親水性分子印跡聚合物用于水中硝基酚類(lèi)污染物的選擇性萃取及去除研究
發(fā)布時(shí)間:2018-06-12 09:25
本文選題:分子印跡聚合物 + 硝基酚類(lèi)污染物。 參考:《華中科技大學(xué)》2013年碩士論文
【摘要】:分子印跡技術(shù)(Molecular Imprinting Technique,MIT),是基于抗原/抗體的基本原理而延伸的分子識(shí)別技術(shù)。分子印跡聚合物(Molecularly Imprinted Polymers,MIPs)是在模板分子存在的情況下,運(yùn)用分子印跡技術(shù)通過(guò)功能單體與交聯(lián)劑的共聚反應(yīng)制得,去除模板分子后,分子印跡聚合物上可形成與模板分子在空間結(jié)構(gòu)上相匹配的三維孔穴,可特異性地吸附模板分子及其結(jié)構(gòu)類(lèi)似物,因此也被稱(chēng)為“人工抗體”。本文采用沉淀聚合的方法,獲得了對(duì)硝基酚類(lèi)污染物具有特異性識(shí)別作用的親水性分子印跡聚合物(MIPs),并實(shí)現(xiàn)水體中痕量硝基酚污染物的選擇性萃取及去除。主要研究?jī)?nèi)容由以下兩部分組成: 1.為了克服傳統(tǒng)固相萃取所具有的缺點(diǎn),本研究采用親水性MIPs-固相微柱萃取技術(shù)對(duì)水樣(東湖,長(zhǎng)江,工業(yè)廢水)中硝基酚類(lèi)污染物進(jìn)行萃取。固相微柱萃取技術(shù)不需要傳統(tǒng)的萃取裝置及蒸發(fā)等復(fù)雜操作流程,僅通過(guò)離心便可完成對(duì)樣品的上樣、淋洗和洗脫,具有操作簡(jiǎn)單、快速的優(yōu)點(diǎn)。在最佳萃取條件下,親水性MIPs-固相微萃取柱對(duì)硝基酚類(lèi)化合物的萃取回收率達(dá)到87%-92.9%,且具有良好的凈化效果。與常規(guī)的萃取吸附劑(活性炭、多壁碳納米管、LC-C18等)相比,,親水性MIPs顯示出更高的萃取效率和更好的選擇性識(shí)別性能。本研究建立親水性MIPs-固相微柱萃取結(jié)合HPLC-UV法對(duì)實(shí)際水樣中硝基酚類(lèi)污染物進(jìn)行檢測(cè),結(jié)果顯示:該方法的線性范圍為2-1000ng/mL(2,4-二硝基酚,2-硝基酚)、6-1000ng/mL(4-硝基酚),相關(guān)系數(shù)(R2)大于0.998,方法檢測(cè)限為0.3-0.5ng/mL,日內(nèi)RSDs值為4.0%-6.7%,日間(5日)RSDs值為5.9%-8.2%。 2.將親水性MIPs作為吸附劑對(duì)地表水及工業(yè)廢水中2,4-二硝基酚進(jìn)行選擇性去除研究。吸附動(dòng)力學(xué)模型及吸附等溫模型結(jié)果顯示,親水性MIPs對(duì)2,4-二硝基酚的最大吸附容量為138.9mg/g,同時(shí),進(jìn)一步研究了吸附過(guò)程中水樣的流速、初始濃度、pH和腐殖酸含量對(duì)去除效果的影響。大體積上樣時(shí)(上樣體積高達(dá)1L),與活性炭、多壁碳納米管、LC-C18等常規(guī)吸附柱及常規(guī)方法制備的MIPs相比,親水性MIPs(100mg)具有最好的去除效率(92%),并可重復(fù)使用5次以上,具有較好的實(shí)際應(yīng)用前景。
[Abstract]:Molecular imprinting technique is an extended molecular recognition technique based on the basic principle of antigen / antibody. Molecularly imprinted polymers (MIPs) were prepared by the copolymerization of functional monomers and crosslinkers in the presence of template molecules, and the template molecules were removed. Molecular imprinted polymers can form three-dimensional pores that match the spatial structure of template molecules, and can specifically adsorb template molecules and their structural analogues, so they are also called "artificial antibodies". In this paper, a hydrophilic molecularly imprinted polymer (MIPsN) with specific recognition effect on nitrophenols was obtained by precipitation polymerization, and the selective extraction and removal of trace nitrophenol pollutants in water were realized. The main research content consists of the following two parts: 1. In order to overcome the shortcomings of traditional solid phase extraction (SPE), the hydrophilic MIPs- solid phase microcolumn extraction (SPME) technique was used to extract nitrophenols from water samples (Donghu, Yangtze River, industrial wastewater). Solid-phase microcolumn extraction technology does not need the traditional extraction equipment and evaporation and other complex operation flow, only by centrifugation can be completed on the sample, elution and elution, has the advantages of simple operation, rapid operation. Under the optimum extraction conditions, the extraction recovery of hydrophilic MIPs- solid phase microextraction column was 87-92. 9%, and it had a good purification effect. Compared with conventional extraction adsorbents (activated carbon, multi-walled carbon nanotubes, LC-C18, etc.), hydrophilic MIPs show higher extraction efficiency and better selective recognition performance. A hydrophilic MIPssolid phase microcolumn extraction (SPME) method combined with HPLC-UV was established for the determination of nitrophenols in real water samples. The results showed that the linear range of the method was 2-1000ng / mL ~ (2) -dinitrophenol ~ (2-nitrophenol) = 6-1000ng / m ~ (-1) N ~ (-1) 路m ~ (-1) N ~ (4-nitrophenol) > 0.998, the detection limit was 0.3-0.5ng 路mL ~ (-1), the value of RSDs within day was 4.0-6.7, and the value of RSDs was 5.9- 8.22. Hydrophilic MIPs were used as adsorbents for selective removal of 2-trichloro-4-dinitrophenol from surface water and industrial wastewater. The results of adsorption kinetics model and adsorption isotherm model show that the maximum adsorption capacity of hydrophilic MIPs for 2o 4-dinitrophenol is 138.9 mg / g. At the same time, the flow rate of water sample during the adsorption process is further studied. Effects of initial concentration pH and humic acid content on removal efficiency. The hydrophilic MIPsn 100mgcompared with conventional adsorption columns such as activated carbon, multi-walled carbon nanotube LC-C18 and MIPs prepared by conventional methods, has the best removal efficiency and can be reused for more than 5 times. It has a good prospect of practical application.
【學(xué)位授予單位】:華中科技大學(xué)
【學(xué)位級(jí)別】:碩士
【學(xué)位授予年份】:2013
【分類(lèi)號(hào)】:R123.1
【參考文獻(xiàn)】
相關(guān)期刊論文 前1條
1 張繼義;王利平;常玉枝;;麥草對(duì)水中苯胺的吸附平衡、熱力學(xué)和動(dòng)力學(xué)研究[J];農(nóng)業(yè)系統(tǒng)科學(xué)與綜合研究;2011年03期
本文編號(hào):2009194
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