本文關(guān)鍵詞： PhACs 改性石英砂 吸附 影響因素 表征　出處：《河北工程大學(xué)》2017年碩士論文　論文類型：學(xué)位論文

【摘要】：由于人類對(duì)醫(yī)藥活性物質(zhì)(Pharmaceutically Active Compounds,PhACs)的過分使用甚至是濫用,導(dǎo)致這類化合物及其代謝產(chǎn)物被持續(xù)不斷地排入地表水、地下水及土壤等各種環(huán)境介質(zhì)中,PhACs在環(huán)境中的遷移、轉(zhuǎn)化、生態(tài)毒理及其控制處理已成為環(huán)境科技界日益關(guān)注的熱點(diǎn)問題。而在我國,還鮮有此方面的研究報(bào)道。而且我國70%以上的污水處理廠并沒有針對(duì)PhACs建設(shè)專門的去除工藝(或工段)。因此,有必要研究新型的深度處理工藝來去除PhACs,以降低PhACs對(duì)水環(huán)境造成的污染。本試驗(yàn)研究,以Piranha溶液、KH-550水解液以及鐵鹽作為改性劑對(duì)石英砂濾料進(jìn)行改性,改性后的石英砂其表面變得凹凸不平,通過掃描電鏡(SEM)、X射線衍射、紅外光譜和有機(jī)碳含量分析對(duì)改性前后的石英砂濾料進(jìn)行表面結(jié)構(gòu)表征�；谖絼�(dòng)力學(xué)試驗(yàn)及等溫吸附平衡試驗(yàn)考察了普通、親水改性、疏水改性和鐵離子改性(生物)石英砂對(duì)PhACs的吸附過程;研究了石英砂改性前后以及生物覆膜前后對(duì)PhACs吸附性能的影響;分析了其吸附機(jī)理以及微生物在生物覆膜石英砂去除PhACs中的貢獻(xiàn)率。研究結(jié)果表明:(1)以Piranha溶液、KH-550水解液以及鐵鹽作為改性劑對(duì)粒徑為1.0mm~1.7mm的石英砂進(jìn)行改性,得到親水改性、疏水改性和鐵離子改性這三種改性石英砂。本試驗(yàn)選用四環(huán)素、環(huán)丙沙星及美托洛爾作為研究對(duì)象。經(jīng)過Piranha溶液處理后,石英砂表面的雜質(zhì)被氧化處理后呈現(xiàn)網(wǎng)狀立體結(jié)構(gòu),比表面積增大,因此親水改性石英砂對(duì)PhACs的吸附去除效果最好;與普通石英砂相比,疏水改性和鐵離子改性石英砂對(duì)所選用的三種PhACs的去除效果有不同程度的下降。(2)基于吸附動(dòng)力學(xué)試驗(yàn)結(jié)果,可發(fā)現(xiàn)改性石英砂和生物覆膜石英砂對(duì)PhACs的靜態(tài)吸附均在2h內(nèi)基本達(dá)到平衡,改性石英砂及生物覆膜石英砂對(duì)PhACs的靜態(tài)吸附過程均符合偽一級(jí)動(dòng)力學(xué)模型,其主要吸附機(jī)制均為表面物理吸附。(3)基于等溫吸附平衡試驗(yàn)結(jié)果,可發(fā)現(xiàn)當(dāng)試驗(yàn)溫度在288.15 K~309.15 K之間變化時(shí),Langmuir等溫吸附模型能更好地描述試驗(yàn)所得改性石英砂及生物覆膜石英砂對(duì)TCN、CIP和MTP的靜態(tài)等溫吸附行為。溫度越接近298.15 K,改性石英砂以及生物覆膜石英砂對(duì)PhACs的靜態(tài)吸附量越大。當(dāng)pH在2.0~12.0的范圍內(nèi)變化時(shí),美托洛爾的靜態(tài)吸附效果不受pH值的影響,但強(qiáng)酸環(huán)境有利于四環(huán)素和環(huán)丙沙星的靜態(tài)吸附,由此推斷改性石英砂和生物覆膜石英砂對(duì)四環(huán)素和環(huán)丙沙星的主要吸附機(jī)制是陽離子吸附,對(duì)美托洛爾的主要吸附機(jī)理則是表面吸附。在PhACs溶液中分別加入K+、Na+和Ca2+時(shí),其吸附效果均有不同程度的降低,其中Ca2+的抑制效果明顯高于K+和Na+。(4)基于電鏡掃描結(jié)果,可發(fā)現(xiàn)生物覆膜石英砂表面所附球菌、短桿菌、長桿菌以及節(jié)桿菌等與胞外聚合物共同形成了多孔且結(jié)構(gòu)復(fù)雜的生物膜,此類生物膜對(duì)PhACs的削減具有明顯的強(qiáng)化作用;通過序批試驗(yàn)研究,發(fā)現(xiàn)覆膜石英砂對(duì)PhACs的削減包含濾料吸附、微生物吸附及微生物降解三個(gè)途徑,各途徑貢獻(xiàn)率隨藥物的品種不同而表現(xiàn)出明顯差異,如除疏水改性、鐵離子改性和普通生物覆膜石英砂對(duì)環(huán)丙沙星的降解率高于40%外;其余生物覆膜石英砂對(duì)PhACs的降解率僅在0~9.84%之間。
[Abstract]:Because of human pharmaceutical active substances (Pharmaceutically Active Compounds, PhACs) the excessive use and even abused, resulting in such compounds and their metabolites is continuously discharged into surface water, groundwater and soil environment, PhACs migration and transformation in the environment, ecological toxicology and control processing has become a hot issue of growing concern environmental science and technology circles. But in China, few studies of this report. And the sewage treatment plant in China more than 70% and not for removal of specialized PhACs construction (or section). Because of this, it is necessary to study the removal of PhACs advanced treatment process model, in order to reduce the PhACs of water environment pollution. This experiment, using Piranha solution, KH-550 hydrolysate and ferric salt as the quartz sand modifier, modified quartz sand the surface becomes uneven, through Scanning electron microscopy (SEM), X ray diffraction, the surface characterization of the modified quartz sand filter before and after the analysis of infrared spectrum and organic carbon content. The adsorption kinetics and isothermal adsorption equilibrium were investigated based on common, hydrophilic, hydrophobic modification and iron ion modified (bio) adsorption process of quartz sand of PhACs the study on the quartz sand; before and after modification and effect of