負(fù)性官能團(tuán)有利于納米零價(jià)鐵的負(fù)載;納米零價(jià)鐵顆粒的粒徑主要分布在30-70 nm之間,且在負(fù)載前后,納米零價(jià)鐵的表面積由20.9 m2/g升高至126.6~138.1 m2/g。(2)使用生物炭負(fù)載納米零價(jià)鐵材料對(duì)甲基橙進(jìn)行去除研究,結(jié)果表明,將納米零價(jià)鐵負(fù)載于生物炭上明顯增加了甲基橙的去除效果,生物炭負(fù)載納米零價(jià)鐵對(duì)甲基橙的去除率均為93.26%以上,其中炭鐵質(zhì)量比為5:1的生物炭負(fù)載納米零價(jià)鐵對(duì)甲基橙的去除效果最好,達(dá)到98.51%。(3)污染物的初始濃度、反應(yīng)溶液中生物炭負(fù)載納米零價(jià)鐵的投加量、反應(yīng)初始pH以及共存陰離子等條件都會(huì)對(duì)降解反應(yīng)的速率產(chǎn)生影響:隨著反應(yīng)初始濃度的升高,生物炭負(fù)載納米零價(jià)鐵材料對(duì)甲基橙的去除率及反應(yīng)速率降低;增加生物炭負(fù)載納米零價(jià)鐵的投加量能夠有效加快反應(yīng)的速率;溶液中pH值的升高不利于反應(yīng)的進(jìn)行;向溶液中添加諸如氯離子、硫酸根離子及硝酸根離子等陰離子時(shí),這些陰離子與污染物在納米零價(jià)鐵表面的活性位點(diǎn)上產(chǎn)生競(jìng)爭(zhēng)吸附。同時(shí)也會(huì)減少溶液中氫離子的數(shù)量,因此,溶液中的共存陰離子會(huì)對(duì)反應(yīng)的速率和降解的效果產(chǎn)生影響。(4)在自然條件下放置一個(gè)月后的生物炭負(fù)載納米零價(jià)鐵仍能夠?qū)谆扔辛己玫娜コЧ?比新鮮制備的生物炭負(fù)載納米零價(jià)鐵對(duì)甲基橙的去除率低3%),說(shuō)明生物炭能夠延緩納米零價(jià)鐵在自然條件下的氧化過(guò)程,有利于材料的工程應(yīng)用。(5)使用生物炭負(fù)載納米零價(jià)鐵能夠有效降解三氯乙烯和1,2,4-三氯苯。降解反應(yīng)完成后使用正己烷對(duì)吸附劑進(jìn)行脫附處理,結(jié)果表明,反應(yīng)溶液中三氯乙烯和1,2,4-三氯苯濃度的降低主要是由于納米零價(jià)鐵的還原作用引起的。(6)為了拓寬生物炭負(fù)載納米零價(jià)鐵材料的應(yīng)用范圍,使用生物炭負(fù)載納米零價(jià)鐵活化過(guò)硫酸鹽并研究其對(duì)三氯乙烯的降解,結(jié)果表明,該反應(yīng)體系對(duì)三氯乙烯的降解反應(yīng)過(guò)程在1 min左右基本達(dá)到平衡,使用炭鐵質(zhì)量比為5:1的生物炭負(fù)載納米零價(jià)鐵材料活化過(guò)硫酸鹽對(duì)三氯乙烯的降解率最高,可以達(dá)到99.4%。
[Abstract]:Nanocrystalline zero-valent iron has a large specific surface area and strong reactive activity, which can effectively remove organic pollutants in the environment, so it is one of the most potential high-efficiency reductants. However, its engineering application is limited because of its easy agglomeration defect in the treatment of pollutants. In order to overcome this defect, the liquid phase reduction method was used to prepare biochar supported nanocrystalline zero-valent iron materials, and the biological carbon supported nano-zero-valent iron materials for methyl orange were used in this study. The degradation of trichloroethylene (trichloroethylene) and trichlorobenzene (4-trichlorobenzene) was studied. Finally, in order to widen the scope of application of the material, the activated persulfate was activated with nano-ferric oxide loaded with biological carbon, and the removal effect of trichloroethylene was studied. The main contents and results are as follows: (1) Nano-sized zero-valent iron materials supported by biological carbon were prepared by liquid phase reduction deposition. The characterization results showed that the micromorphology of biochar was flake, and the electronegativity groups such as hydroxyl, carboxyl and carbonyl on the biochar were favorable to the loading of nano-zero-valent iron. The particle size of nanocrystalline zero-valent iron particles is mainly between 30-70 nm, and the surface area of nano-zero-valent iron increases from 20.9 m2 / g to 126.6n 138.1 m2 / g before and after loading. (2) the removal of methyl orange by biochar supported nano-zero-valent iron nanoparticles is studied. The removal efficiency of methyl orange was obviously increased by loading nano-zero valent iron onto biochar, and the removal efficiency of methyl orange was more than 93.26%. Among them, the removal efficiency of methyl orange was the best when the mass ratio of carbon to iron was 5:1, which reached 98.51. (3) the initial concentration of pollutants and the amount of nano-zero-valent iron loaded by biological carbon in the reaction solution. The initial pH of the reaction and the coexistence of anions will affect the degradation rate: with the increase of the initial concentration of the reaction, the removal rate and the reaction rate of methyl orange are decreased with the increase of the initial concentration of biochar supported nanocrystalline iron. Increasing the amount of nano-zero-valent iron loaded with biological carbon can effectively accelerate the reaction rate; the increase of pH value in the solution is not conducive to the reaction; when the anions such as chloride ion, sulfate ion and nitrate ion are added to the solution, These anions and pollutants are competitively adsorbed on the active sites on the surface of nanocrystalline zero-valent iron. It also reduces the amount of hydrogen ions in the solution. The coexistence of anions in the solution will affect the reaction rate and the degradation effect. (4) after a month's storage under natural conditions, the nano-zero-valent iron supported by biological carbon can still have a good removal effect on methyl orange (compared with fresh preparation). The removal rate of methyl orange is 3% lower than that of the prepared biochar loaded with nanometer zero-valent iron, which indicates that biochar can delay the oxidation process of nano-zero-valent iron under natural conditions. It is beneficial to the engineering application of the materials. (5) trichloroethylene and 1-trichlorobenzene can be effectively degraded by using biochar supported nano-zero-valent iron. The adsorbent was desorbed with n-hexane after the degradation reaction was completed. The decrease in the concentration of trichloroethylene and 1-trichlorobenzene in the reaction solution is mainly caused by the reduction of nanometer zero-valent iron. (6) in order to widen the application range of nano-zero valent iron loaded with biological carbon, Activated persulfate with nano-zero-valent iron supported by biochar and studied its degradation of trichloroethylene. The results showed that the degradation process of trichloroethylene was basically balanced at about 1 min. The degradation rate of trichloroethylene by activated persulfate was the highest when the mass ratio of carbon to iron was 5:1, and the degradation rate of trichloroethylene was 99.4%.
【學(xué)位授予單位】：蘇州科技學(xué)院
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2015
【分類號(hào)】：X505

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