本文關(guān)鍵詞： 氧化石墨烯 改性 吸附 類金屬砷 四環(huán)素　出處：《蘇州科技學(xué)院》2015年碩士論文　論文類型：學(xué)位論文

【摘要】：目前地下水中類金屬以及抗生素環(huán)境污染問題越來越嚴(yán)重。針對水體環(huán)境的惡化，對于水中這些污染物的去除已經(jīng)迫在眉睫。對水中類金屬及抗生素的去除常規(guī)處理技術(shù)有：生物法、化學(xué)氧化法和吸附法。其中，吸附法由于具備低成本、易操作、易再生、不易發(fā)生二次污染等優(yōu)勢，被廣泛應(yīng)用。而吸附劑性能是評判吸附效果的重要指標(biāo)。氧化石墨烯作為一種新型吸附劑由于具有獨特的孔隙結(jié)構(gòu)、較大的比表面積、豐富的含氧官能團(tuán)以及能與污染物產(chǎn)生多種相互作用的特性，對水中許多無機(jī)和有機(jī)污染物具有優(yōu)異的吸附能力。 論文根據(jù)氧化石墨烯表面的物理化學(xué)性質(zhì)，通過固相活化和磁性修飾等化學(xué)方法，獲得一系列新型改性氧化石墨烯吸附劑。論文系統(tǒng)研究了改性氧化石墨烯的物理、化學(xué)性質(zhì)等與污染物吸附特性之間的內(nèi)在關(guān)系，并結(jié)合多種表征手段，從微觀上探討了改性氧化石墨烯與單一污染物及多種污染物共存的吸附機(jī)理。 論文主要研究內(nèi)容與結(jié)果如下： （1）通過簡單化學(xué)一步法制備出高含鐵量的磁性氧化石墨烯（MGO），并對水體中的類金屬砷進(jìn)行了吸附研究。 通過高倍透射電鏡掃描（HRTEM）、X射線衍射分析（XRD）、拉曼光譜分析（Raman）、熱分析（TGA-DTA）、X射線光電子能譜分析（XPS）、磁性分析、X射線吸收近邊結(jié)構(gòu)（XANES）等手段表征后得知：MGO具有褶皺的石墨片層結(jié)構(gòu)，鐵顆粒均勻分布在MGO表面上并以α-Fe2O3和Fe3O4形態(tài)存在，且鐵含量高達(dá)51%。此外，根據(jù)μ-XAFS圖譜可以從宏觀和微觀上看到As(V)的分布與鐵的分布是緊密相連的，鐵在整個吸附過程起到極其重要的作用。 （2）研究了磁性氧化石墨烯對水體中三價砷As(III)和五價砷As(V)的吸附性能。 結(jié)果表明：在pH=8的條件下，MGO對三價砷As(III)的最大吸附容量高達(dá)54.18mg/g；在pH=5的條件下，MGO對五價砷As(V)的吸附性能最大高達(dá)26.76mg/g；二者吸附等溫線符合Freundlich模型，動力學(xué)符合二級動力學(xué)，pH、離子強(qiáng)度、共存離子對MGO吸附As(III)和As(V)存在影響。此外，還發(fā)現(xiàn)MGO具備解吸附的能力，具有再次被利用的潛力。 （3）通過KOH活化的方法制備出活化氧化石墨烯（KOH-GO），并在此基礎(chǔ)上，探討了活化的KOH-GO與未活化的氧化石墨烯(GO)與對水中四環(huán)素的吸附性能，并對吸附等溫模型、吸附動力學(xué)模型、pH、離子強(qiáng)度以及在陰陽離子共存條件下的吸附性能進(jìn)行了研究。 結(jié)果表明：根據(jù)對固液比、動力學(xué)和等溫線擬合的分析，可知通過KOH活化的氧化石墨烯對四環(huán)素的吸附性能要優(yōu)于未活化的氧化石墨烯。KOH-GO材料對四環(huán)素的吸附等溫線符合Langmuir模型。GO和KOH-GO對四環(huán)素的最大吸附容量分別為269.36mg/g和525.64mg/g；GO和KOH-GO對四環(huán)素的動力學(xué)吸附符合二級動力學(xué)模型；pH、離子強(qiáng)度對KOH-GO吸附四環(huán)素的存在影響；在陰陽離子存在條件下，陰陽離子均對KOH-GO的吸附產(chǎn)生抑制作用，，同時，陰陽離子還能與復(fù)合污染物之間展開競爭，占據(jù)吸附孔位，從而降低KOH-GO對四環(huán)素的吸附能力。
[Abstract]:The groundwater in the metal and antibiotic pollution is increasingly serious. In view of the deterioration of water environment, for the removal of these pollutants is imminent. The removal of conventional processing technology of water metal and antibiotics: biological method, chemical oxidation and adsorption. The adsorption method with low cost, easy to operate. Easy regeneration, easy occurrence of two pollution and other advantages, is widely used. But the adsorbent performance is an important index of evaluation. The adsorption effect of graphene oxide as a new adsorbent because of its unique structure and pore structure, large surface area, abundant oxygen-containing functional groups and can produce various characteristics of the interaction with pollutants, has excellent adsorption capacity in many inorganic and organic pollutants.
According to the physical and chemical properties of the graphene oxide surface, through the activation and modification of magnetic solid phase chemical method, a series of new modified graphene oxide adsorbent. This thesis studies the physical modification of graphene oxide, chemical properties and the relationship between the pollutant adsorption characteristics, combined with a variety of characterization methods, discussion the adsorption mechanism of coexistence of graphene oxide and single pollutant and various pollutants from microcosmic.
