本文選題：雙子型兩親性離子液體 + 自組裝��； 參考：《山東大學(xué)》2017年碩士論文

【摘要】：針對貴金屬Au分離困難、選擇性差、后處理不充分等問題,本課題將雙子型表面活性劑與離子液體相結(jié)8合,利用雙子型兩親性離子液體構(gòu)建了 W/O型微乳液、反相囊泡、囊泡等分子自組裝體系萃取HC1介質(zhì)中的Au(Ⅲ)。通過電導(dǎo)率、TEM、DLS等手段對構(gòu)建出的自組裝體系進行了表征,采用UV-vis、FT-IR、1H NMR、zeta電位等多種方法分析了三種自組裝體系的萃取機理。對影響萃取的因素,如平衡時間、萃取劑濃度、Au(Ⅲ)液中HC1濃度、Au(Ⅲ)液中鹽濃度等進行了優(yōu)化,采用草酸、NaBH4、水合肼、萃取劑自還原等多種手段反萃得到了單質(zhì)Au。本課題的研究豐富了貴金屬Au的分離方法,為其工業(yè)化萃取中的工藝設(shè)計、設(shè)備選型、條件優(yōu)化等提供了理論依據(jù)。首先,我們構(gòu)建了[C_(14)-4-C_(14)im]Br_2/正庚烷/正戊醇/HC1微乳液自組裝體系用于萃取HC1介質(zhì)中的Au。在該自組裝體系中,[C_(14)-4-C_(14)im]Br_2平鋪在油水界面處,正戊醇穿插其中,兩者合作形成液膜。相比于[C_(14)mim]Br/正庚烷/正戊醇/HC1體系,[C_(14)-4-C_(14)im]Br_2/正庚烷/正戊醇/HC1微乳液體系持水量大、電荷數(shù)量多,穩(wěn)定時間長。UV-vis、FT-IR、1HNMR、斜率法確定了陰離子交換的萃取機理。本研究還對影響萃取的因素(平衡時間、水乳比、醇的體積比、Au(Ⅲ)液中HC1濃度等)進行了優(yōu)化。此外,[C_(14)-4-C_(14)im]Br_2/正庚烷/正戊醇/HC1體系表現(xiàn)出了較高的選擇性:Au的萃取率能達到99.55%,分配比可達3000以上,而其他雜質(zhì)離子Co(Ⅱ)、Cu(Ⅱ)、Fe(Ⅲ)、Ni(Ⅱ)、Sn(Ⅳ)、Al(Ⅲ)萃取率均在7%以下,分配比在1以下。H2C2O4、水合肼、NaBH4用于Au(Ⅲ)的反萃,反萃率接近100%。[C_(14)-4-C_(14)im]Br_2/正庚烷/正戊醇/HC1微乳液體系在萃取Au的方面展現(xiàn)了較好的優(yōu)勢,是一種萃取率高、選擇性好的方法。其次,雙子型兩親性離子液體12-2-12分別與4種陰離子表面活性劑復(fù)配構(gòu)建反相囊泡自組裝體系萃取HCl介質(zhì)中的Au((Ⅲ)。通過調(diào)節(jié)陰陽離子表面活性劑的摩爾比確定了 12-2-12/SDBS為n12-2-12:nSDBS=1:1時最佳萃取體系。在此比例下,12-2-12/SDBS對Au的萃取率最高,并且通過TEM表征發(fā)現(xiàn)形成了反相囊泡。通過改進的等摩爾變換法,確定了 12-2-12/SDBS體系萃取AuCl4-依據(jù)離子交換萃取機理。我們還對Au(Ⅲ)液中HC1濃度、反相囊泡濃度等影響萃取的因素進行了考察。該體系的選擇性相對其他體系來說較高,在相同的萃取實驗條件下Au的萃取率能高達99.26%,而其他雜質(zhì)離子Co(Ⅱ)、Cu(Ⅱ)、Fe(Ⅲ)、Ni(Ⅱ)、Sn(Ⅳ)、Al(Ⅲ)萃取率均在6%以下。利用萃取劑自身可還原的性質(zhì)優(yōu)點,在該體系中得到了球形Au納米顆粒,反萃率可接近100%。該自組裝體系協(xié)同效果好,反萃方法簡單,適用于Au的回收。最后,雙子型兩親性離子液體12-3-12與脫氧膽酸鈉(SDC)復(fù)配得到了雙分子層的囊泡自組裝體系。通過調(diào)節(jié)12-3-12與SDC的摩爾比,可調(diào)控囊泡表面的帶電性質(zhì)。通過動態(tài)光散射與zeta電位可確定,12-3-12與SDC摩爾比為1:2時,囊泡表面帶正電且較為穩(wěn)定,尺寸在240 nm左右,適于HC1介質(zhì)中Au的萃取。與囊泡萃取前相比,萃取后的zeta電位降低了約15 mV左右,TEM照片顯示的微觀結(jié)構(gòu)沒有明顯變化,從而確定了正負電荷相互吸引的萃取機理。本部分還對萃取達到平衡的過程條件進行了優(yōu)化,在最優(yōu)條件下,Au的萃取率可高達99.67%。通過分步萃取與金屬配體離子改進的相互結(jié)合,完成了 Au(Ⅲ)、Cu(Ⅱ)、Fe(Ⅲ)三種金屬的分離。利用NaCl-NH3·H20將Au(Ⅲ)從囊泡上洗脫下來,并通過還原劑還原,得到了樹枝狀A(yù)u納米顆粒。
[Abstract]:In view of the difficulties in separating Au from precious metals, poor selectivity and inadequate post-processing, this topic combines the double sub type surfactants with ionic liquids 8, and constructs a W/O microemulsion, reverse phase vesicles, vesicles and other molecular self-assembly systems to extract Au (III) in the HC1 medium by using a dual type two Pro ionic liquid. By means of conductivity, TEM, DLS and other means UV-vis, FT-IR, 1H NMR, zeta potential were used to analyze the extraction mechanism of the three self-assembly systems. The factors affecting the extraction, such as equilibrium time, concentration of extractant, HC1 concentration in Au (III) solution and the concentration of salt in Au (III) liquid, were optimized, using oxalic acid, NaBH4, hydrazine and extraction. A variety of methods, such as agent self reduction, have been used to reverse the extraction of Au., which has enriched