本文選題：染料廢水 + 吸附��； 參考：《安徽工業(yè)大學(xué)》2017年碩士論文

【摘要】：吸附法由于操作簡單,能在溫和條件下選擇性脫除廢水中的染料分子,其在染料廢水治理中得到廣泛應(yīng)用。吸附劑是吸附技術(shù)的核心。本文以石油瀝青為碳源、氧化鋅為模板,KOH為活化劑,采用常規(guī)加熱法制備分級多孔炭,并考察了其對亞甲基藍(lán)、直接黑38染料的吸附性能。為了拓展其應(yīng)用領(lǐng)域,對其表面進(jìn)行了負(fù)載金屬離子改性。為了提高多孔炭對酸性染料的吸附性能,對煤瀝青基多孔炭表面進(jìn)行嫁接聚酰胺胺(PAMAM)樹狀大分子改性,并研究其對酸性橙74、剛果紅染料的吸附性能。通過氮氣吸脫附、TEM、FESEM、XRD、XPS對分級多孔炭的物理結(jié)構(gòu)和表面化學(xué)性質(zhì)進(jìn)行了表征,其主要結(jié)果如下:(1)以石油瀝青為碳源,氧化鋅為模板耦合KOH活化,制備出分級多孔炭(PCs)。結(jié)果表明;所制備的分級多孔炭具有相互連接的薄片狀結(jié)構(gòu),且含有豐富的微孔和中孔。當(dāng)石油瀝青、氧化鋅和KOH的質(zhì)量分別為2,19和6 g,活化終溫為850℃,制得的PC_(2-19-850)的比表面積高達(dá)1913 m2/g。對染料的吸附性能研究表明,由于存在大量的超級微孔,分級多孔炭對分子尺寸較小的亞甲基藍(lán)表現(xiàn)出優(yōu)異的吸附性能;同時分級多孔炭存在一定量的中孔,其對分子尺寸較大的直接黑38也具有一定的吸附性能。PC_(2-19-850)對亞甲基藍(lán)染料的吸附等溫線可以用Langmuir模型描述,最大吸附量可達(dá)887 mg/g,對直接黑38染料的吸附等溫線可以用Freundlich模型來描述。動力學(xué)研究表明,擬二級動力學(xué)模型可以較好地描述多孔炭對亞甲基藍(lán)的吸附行為,而擬一級動力學(xué)模型則可以描述多孔炭對直接黑38染料的吸附行為。(2)以PC_(2-19-850)為初始炭,對其表面負(fù)載金屬離子,制備出改性多孔炭Zn(II)/PC和Fe(III)/PC。結(jié)果表明;經(jīng)負(fù)載改性后的Zn(II)/PC和Fe(III)/PC依然含有微孔和中孔,但由于金屬離子堵塞部分微孔導(dǎo)致其比表面積有不同程度下降。經(jīng)負(fù)載金屬離子后,其表面化學(xué)性質(zhì)發(fā)生了明顯變化,金屬離子含量增大,含氧官能團(tuán)增加。負(fù)載金屬離子改性多孔炭對其染料吸附性能有重要影響,由于表面含有大量分散的Zn(II),Zn(Ⅱ)/PC表面形成新的吸附活性位,在較低濃度下,其對亞甲基藍(lán)和直接黑38都表現(xiàn)出優(yōu)異的吸附性能。由于比表面積劇烈下降,Fe(III)/PC對亞甲基藍(lán)的吸附性能較初始炭降低了,但對于分子尺寸較大的直接黑38染料,其吸附性能卻有了明顯提高。動力學(xué)研究表明,擬二級動力學(xué)模型都可以描述改性多孔炭對亞甲基藍(lán)和直接黑38染料的吸附行為。(3)以乙二胺、丙烯酸甲酯、甲醇為原料,采用”一鍋法”制備2.0代的PAMAM。以MC2-19-850為初始炭,通過其表面的羧基與PAMAM發(fā)生氨基酰胺化反應(yīng),將PAMAM嫁接到分級多孔炭上制備新型復(fù)合炭材料PMC。結(jié)果表明;PMC依然含有微孔和中孔,但由于PAMAM的負(fù)載,導(dǎo)致復(fù)合炭的比表面積較初始炭有不同程度下降。對染料的吸附研究表明,調(diào)節(jié)溶液pH值,可改變PMC對酸性染料的吸附性能;中性條件下,由于PMC的比表面積比初始炭小,其對酸性橙74和剛果紅染料的吸附性能低于初始炭。酸性條件下,PMC表面的PAMAM質(zhì)子化,能和染料之間形成靜電吸引作用,其對染料的吸附能力大幅提高,在很低的平衡濃度下,都能表現(xiàn)出極其優(yōu)異的吸附性能。當(dāng)pH值分別為4.4和2.3時,PMC對酸性橙74和剛果紅染料的吸附性能達(dá)到最佳。PMC表面含N量越高,其對染料的吸附性能越高。所制備的復(fù)合炭可用于酸性染料的超深度脫除。
[Abstract]:Adsorption method can be used for selective removal of dye molecules in wastewater under mild conditions. It is widely used in the treatment of dye wastewater. Adsorbents are the core of adsorption technology. This paper takes petroleum asphalt as the carbon source, Zinc Oxide as a template and KOH as activator. The adsorption properties of methyl blue and Direct Black 38 dye were carried out. In order to expand its application field, metal ions were modified on its surface. In order to improve the adsorption properties of porous carbon to acid dyes, the grafting polyamines (PAMAM) tree like macromolecular modification on the surface of coal tar pitch carbon was carried out, and its effect on Acid Orange 74, Congo red dye was studied. The physical structure and surface chemical properties of the graded porous carbon were characterized by nitrogen adsorption and desorption, TEM, FESEM, XRD, XPS. The main results were as follows: (1) using petroleum asphalt as the carbon source, Zinc Oxide was activated by the template coupling KOH to prepare the graded porous carbon (PCs). The results showed that the prepared graded porous carbon was connected with each other. The mass of oil bitumen, Zinc Oxide and KOH are 2,19 and 6 g respectively, and the activation end temperature is 850 C, and the specific surface area of PC_ (2-19-850) is up to 1913 m2/g. to the dye adsorption properties. Methylene blue showed excellent adsorption properties; at the same time, the porous carbon had a certain amount of mesopore, which had a certain adsorption property for the Direct Black 38 