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催化臭氧響應(yīng)膜制備及應(yīng)用研究

發(fā)布時(shí)間:2018-06-13 13:44

  本文選題:腐植酸 + 催化臭氧化; 參考:《東北電力大學(xué)》2017年碩士論文


【摘要】:腐植酸(Humic Acids,HA)廣泛地分布在地表水中,因使水變成褐色,與金屬或有機(jī)物反應(yīng)生成復(fù)雜物質(zhì),與活性氯反應(yīng)生成消毒副產(chǎn)物而得到廣泛關(guān)注,如何有效去除水中HA具有重要意義。膜分離技術(shù)在HA處理過(guò)程中的得到廣泛關(guān)注,然而膜污染問(wèn)題是制約該技術(shù)發(fā)展的瓶頸。催化臭氧化技術(shù)可有效降解水中有機(jī)物,但催化降解過(guò)程中存在著催化劑流失和回收等問(wèn)題。通過(guò)將具有催化臭氧能力強(qiáng)的催化劑負(fù)載到膜上,制備出催化臭氧化響應(yīng)膜,依靠膜分離與催化臭氧化技術(shù)耦合來(lái)提高膜分離效率,并解決催化劑流失、回收以及膜污染的問(wèn)題。本研究開(kāi)發(fā)了一種具有高催化活性的催化臭氧響應(yīng)膜,并將其與催化臭氧化技術(shù)耦合來(lái)處理HA,研究?jī)?nèi)容和結(jié)果如下:(1)采用溶膠-凝膠法制備納米TiO_2,用響應(yīng)面法優(yōu)化納米TiO_2催化臭氧降解HA的最佳實(shí)驗(yàn)條件,得到的最佳實(shí)驗(yàn)條件為:煅燒溫度為565℃,TiO_2投加量為0.31 g/L,臭氧濃度為16.75 mg/L,溶液pH為6.91;此條件下HA的去除率為87.15%。(2)采用溶膠-凝膠法制備出不同Ti-Ce復(fù)合物(摻雜Ti/Ce摩爾比為0.2-1.0)。在最佳實(shí)驗(yàn)條件下,通過(guò)考察催化臭氧氧化HA的活性,篩選出最佳的Ti/Ce摻雜比為1/0.8;通過(guò)比較單獨(dú)臭氧氧化、TiO_2催化臭氧化、Ti-Ce(1/0.8)復(fù)合物催化臭氧化中臭氧利用率、表觀分子量分布,發(fā)現(xiàn)Ti-Ce(1/0.8)復(fù)合物催化臭氧化中臭氧的利用率最高,達(dá)到62%,并且其催化降解HA和中間產(chǎn)物的效果最好,表明Ti-Ce(1/0.8)復(fù)合物具有高的催化活性;在催化臭氧降解HA過(guò)程中,通過(guò)研究均相和異相反應(yīng)的動(dòng)力學(xué)表明:均相和異相反應(yīng)的速率分別為0.054 min-1及0.066 g·L-1·min-1;此外,異相反應(yīng)對(duì)污染物去除貢獻(xiàn)率在所有pH下均小于50%,說(shuō)明催化降解HA的反應(yīng)主要發(fā)生在本體溶液中。(3)采用共混法制備了不同含量Ti-Ce(1/0.8)復(fù)合物的催化膜,通過(guò)SEM表明Ti-Ce復(fù)合物成功共混于催化膜,Ti-Ce(1/0.8)復(fù)合物添加量為2%時(shí),催化膜的孔隙率和平均孔徑均增大;Ti-Ce(1/0.8)復(fù)合物的添加影響著膜的親疏水性、純水通量、截留率、平均孔徑及孔隙率;通過(guò)接觸角測(cè)定表明:Ti-Ce復(fù)合物添加量為2%時(shí),催化臭氧化膜的接觸角降低的最為明顯,繼續(xù)增加復(fù)合物添加量沒(méi)有引起接觸角顯著降低;通過(guò)與PVDF純膜、1%Ti-Ce(1/0.8)/PVDF膜和3%Ti-Ce(1/0.8)/PVDF膜相比,2%Ti-Ce(1/0.8)/PVDF膜的純水通量增加最明顯,達(dá)到32.61 L·m-2·h-1,但其截留率有所降低。(4)對(duì)催化臭氧響應(yīng)膜處理HA的研究表明:催化臭氧化響應(yīng)膜對(duì)HA和溶液TOC的去除率大小順序?yàn)?2%Ti-Ce(1/0.8)/PVDF膜+O33%Ti-Ce(1/0.8)/PVDF膜+O_31%Ti-Ce(1/0.8)/PVDF膜+O3PVDF膜+O_3。PVDF膜的通量衰減最嚴(yán)重,為初始值的31%,2%Ti-Ce(1/0.8)/PVDF膜的通量明顯提高,衰減量?jī)H為初始量的23%。進(jìn)一步研究表明,與純膜相比,2%Ti-Ce(1/0.8)/PVDF膜的可逆污染阻力和不可逆污染阻力分別降低了37%和58%,表明2%Ti-Ce(1/0.8)復(fù)合物強(qiáng)化了膜孔中的催化臭氧化反應(yīng),具有自清潔膜的特征。
[Abstract]:Humic acid (humic acid) is widely distributed in surface water. It is widely concerned about how to effectively remove HA from water because it becomes brown, reacts with metal or organic compounds to form complex substances and reacts with active chlorine to form disinfection by-products. Membrane separation technology has been widely concerned in the process of HA treatment. However, membrane fouling is the bottleneck to the development of this technology. Catalytic ozonation can effectively degrade organic matter in water, but there are some problems such as catalyst loss and recovery in the process of catalytic degradation. The catalytic ozonation response membrane was prepared by loading the catalyst with strong catalytic ozone ability onto the membrane. The membrane separation efficiency was improved by the coupling of membrane separation and catalytic ozonation technology, and the loss of catalyst was solved. Recovery and membrane fouling. In this study, a catalytic ozone responsive membrane with high catalytic activity was developed. The results are as follows: (1) Nano-TiO-2 was prepared by sol-gel method, and the optimum experimental conditions for the catalytic ozonation of HA were optimized by response surface method. The optimum experimental conditions are as follows: calcination temperature is 565 鈩,

本文編號(hào):2014218

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