本文關(guān)鍵詞：工業(yè)粉煤灰制備硅材料及其吸附水中六價鉻的研究　出處：《昆明理工大學(xué)》2015年碩士論文　論文類型：學(xué)位論文

  更多相關(guān)文章： 粉煤灰 硅材料 六價鉻 吸附機(jī)理

【摘要】：六價鉻(Cr(Ⅵ))是高度毒性的重金屬污染物,具有致畸、致癌和致突變作用,是美國EPA列為水體一級優(yōu)先控制污染物,也是我國列為"十二五"規(guī)劃中的重點防控的重金屬污染物。我國是有色金屬生產(chǎn)第一大國,工業(yè)生產(chǎn)過程中排放大量的含Cr(Ⅵ)廢水廢渣,水體的鉻污染嚴(yán)重影響居民飲用水安全和工業(yè)生產(chǎn)用水,加之我國面臨嚴(yán)重的水資源短缺問題,水體Cr(Ⅵ)污染的防治是工業(yè)廢水治理的重中之重。吸附法處理重金屬廢水效果明顯,操作簡便,原料來源廣泛且可循環(huán)利用,因而廣泛運用于處理Cr(Ⅵ)廢水。吸附法的技術(shù)關(guān)鍵在于吸附劑的選擇。本課題采用不同硅源、不同模板劑、不同的老化和改性方法制備了硅材料SBA-15和MCM-41,并將其作為吸附劑,通過靜態(tài)實驗吸附水中的Cr(Ⅵ),通過比較吸附效果篩選出最優(yōu)吸附劑。實驗結(jié)果發(fā)現(xiàn),以工業(yè)粉煤灰為硅源、十六烷基三甲基溴化銨(CTAB)為模板劑,通過堿熔融-微波老化合成法制備的硅材料MCM-41(命名為FMC)對Cr(Ⅵ)的吸附效果最佳。對粉煤灰制備的介孔硅材料MCM-41進(jìn)行XRD和N2吸附-脫附表征,表征結(jié)果說明該材料具有介孔結(jié)構(gòu)的特征,但有序度差,比表面積小,原因是粉煤灰中雜質(zhì)較多,在制備過程中影響了材料的孔隙形成和分布�？疾旌Y選出的最優(yōu)吸附劑FMC對Cr(Ⅵ)的吸附性能,考察內(nèi)容包括溶液初始pH值、吸附時間、初始Cr(Ⅵ)濃度、共存陰陽離子、光照和吸附溫度等因素;在此基礎(chǔ)上,對吸附劑FMC進(jìn)行了吸附動力學(xué)和吸附熱力學(xué)研究,同時對FMC進(jìn)行吸附-解吸的再生研究。此外,采用XRD、N2吸附-脫附和FT-IR對硅材料FMC進(jìn)行表征。實驗結(jié)果表明,FMC對水中Cr(Ⅵ)具有顯著的吸附作用,酸性條件利于吸附,最佳pH=1.5～2.5;共存陰、陽離子對其吸附效果幾乎無影響,FMC對Cr(Ⅵ)具有很高的選擇性;提高吸附溫度利于FMC吸附Cr(Ⅵ),但溫度的影響很不明顯;光照條件大大提高了 FMC的吸附效果。FMC吸附Cr(Ⅵ)的過程符合Langmuir等溫模型,光照條件下的最大擬合吸附容量為256.41 mg/g,無光照條件下最大擬合吸附容量為153.85 mg/g,吸附為吸熱過程,并遵循準(zhǔn)二級動力學(xué)模型。通過吸附性能的研究及XRD、N2吸附-脫附和FT-IR表征分析,得出FMC吸附水中Cr(Ⅵ)的吸附機(jī)理為:Cr(Ⅵ)陰離子為主要吸附對象,硅材料FMC外表面的正電荷硅物種和其內(nèi)表面的銨根離子(N[CH3(CH2)15](CH3)3+)為吸附位點,吸附過程主要在酸性條件下進(jìn)行;在酸性條件下,FMC表面的正電荷硅物種與內(nèi)表面的銨根離子通過靜電作用吸附Cr(Ⅵ)陰離子,最終以N-H鍵進(jìn)行鍵合;隨著pH值的升高,FMC表面的硅物種逐漸帶負(fù)電荷,其與Cr(Ⅵ)陰離子的靜電吸附作用減弱、甚至消失,由于溶液中大量OH-的競爭作用,FMC內(nèi)表面的吸附位點對Cr(Ⅵ)陰離子的吸附作用減小,兩方面原因?qū)е翪r(Ⅵ)去除率隨pH值的升高而下降。脫附為吸附的逆過程,使用堿液對FMC進(jìn)行脫附解吸。在堿性解吸液中,FMC表面帶有大量的負(fù)電荷,并排斥吸附在吸附劑上的Cr(Ⅵ)陰離子而釋放到液相中。本課題制備的硅材料FMC吸附Cr(Ⅵ)的效果顯著,且制備成本低,原料來源廣泛,制備過程簡單快速,在Cr(Ⅵ)廢水處理方面有很大的應(yīng)用前景和現(xiàn)實意義。
[Abstract]:Six hexavalent chromium (Cr (VI)) is a highly toxic heavy metal pollutants, teratogenicity, carcinogenicity and mutagenicity, EPA of the United States listed as water level priority pollutants, heavy metal pollutants in China is listed as the focus of prevention and control planning in 12th Five-Year ". China is a non-ferrous metal production country, industry in the production process emissions of Cr (VI) containing a large amount of waste water, chromium pollution seriously affected the safety of drinking water and industrial water production, and China is facing a severe water shortage, water pollution prevention and control of Cr (VI) is the priority among priorities of industrial wastewater treatment. The adsorption treatment of heavy metal wastewater obviously, simple operation, wide source of raw materials and can be recycled, so it is widely used in treatment of Cr (VI) wastewater. Key technologies of adsorption is the selection of the adsorbent. The different silicon source, different templates, different aging Silicon SBA-15 and MCM-41 preparation and modification methods of preparation, and as adsorbent, the adsorption of Cr by the static experiment (VI), by comparing the adsorption effect of selected optimal adsorbent. The experimental results showed that the industrial fly ash as silicon source, sixteen alkyl three methyl bromide (CTAB) as the template by alkali melt microwave aging silicon material prepared by MCM-41 (named FMC) of Cr (VI) the best adsorption effect. The mesoporous silica MCM-41 prepared by