零價(jià)鐵復(fù)合膜制備及對(duì)有機(jī)污染物的催化還原效能
本文選題:層層自組裝技術(shù) + 配位作用; 參考:《天津工業(yè)大學(xué)》2017年碩士論文
【摘要】:本文采用聚丙烯腈(PAN)平板膜作為基膜材料,通過(guò)靜態(tài)層層自組裝技術(shù)制備聚二烯丙基二甲基氯化銨(PDADMAC)、聚丙烯酸(PAA)組裝聚電解質(zhì)復(fù)合膜,再經(jīng)過(guò)羧基-亞鐵離了的配位作用以及經(jīng)典液相還原法制備(Fe~0-PDADMAC/PAA)n復(fù)合催化膜。用于水體中亞硝基二甲胺(NDMA)和酸性紅染料(ARB)的還原轉(zhuǎn)化研究。研究中,FTIR分析發(fā)現(xiàn)增強(qiáng)基膜表面親水性和荷電性,有利于后續(xù)的聚電解質(zhì)在膜表面的組裝;掃描電鏡圖顯示復(fù)合膜表面的零價(jià)鐵分散均勻,粒徑在200nm左右;紫外分析可知,層數(shù)n==,3,5,7,9時(shí),復(fù)合膜中鐵的含量分別為 25.7,77.6,114,151.7,171.4 mg·g-1;XPS 和 XRD 數(shù)據(jù)分析表明,零價(jià)鐵與有機(jī)污染物反應(yīng)后,零價(jià)鐵轉(zhuǎn)化為Fe3+/Fe2+,并主要以Fe203和Fe3O4存在于膜表面上。在研究復(fù)合膜對(duì)NDMA和ARB還原轉(zhuǎn)化過(guò)程中發(fā)現(xiàn),反應(yīng)初期的反應(yīng)速率較快,后期達(dá)到平穩(wěn),反應(yīng)時(shí)間較短。(Fe~0-PDADMAC/PAA)9對(duì)于初始濃度為150μg·L-1的NDMA溶液的去除效率為65.8%,對(duì)于初始濃度為100mg·L-1的ARB溶液的去除效率接近100%。pH值、反應(yīng)溫度和共存離子等因素均對(duì)污染物的去除有一定的影響。(Fe~0-PDADMAC/PAA)n復(fù)合催化膜中的Fe~0氧化釋放電子,使得氫原子活化,與目標(biāo)污染物發(fā)生還原反應(yīng),達(dá)到降解去除的作用。研究表明降解反應(yīng)過(guò)程中,Fe還原污染物后,單位質(zhì)量膜上Fe的溶出量均小于0.1mg·g-1。復(fù)合膜表面具有的羧基與還原反應(yīng)過(guò)程中生成的鐵離子再次絡(luò)合,將鐵離子繼續(xù)固定在PAN膜上。
[Abstract]:In this paper, polyacrylonitrile (PAN) flat film was used as the base film material, and the polydiallyl dimethyl ammonium chloride (PDADMAC), polyacrylic acid (PAA) polyelectrolyte composite film was prepared by static layer self-assembly technique. The Fe0-PDADMAC / PAA _ (n) composite catalytic membrane was prepared by the coordination of carboxyl-ferrous ionization and the classical liquid-phase reduction method. It was used to study the reduction and transformation of nitrosodimethylamine (NDMA) and acid red dye (ARB) in water. FTIR analysis showed that the enhancement of the hydrophilicity and charge-resistance of the substrate surface was beneficial to the subsequent assembly of polyelectrolytes on the membrane surface, and the scanning electron microscopy showed that the zero-valent iron on the surface of the composite film was uniformly dispersed and the particle size was about 200nm. The iron content in the composite membrane was 25.77.6114151.7mg / g ~ (-1) and 171.4 mg / g ~ (-1) XRD, respectively. The results showed that after the reaction of zero-valent iron with organic pollutants, the zero-valent iron was converted to Fe3 / Fe _ 2 and mainly existed on the surface of the film as Fe203 and Fe3O4. In the study of the reduction and conversion of NDMA and ARB by the composite membrane, it was found that the reaction rate was relatively fast at the initial stage of the reaction, and the reaction rate was stable at the later stage. The removal efficiency of NDMA solution with initial concentration of 150 渭 g 路L ~ (-1) was 65.8%, and the removal efficiency of ARB solution with initial concentration of 100mg ~ (-1) was close to 100%.pH value. Factors such as reaction temperature and co-existing ions have a certain effect on the removal of pollutants. The oxidation and release of electrons by Fe~0 in the Fe0-PDADMAC / PAA _ (n) composite catalytic membrane lead to the activation of hydrogen atoms and the reduction of hydrogen atoms with the target pollutants, so as to achieve the effect of degradation and removal. The results showed that the amount of Fe dissolved on the film was lower than that of 0.1mg g ~ (-1). The carboxyl group on the surface of the composite membrane was recomplexed with the iron ions produced during the reduction reaction, and the iron ions were immobilized on the PAN film.
【學(xué)位授予單位】:天津工業(yè)大學(xué)
【學(xué)位級(jí)別】:碩士
【學(xué)位授予年份】:2017
【分類(lèi)號(hào)】:TB383.2;X703
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