with larger molecular size. The adsorption isotherm of the methylene blue dye could be described by Langmuir model, the maximum adsorption amount could reach 887 mg/g, and the adsorption of Direct Black 38 dye, and so on. The temperature line can be described by the Freundlich model. The kinetic study shows that the quasi two order kinetic model can describe the adsorption behavior of the methylene blue to the porous carbon well, and the pseudo first order kinetic model can describe the adsorption behavior of the porous carbon to the Direct Black 38 dye. (2) PC_ (2-19-850) is the initial carbon and the metal ions are loaded on the surface of the carbon. The results of the preparation of modified porous carbon Zn (II) /PC and Fe (III) /PC. showed that the Zn (II) /PC and Fe (III) /PC still contained micropores and mesopore, but the specific surface area of the micropores caused by metal ions blocked the surface area to varying degrees. After loading metal ions, the surface chemical properties of the metal ions changed obviously, the metal ion content was changed. Increased oxygen functional groups increased. The porous carbon loaded with metal ions has an important effect on the adsorption properties of the dyes. Because the surface contains a large number of dispersed Zn (II), the surface of Zn (II) /PC forms a new adsorption active site, and at a lower concentration, it exhibits excellent adsorption properties for methylene blue and Direct Black 38. The adsorption performance of Fe (III) /PC on methylene blue decreased compared with the initial carbon, but the adsorption performance of the Direct Black 38 dye with larger molecular size has been obviously improved. The kinetic study shows that the pseudo two kinetic model can describe the adsorption behavior of modified porous carbon to methylene blue and Direct Black 38 dye. (3) ethylene diamine, C Methyl enate and methanol were used as raw materials. The 2 generation of PAMAM. was prepared by one pot method, and MC2-19-850 was used as initial carbon. Through the carboxyl group on its surface and amidoylation of PAMAM, PAMAM was grafted onto graded porous carbon to prepare a new type of composite carbon material PMC. results. PMC still contained micropores and mesopore, but due to PAMAM load. The specific surface area of the composite carbon decreased in varying degrees than that of the initial carbon. The study on the adsorption of dyes showed that the pH value of the solution could change the adsorption properties of the acid dyes by PMC; under the neutral condition, the adsorption property of the acid orange 74 and the Congo red dye was lower than the initial carbon. Under the acidic condition, the surface of PMC was lower than the initial carbon. The PAMAM protonation can form the electrostatic attraction between the dye and the dye, and the adsorption capacity of the dye is greatly improved. At a very low equilibrium concentration, it can all show excellent adsorption properties. When the pH value is 4.4 and 2.3, the adsorption property of PMC to the acid orange 74 and the Congo red dye is higher than that of the best.PMC surface. The adsorption capacity of the material is higher. The prepared composite carbon can be used for ultra deep removal of acid dyes.

【學(xué)位授予單位】：安徽工業(yè)大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2017
【分類號】：TQ424;X788

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本文編號：1784824