fly ash were XRD and N2 adsorptiondesorption, the results show that the material has the characteristics of mesoporous structure. But the order of the poor, small specific surface area, the reason is a lot of impurities in fly ash, in the process of preparation and distribution of materials affect the pore formation. The optimal study screened FMC adsorbent on Adsorption Properties of Cr (VI), examining the contents including the initial pH value of solution, adsorption time, initial Cr (VI). Of co existing ions, adsorption temperature and light factors; on this basis, the adsorbent FMC for the adsorption kinetics and Adsorption Thermodynamics Study on adsorption desorption and regeneration of FMC. In addition, by XRD, N2 adsorption desorption and FT-IR on silicon FMC by XRD. The experimental results show that the FMC, Cr in water (VI) has significant adsorption, adsorption to acidic conditions, the best pH=1.5 ~ 2.5; the coexistence of Yin, cation has little effect on the adsorption effect of FMC, Cr (VI) has high selectivity; improve the adsorption temperature on FMC adsorption of Cr (VI), but the effect of temperature it is not obvious; the light conditions can greatly improve the adsorption effect of.FMC adsorption Cr FMC (VI) process accords with Langmuir isothermal model, light conditions the maximum fitting adsorption capacity is 256.41 mg/g, the maximum fitting without illumination conditions, adsorption capacity is 153.85 mg/g, adsorption absorption The thermal process, and follow the two level dynamic model. And through the study of the adsorption of XRD, N2 adsorption desorption and FT-IR analysis, the FMC adsorption of Cr (VI) adsorption mechanism: Cr (VI) anion adsorption as the main object, the positive charge of silicon silicon material on the outer surface of FMC species and the the surface of the ammonium ion (N[CH3 (CH2) 15] (CH3) 3+) for the adsorption sites, the adsorption process is mainly carried out in acidic condition; under acidic conditions, ammonium ions on the surface of FMC positively charged silicon species and the inner surface by electrostatic adsorption of Cr (VI) anion, N-H in the final key key; with the increase of pH value of silica species on the surface of FMC has negative charge, and the Cr (VI) electrostatic adsorption of anions weaken or even disappear, because of the competition effect of a large number of OH- solution, FMC adsorption sites on the surface of the Cr (VI) reduce the adsorption of anion, for two reasons Guide Cr (VI) removal rate decreases with the increase of pH value decreased. As the inverse process of adsorption desorption, using alkali desorption and desorption of FMC in alkaline solution. In desorption, the surface of FMC with a large amount of negative charge and rejection adsorbed onto the adsorbent of Cr (VI) anion released to the liquid phase the adsorption of Cr FMC. The silicon material prepared in this project (VI) a significant effect, and low preparation cost, wide sources of raw materials, the preparation process is simple and rapid in Cr (VI) has great application prospect and practical significance of wastewater treatment.

【學(xué)位授予單位】：昆明理工大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2015
【分類號】：TQ424;X703

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