本文關(guān)鍵詞： 三維 氧化石墨烯 鈾 吸附　出處：《東華理工大學(xué)》2017年碩士論文　論文類型：學(xué)位論文

【摘要】：鈾是核能的主要來(lái)源,也是最有毒的一種重金屬。因此,從廢水中去除和富集鈾十分必要。近年來(lái)石墨烯基材料因其大的比表面積和對(duì)環(huán)境中的污染物表現(xiàn)出優(yōu)良的吸附性能而受到廣泛關(guān)注。其中三維石墨烯基材料又具有多孔和易于回收的優(yōu)點(diǎn),在吸附領(lǐng)域具有潛在的應(yīng)用。本文以氧化石墨烯(GO)為前驅(qū)體,通過(guò)水熱法和冷凍干燥法分別制備出具有三維立體結(jié)構(gòu)的L-精氨酸(L-Arginine)改性氧化石墨烯海綿(L-Ar-GOS)、磺酸化杯[4]芳烴改性氧化石墨烯海綿(S-GOS)和二乙烯三胺五乙酸(DTPA)改性氧化石墨烯海綿(D-GOS)。采用SEM、XRD、FT-IR和XPS等分析手段對(duì)其進(jìn)行分析,并探究其對(duì)鈾(VI)的吸附性能,具體研究?jī)?nèi)容如下:(1)L-Ar-GOS具有交聯(lián)的分層多孔結(jié)構(gòu),在水熱過(guò)程中GO和L-Arginine發(fā)生了交聯(lián)反應(yīng)。L-Ar-GOS對(duì)鈾(VI)的吸附受pH影響很大,但不受離子強(qiáng)度的影響,吸附的最佳pH為5.0;吸附平衡時(shí)間為9 h;吸附過(guò)程可用準(zhǔn)二級(jí)動(dòng)力學(xué)方程來(lái)描述,即其對(duì)鈾(VI)的吸附受化學(xué)作用控制;吸附行為符合Langmuir吸附等溫模型,單分子層吸附量為238.66 mg·g-1。吸附熱力學(xué)函數(shù)值表明,鈾(VI)的吸附是吸熱的和自發(fā)的。吸附/解吸循環(huán)的實(shí)驗(yàn)結(jié)果表明,L-Ar-GOS具有較好的再生、可重復(fù)使用性。另外,L-Ar-GOS對(duì)鈾的選擇性優(yōu)于GO。(2)S-GOS也同樣具有三維互連分層多孔結(jié)構(gòu),在自主裝形成三維石墨烯結(jié)構(gòu)的過(guò)程中,磺酸化杯[4]芳烴起交聯(lián)劑的作用。S-GOS對(duì)鈾(VI)的吸附性能受溶液的初始pH值,吸附時(shí)間、鈾初始濃度和離子強(qiáng)度等因素的影響。吸附鈾(VI)的最佳pH為6.0,在180 min內(nèi)即可達(dá)到吸附平衡。對(duì)鈾(VI)的吸附更適合用準(zhǔn)二級(jí)動(dòng)力學(xué)和Langmuir等溫模型來(lái)描述,吸附過(guò)程受化學(xué)作用主導(dǎo),對(duì)鈾(VI)的單層吸附容量為257.07 mg·g-1。另外,吸附熱力學(xué)結(jié)果表明,S-GOS對(duì)鈾(VI)的吸附是吸熱和自發(fā)的過(guò)程。S-GOS具有良好的再生-可重復(fù)使用性,用1.0 mol·L-1HCl溶液可把大部分鈾(VI)從中解吸出來(lái),吸附/解吸循環(huán)五次后,對(duì)鈾的吸附量?jī)H下降13%。(3)D-GOS的結(jié)構(gòu)同L-Ar-GOS和S-GOS有差異,它具有相對(duì)有序的三維層狀結(jié)構(gòu)。這可能是因?yàn)橹苽銬-GOS時(shí)水熱反應(yīng)是在堿性條件下進(jìn)行的。其對(duì)鈾(VI)的吸附性能受溶液的初始pH值、吸附時(shí)間、鈾初始濃度和溫度等因素的影響,不受離子強(qiáng)度的影響。在pH=6時(shí),其對(duì)鈾(VI)的吸附量最大,為312.1 mg·g-1。吸附240 min即可達(dá)到吸附平衡。吸附動(dòng)力學(xué)結(jié)果表明,準(zhǔn)二級(jí)動(dòng)力學(xué)方程能更準(zhǔn)確地描述其對(duì)鈾(VI)的吸附過(guò)程。吸附行為更符合Langmuir等溫模型,D-GOS對(duì)鈾(VI)的單層吸附量為418.4 mg·g-1,遠(yuǎn)高于GO(192.68 mg·g-1)。熱力學(xué)研究表明,D-GOS對(duì)鈾(VI)的吸附是吸熱和自發(fā)的過(guò)程。另外,D-GOS具有良好的再生和可重復(fù)使用性。
[Abstract]:Uranium is the main source of nuclear energy and the most toxic heavy metal. It is necessary to remove and enrich uranium from waste water. In recent years, graphene based materials have attracted much attention due to their large specific surface area and excellent adsorption performance to pollutants in the environment. Have the advantage of porous and easy to recycle, In this paper, graphene oxide is used as the precursor. The modified graphene oxide sponge L-Ar-GOS, modified by calix sulfonic acid [4] arene, and diethyltriamine pentaacetic acid (DTPA) modified oxygen were prepared by hydrothermal method and freeze-drying method, respectively. The modified graphene oxide sponge L-Ar-GOS was modified by L-Arginine, and the modified graphene sponge S-GOS by calix [4] arene sulfonic acid and DTPA modified by diethyltriamine pentaacetic acid were prepared, respectively. Graphene sponges were analyzed by means of SEMX XRDX FT-IR and XPS. The adsorption properties of Vi for uranium were also investigated. The main contents are as follows: (1) the L-Ar-GOS has cross-linked layered porous structure. During hydrothermal