微波Fenton活性炭协同作用去除水体中盐酸黄连素的研究

发布时间：2018-07-16 16:46

【摘要】：随着全球化的脚步,经济社会高速发展,与此同时制药领域伴随出现大量新的药品,其中就包括盐酸黄连素。其出现对于病患有着重要的意义,与此同时对于环保领域,也带来了新的挑战。盐酸黄连素(分子式C20H18NO4)是常见的制药行业产生物,一般情况下为黄色针状结晶或者粉末状,无臭、味苦。盐酸黄连素被服用后在生物体内的吸收率较低,未被吸收的盐酸黄连素排出生物体外,通过环境中的迁移转化规律进入到环境水体中,再加上工业生产盐酸黄连素会产生大量含有盐酸黄连素的废水排入水环境中,水环境中的很多微生物的生长会受到其抑制,甚至被盐酸黄连素消除,导致生存于水环境中的很大一部分微生物在其生长与繁殖的过程中受到严重影响,从而破坏了生态系统的平衡性以及生态系统中食物链的流通性和完整性;同时,在环境中生物体内积累并沿食物链传递,因此可能会诱导产生抗药基因,会在环境中传播及扩散,对人类健康和食品及饮用水安全构成严重威胁,尤其是近些年来出现的超级致病菌已成为医学难题。但国内对该废液的具体去除却鲜有报道.目前盐酸黄连素的处理方法主要有物理法、电化学法、生物法等。然而,物理法处理盐酸黄连素只完成了环境介质的转移,并未使之得到降解,大部分高级氧化技术实际工程化应用非常少,而且有对环境产生二次污染的风险,电化学法因其成本偏高,故实际工程的应用价值有限,用生物法处理初始浓度较高或变化较大的盐酸黄连素废水,处理效果很可能不够理想,相关的技术研究难以应用于实际污水特别是水环境中高浓度抗菌药类物质的处理中,同时,由于微波具有强穿透效果的能力,因为可以直接加热于反应物分子,使分子的化学键强度和反应物体系的活化能得到改变,与此同时使用活性炭与Fenton作为催化剂,使反应活性大大增强,从而达到更好的去除效果。实验针对模拟盐酸黄连素废水进行预处理,为解决同类制药废水去除问题提供了技术参考。分别采用光降解、单独微波、单独活性炭、单独Fenton试剂、Fenton-活性炭联用、微波-Fenton-活性炭联用技术五种方法去除水中盐酸黄连素,分别考察不同方法对盐酸黄连素去除效果的影响,同时考察微波时间、微波功率、活性炭投加量、腐殖酸投加量、Fe~(2+)投加量、H_2O_2投加量对盐酸黄连素去除率的影响,并分别使用氢氧化钠、硫酸、氯化钠、硅酸钠对活性炭进行改性效果比较。最后确定一定浓度的盐酸黄连素溶液,通过正交实验确定盐酸黄连素的最佳去除条件,并探究此条件下盐酸黄连素残液的可生化性,以及是否符合一级动力学模型。结果表明:单独微波技术对盐酸黄连素去除基本没有效果,单独活性炭技术、光降解以及单独Fenton技术耗时长,效果低。Fenton-活性炭技术的去除效果高于单独技术,而微波-Fenton-活性炭联用技术对盐酸黄连素的去除效果远大于其他技术。随着溶液中盐酸黄连素初始浓度的不断增加,去除率呈现降低趋势;加大活性炭的投加量,去除率先增加后降低;过氧化氢浓度、腐殖酸浓度、Fe~(2+)投加量的不断增加,整体呈现出基本增加再趋于减少的态势。而随着微波时间以及微波功率的增加,盐酸黄连素的去除率却不停增大。研究确定了六因子三水平,通过正交实验得出了盐酸黄连素去除的最佳去除条件。得到盐酸黄连素的最佳去除条件为:腐殖酸0.008g/L,Fe~(2+)0.41g/L,活性炭0.7 g,微波功率700W,微波时间5min,H_2O_26mol/L,在此条件下盐酸黄连素的去除率达到了86.47%。根据上述最佳条件,通过实验得到最佳去除条件下的残液,考察其可生化性。结果表明:该残液的BOD/COD值为0.353,TOC/TN值为101.65,认为此液体具有一定的可生化性,并且基本符合一级动力学。
[Abstract]:With the pace of globalization and the rapid development of the economy and society, at the same time, a large number of new drugs are accompanied in the pharmaceutical field, including berberine hydrochloride, which has an important significance for the disease. At the same time, it also brings new challenges to the field of environmental protection. The hydrochloric acid (C20H18NO4) is a common pharmaceutical industry. Biological, usually yellow needle like crystalline or powdery, odorless, bitter. The absorption rate of berberine hydrochloride in the organism is low, and berberine hydrochloride, which is not absorbed, is discharged into the environment by the law of transfer and transformation in the environment, and the production of berberine hydrochloride in industrial production will produce a large amount of content. The wastewater containing berberine hydrochloride is discharged into the water environment, and the growth of many microorganisms in the water environment will be inhibited, even by berberine hydrochloride. A large portion of microorganisms living in the water environment are seriously affected during their growth and reproduction, which destroys the balance of the ecosystem and the ecosystem. The circulation and integrity of the food chain in the medium, as well as the accumulation in the environment and the transmission along the food chain, may induce the production of antidrug genes, spread and spread in the environment, and pose a serious threat to the health of human health and the safety of food and drinking water, especially the super pathogenic bacteria that have emerged in recent years have become a medical problem. At present, there are few reports on the specific removal of the waste liquid in China. At present, there are physical, electrochemical and biological methods for the treatment of berberine hydrochloride. However, the physical treatment of berberine hydrochloride only completes the transfer of the environmental medium, and does not degrade it. Most advanced oxygenation techniques have very