biological film before and after the adsorption of PhACs on the analysis; the adsorption mechanism and microorganisms in biological removal of PhACs coated quartz sand in the contribution rate. The results show that: (1) to Piranha solution, KH-550 hydrolysate and ferric salt as a modifier of the particle size of 1.0mm~1.7mm the quartz sand was modified by hydrophilic and hydrophobic modification and iron ion modification of these three kinds of modified quartz sand. The tetracycline, ciprofloxacin and metoprolol as the research object. Through the Piranha solution After treatment, the surface impurities of quartz sand by oxidation treatment showed mesh structure, specific surface area increases, so the hydrophilic modification of quartz sand on the adsorption of PhACs had the best removal effect; compared with the ordinary quartz sand, hydrophobic modification and iron ion modified quartz sand for three PhACs the removal effect decreased different degree. (2) the results of adsorption kinetics can be found based on the modified quartz sand and bio coated quartz sand of PhACs static adsorption were basically reached equilibrium in 2H process, the static adsorption of PhACs on modified quartz sand coated quartz sand and biological are in line with the pseudo first order kinetic model, the adsorption mechanism are the physical surface adsorption isotherm. (3) based on the experimental results can be found when the test temperature changes between 288.15 K~309.15 K, Langmuir isotherm model can better describe the test of the modified quartz sand and The biological behavior of TCN coated quartz sand, static adsorption CIP and MTP. The temperature is close to 298.15 K, modified quartz sand coated quartz sand and biological adsorption capacity of PhACs increases. When the pH changes in the range of 2.0~12.0, effects of static adsorption of metoprolol was not affected by pH value, but the strong acid environment is the static adsorption to tetracycline and ciprofloxacin, concluded that the modified quartz sand coated quartz sand and biological adsorption mechanism mainly to tetracycline and ciprofloxacin is the main mechanism of cation adsorption, adsorption of metoprolol is adsorbed on the surface. K+ were added in PhACs solution, Na+ and Ca2+, reduce the adsorption effect in varying degrees among them, the inhibitory effect of Ca2+ was significantly higher than that of K+ and Na+. (4) based on the results of scanning electron microscope, can be found in bio coated quartz sand surface of coccus, Bacillus brevis and Bacillus coli, long day and cell Polymer together form the biofilm structure and complex porous, the biofilm has obvious effect on the strength of PhACs cut; by batch experiments, found that the coated quartz sand on the PhACs cut filter contains microbial adsorption, adsorption and microbial degradation of three ways, the way of contribution rate of different varieties with drugs significant differences, such as hydrophobic modification, iron ion modification and biological degradation of ciprofloxacin coated quartz sand rate is higher than 40%; the remaining bio coated quartz sand on the degradation rate of PhACs is only 0~9.84%.

【學(xué)位授予單位】：河北工程大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2017
【分類號(hào)】：X703

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1 尹然;改性生物砂濾工藝對(duì)城市污水廠尾水中典型PhACs的去除機(jī)理研究[D];河北工程大學(xué);2017年

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本文編號(hào)：1530297