【摘要】：近年來,超濾技術(shù)在水處理領(lǐng)域應(yīng)用逐漸變得非常廣泛。但由于超濾膜易污染,使用成本較高,使得其在推廣過程中受到了極大的限制。本文首先論述了三種自制超濾膜的性能及微觀結(jié)構(gòu),后討論了在不同離子種類(Na+、Ca2+),離子濃度下牛血清蛋白(BSA)對(duì)三種膜材料(PVDF、PES和EVOH)的污染規(guī)律,并結(jié)合石英晶體微天平(QCM-D)等尖端分析手段,對(duì)膜污染機(jī)制進(jìn)行了探討。實(shí)驗(yàn)結(jié)果表明:(1)三種膜材料親水性大小依次為EVOHPESPVDF,膜的親疏水性與膜的被污染能力有關(guān),當(dāng)膜親水時(shí),相比疏水性的膜,不易被污染,因此三種膜的污染嚴(yán)重程度依次為EVOHPESPVDF。對(duì)于膜孔較大的PVDF膜和EVOH膜,由于BSA分子為均勻的橢球體結(jié)構(gòu),分子之間不但不容易互相穿插,且單個(gè)分子更容易透過膜面進(jìn)入膜孔內(nèi),BSA分子容易流失,因此這兩種膜的BSA截留率比PES低。因此這三種膜中PES膜對(duì)BSA的截留能力最強(qiáng)。三種膜中對(duì)BSA吸附量最大的是PVDF膜,其次是PES膜,EVOH膜對(duì)BSA在無離子共存條件下的吸附量最小。(2)三種膜在Na+離子共存條件下的BSA截留率,就整體情況看,PES膜的截留率最高,EOVH的截留率次之,PVDF膜最低。同種超濾膜材料都表現(xiàn)出一致的規(guī)律,即Na+離子濃度越高,BSA的截留率越低,對(duì)于PVDF膜和EVOH膜,當(dāng)Na+離子濃度為100mmol/L時(shí),幾乎不能截留BSA。這可能是由于牛血清蛋白分子與膜表面形成的水合力,使得牛血清蛋白分子很難相互聚集,且它本身分子量較小,反而易于穿過膜孔而使截留率降低。通量恢復(fù)率表現(xiàn)為,隨著離子濃度增大而降低,離子濃度增大到一定程度,通量恢復(fù)率反而升高。Na+離子濃度為0mmol/L,1mmol/L,10mmol/L,100mmol/L時(shí),三種超濾膜在對(duì)BSA的吸附過程中,污染過程初期,吸附速率非常快,形成剛性吸附薄層,而到一定時(shí)間后,吸附層開始展現(xiàn)出粘彈性,吸附量不再增加,吸附過程達(dá)到吸附平衡。當(dāng)離子濃度增大,吸附量越來越大,但當(dāng)離子濃度增大到一定程度,水合作用力成為主導(dǎo)作用力時(shí),由于水合排斥力增加,吸附量反而開始降低。(3)Ca2+離子共存時(shí),在進(jìn)行膜通量衰減實(shí)驗(yàn)、BSA截留率測(cè)定實(shí)驗(yàn)、膜通量恢復(fù)率測(cè)定實(shí)驗(yàn)、BSA在三種材質(zhì)超濾膜上的吸附行為研究實(shí)驗(yàn)時(shí),發(fā)現(xiàn)了與Na+離子共存時(shí)相類似的污染規(guī)律,即Ca2+離子濃度越高,BSA的截留率越低,對(duì)于PVDF膜和EVOH膜,當(dāng)Ca2+離子濃度為100mmol/L時(shí),幾乎不能截留BSA。通量恢復(fù)率表現(xiàn)為,隨著離子濃度增大降低,離子濃度增大到一定程度,通量恢復(fù)率反而升高,吸附行為規(guī)律也與Na+離子共存時(shí)類似。主要由于二價(jià)Ca2+離子與一價(jià)Na+離子同為陽離子,因此其與帶負(fù)電的BSA會(huì)形成靜電屏蔽效應(yīng),使得靜電排斥力減小,膜污染加重。而由于二價(jià)Ca2+離子還存在絡(luò)合作用,其對(duì)膜通量衰減造成的影響較Na+離子略大。
[Abstract]:In recent years, ultrafiltration technology has been widely used in the field of water treatment. However, the UF membrane is easy to pollute and its cost is high, so it is restricted greatly in the process of popularization. In this paper, the properties and microstructure of three kinds of self-made ultrafiltration membranes are discussed, and then the contamination of bovine serum protein (BSA) to three kinds of membrane materials (PVDF, PES and EVOH) under different kinds of ions (Na ~ (2 +) and ion concentration is discussed. The mechanism of membrane fouling was discussed by means of quartz crystal microbalance (QCM-D). The results showed that: (1) the hydrophilicity of the three membrane materials was EVOHPESPVDF.The hydrophobicity of the three membranes was related to the fouling ability of the membrane. When the hydrophilic membrane was hydrophilic, the hydrophobic membrane was not easy to be contaminated, so the serious pollution degree of the three membranes was EVOHPESPVDF. For PVDF and EVOH membranes with larger membrane pores, because the BSA molecule is a uniform ellipsoid structure, it is not easy for the molecules to intersect with each other, and it is easier for a single molecule to enter into the membrane pore through the membrane surface and the BSA molecule is easily lost. Therefore, the BSA retention rate of these two membranes is lower than that of PES. Therefore, PES membrane has the strongest