process, the adsorption of uranium Vi by go and L-Arginine is greatly affected by pH, but not by ionic strength. The optimum pH of adsorption is 5.0, the adsorption equilibrium time is 9 h, the adsorption process can be described by quasi-second-order kinetic equation, that is, the adsorption of uranium Vi is controlled by chemical interaction, and the adsorption behavior accords with the Langmuir adsorption isotherm model. The adsorption capacity of monolayer is 238.66 mg 路g-1.The thermodynamic function of adsorption shows that the adsorption of uranium Vi is endothermic and spontaneous. The experimental results of adsorption / desorption cycle show that L-Ar-GOS has good regeneration. Moreover, the selectivity of L-Ar-GOS to uranium is superior to that of GO.(2)S-GOS, and it also has a three-dimensional interconnect layered porous structure. The adsorption properties of calix [4] arene sulfonic acid acting as crosslinker. S-GOS for uranium Vi are determined by the initial pH value of the solution and the adsorption time. The optimum pH of the adsorbed uranium Vi is 6.0, and the adsorption equilibrium can be reached within 180 min. The adsorption of Vi) is more suitable to be described by quasi-second-order kinetics and Langmuir isothermal model. The adsorption process is dominated by chemical action, and the adsorption capacity of the monolayer of uranium Vi is 257.07 mg 路g ~ (-1). In addition, the adsorption thermodynamic results show that the adsorption of uranium Vi by S-GOS is an endothermic and spontaneous process. S-GOS has a good regeneration and reusability, and the adsorption capacity of the monolayer is 257.07 mg 路g ~ (-1). Most of uranium can be desorbed with 1.0 mol 路L ~ (-1) HCl solution. After five cycles of adsorption / desorption, the adsorption capacity of uranium decreased by only 13%. The structure of D-GOS is different from that of L-Ar-GOS and S-GOS. It has a relatively ordered three-dimensional layered structure. This may be due to the hydrothermal reaction in the preparation of D-GOS under alkaline conditions. Its adsorption performance for uranium ion VI is determined by the initial pH value of the solution and the adsorption time. The initial concentration and temperature of uranium are not affected by the ionic strength. At pH = 6:00, the adsorption capacity of Vi is 312.1 mg 路g-1.The adsorption equilibrium can be reached at 240 min. The quasi-second-order kinetic equation can more accurately describe the adsorption process of uranium Vi, and the adsorption behavior is more in line with the Langmuir isothermal model (D-GOS), the monolayer adsorption capacity of Vi is 418.4 mg 路g-1, which is much higher than that of GO(192.68 mg 路g-1.The thermodynamic study shows that the adsorption of Vi to uranium by D-GOS is as follows: 1. Endothermic and spontaneous processes. In addition, D-GOS has good regeneration and reusability.
【學(xué)位授予單位】：東華理工大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2017
【分類號(hào)】：O647.3

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