The main contents and results of this paper are as follows:
(1) by a simple chemical step method to produce magnetic graphene oxide with high iron content (MGO), and the metal arsenic in water were studied.
Through high-resolution transmission electron microscope scanning (HRTEM), X ray diffraction (XRD), Raman spectroscopy (Raman), thermal analysis (TGA-DTA), X ray photoelectron spectroscopy (XPS), magnetic analysis, X ray absorption near edge structure (XANES) characterized that: graphite layer structure MGO has the folds of the iron particles uniformly on the surface of MGO and -Fe2O3 and Fe3O4 in alpha form, and the iron content is as high as 51%. in addition, according to the -XAFS of As can be seen from the macro and micro (V) distribution and iron are closely linked, to the extremely important role in the whole the adsorption process.
(2) on the magnetic properties of graphene oxide on the trivalent arsenic in water As (III) As (V) and pentavalent arsenic adsorption properties.
The results show that under the condition of pH=8 MGO As (III) on arsenic. The maximum adsorption capacity of up to 54.18mg/g; under the condition of pH=5 MGO As (V) on arsenic adsorption performance of up to 26.76mg/g; two Freundlich adsorption isotherm model, kinetics of two order kinetics, pH, ion the strength of adsorption of As ions on the coexistence of MGO (III) and As (V) effect. In addition, MGO was also found to have the ability of desorption, has the potential to be utilized again.
(3) by KOH activation of the prepared activated graphene oxide (KOH-GO), and on this basis, discussed the activation of KOH-GO and non activated graphene oxide (GO) and the adsorption of tetracycline in water, and the adsorption isotherm, adsorption kinetics model, pH, ionic strength and adsorption the performance under the condition of coexistence ions were studied.
The results showed that according to the analysis of solid-liquid ratio, kinetics and isotherm fitting, the adsorption properties of graphene oxide by KOH activation of tetracycline to the adsorption isotherms of graphene oxide.KOH-GO material is better than that without activation of tetracycline with Langmuir model.GO and KOH-GO maximum adsorption capacity of tetracycline were 269.36mg/g and 525.64mg/g; GO adsorption kinetics and KOH-GO of tetracycline with two levels of dynamic model; pH, KOH-GO has the effect of ionic strength on adsorption of tetracycline; in the presence of ions produced under the conditions, the adsorption of KOH-GO ions were inhibited at the same time, the competition among the ions can occupy and compound pollutants, adsorption holes, thereby reducing the adsorption capacity of KOH-GO tetracycline.

【學(xué)位授予單位】：蘇州科技學(xué)院
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2015
【分類號】：X523

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