retention ability to BSA. The highest amount of BSA adsorption was PVDF membrane, followed by PES membrane EVOH membrane under the condition of ion-free coexistence. (2) the BSA retention rate of the three membranes under Na ion coexistence condition. On the whole, the PES membrane had the highest rejection rate and the lowest EOVH membrane was PVDF membrane. The same ultrafiltration membrane material showed the same rule that the higher the concentration of Na ion, the lower the rejection rate of BSA. For PVDF membrane and EVOH membrane, when Na ion concentration was 100 mmol / L, BSAs could hardly be intercepted. This may be due to the water binding between bovine serum protein molecules and the membrane surface, which makes it difficult for the bovine serum protein molecules to aggregate with each other, and its molecular weight is small, which makes it easy to penetrate the membrane pore and reduce the rejection rate. The flux recovery rate decreases with the increase of ion concentration, increases to a certain extent, and increases to a certain extent. When the concentration of Na ion is 0 mmol / L ~ (-1) mol / L ~ (10) mmol / L ~ (10) mmol / L ~ (-1), the three kinds of ultrafiltration membranes are in the initial stage of fouling process in the process of adsorption of BSA. The adsorption rate is very fast and the rigid adsorption layer is formed. After a certain time the adsorption layer begins to show viscoelasticity and the adsorption amount does not increase and the adsorption process reaches the adsorption equilibrium. When the ion concentration increases, the adsorption capacity increases, but when the ion concentration increases to a certain extent and the hydration force becomes the dominant force, the adsorption capacity begins to decrease because of the increase of the hydration repulsion force. (3) when the Ca 2 + coexists, the adsorption capacity begins to decrease. In the experiments of membrane flux attenuation and membrane flux recovery, the adsorption behavior of BSA on three kinds of ultrafiltration membranes was studied, and the pollution law was found to be similar to that of Na ions. The higher the concentration of Ca 2 +, the lower the rejection rate of BSA. For PVDF and EVOH membranes, when Ca 2 + concentration is 100 mmol / L, BSAs can hardly be intercepted. The flux recovery rate shows that with the increase of ion concentration, ion concentration increases to a certain extent, the flux recovery rate increases, and the adsorption behavior is similar to that when Na ion coexists. Because the bivalent Ca2 + and monovalent Na are cations, the electrostatic shielding effect is formed with the negative BSA, and the electrostatic repulsive force decreases and the membrane fouling is aggravated. Because of the complexation of the bivalent Ca 2 +, the effect of Ca 2 + on the flux attenuation of the membrane is slightly greater than that of Na ion.
【學(xué)位授予單位】：西安建筑科技大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2015
【分類號(hào)】：X703;TQ028.8

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