little engineering application and have the opposite ring. Because of the high risk of two pollution, the electrochemical method has a high cost because of its high cost, so the application value of the practical engineering is limited. It is not ideal to treat berberine hydrochloric acid wastewater with higher initial concentration or larger change by biological method. The related technical research is difficult to apply to the practical wastewater, especially the high concentration antibiotics in water environment. In the process of material treatment, at the same time, because microwave has the ability of strong penetration effect, because it can be heated directly to the reactant molecules, the chemical bond strength of the molecule and the activation energy of the reactant system can be changed. At the same time, the active carbon and Fenton are used as catalysts to greatly enhance the activity of the reaction, thus achieving a better removal effect. The pretreatment of berberine hydrochloric acid wastewater has provided a technical reference for the removal of similar pharmaceutical wastewater. Five methods were used to remove berberine hydrochloride in water respectively by five methods, such as photodegradation, separate microwave, separate active carbon, separate Fenton reagent, Fenton- activated carbon, and microwave -Fenton- activated carbon. Methods on the effect of berberine hydrochloride removal, the effects of microwave time, microwave power, activated carbon dosage, humic acid dosage, Fe~ (2+) dosage and H_2O_2 dosage on the removal rate of berberine hydrochloride were investigated. The effects of sodium hydroxide, sulphuric acid, sodium chloride and sodium silicate on the modified activated carbon were compared. The optimum removal condition of berberine hydrochloride was determined by orthogonal experiment, and the biodegradability of berberine hydrochloride residue was investigated and the first order kinetic model was found. The results showed that the isolation of Berberine Hydrochloride by separate microwave technology was not effective. As well as the long time of Fenton technology, the removal efficiency of.Fenton- activated carbon technology is higher than that of the single technology, and the removal efficiency of Berberine Hydrochloride by microwave -Fenton- activated carbon technology is much greater than that of other technologies. In addition, the removal rate of hydrogen peroxide concentration, humic acid concentration and Fe~ (2+) increased gradually, and the overall increase tended to decrease, while the removal rate of berberine hydrochloride increased with the increase of microwave time and microwave power. The study determined the six factor and three level, through orthogonal reality. The optimum removal conditions for the removal of berberine hydrochloride were obtained. The optimum removal conditions for berberine hydrochloride were as follows: humic acid 0.008g/L, Fe~ (2+) 0.41g/L, activated carbon 0.7 g, microwave power 700W, microwave time 5min, H_2O_26mol/L. Under these conditions, the removal rate of berberine hydrochloride reached 86.47%. according to the above conditions and obtained through experiments. The biodegradability of the residual liquid under the optimum conditions was investigated. The results showed that the BOD/COD value of the residual liquid was 0.353 and the value of TOC/TN was 101.65. It was considered that the liquid had a certain biodegradability and was basically in accordance with the first order kinetics.
【学位授予单位】：辽宁大学
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：X52

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