the separation method of precious metal Au. It provides a theoretical basis for the process design, equipment selection and conditions optimization in the industrial extraction. First, we constructed the [C_ (14) -4-C_ (14) im] Br_2/ n-Heptane / pentyl alcohol /HC1 microemulsion self assembly system for the extraction of the Au. In the HC1 medium, Au. in the self-assembly system, [C_ (14) -4-C_ (14) im]Br_2 is spread at the oil and water interface, and n-pentyl alcohol is interspersed and the two forms a liquid film. Compared to [C_ (14) mim]Br/ n-Heptane / n-pentyl alcohol /HC1 system, [C_ (14) -4-C_ (14) im]Br_2/ n-Heptane / n-pentyl alcohol microemulsion system has large water holding capacity, more charge and stable time. The extraction mechanism of anion exchange is determined by long.UV-vis, FT-IR, 1HNMR and slope method. This study also optimizes the factors affecting extraction (equilibrium time, water emulsion ratio, volume ratio of alcohol, HC1 concentration in Au (III)). In addition, [C_ (14) -4-C_ (14) im]Br_2/ n-Heptane / n-pentyl alcohol /HC1 system shows higher selectivity: Au extraction rate energy Up to 99.55%, the distribution ratio can be over 3000, while other impurity ions Co (II), Cu (II), Fe (III), Ni (II), Sn (IV), Al (III) are all under 7%, the distribution ratio is below 1.H2C2O4, hydrazine hydrate, NaBH4 is used in the reverse extraction of Au (III), and the stripping rate is close to 100%.[C_ (14) -4-C_ (14) im]Br_2/ n-Heptane / pentyl alcohol micro emulsion system in extraction It shows a good advantage, which is a high extraction rate and good selectivity. Secondly, double sub type two Pro ionic liquid 12-2-12 is combined with 4 kinds of anionic surfactants to construct the Au ((III) in the HCl medium for the reverse phase vesicle self assembly system. The 12-2-12/SDBS is n12- by adjusting the mole ratio of the cation and cation surfactants. The best extraction system at 2-12:nSDBS=1:1. Under this proportion, the extraction rate of 12-2-12/SDBS to Au is the highest, and the reverse phase vesicles are formed by TEM characterization. Through the improved equimolar transformation method, the mechanism of the extraction of AuCl4- based on the ion exchange extraction is determined by the 12-2-12/SDBS system. We also have the concentration of HC1 in the Au (III) liquid and the concentration of the reverse phase vesicle in the Au (III) liquid. The factors affecting extraction are investigated. The selectivity of this system is higher than that of other systems. The extraction rate of Au can be as high as 99.26% under the same extraction conditions, while other impurity ions Co (II), Cu (II), Fe (III), Ni (II), Sn (IV), and Al (III) are both less than 6%. The properties of the extractant's self reducible property are in this body. Spherical Au nanoparticles were obtained in the system, and the stripping rate was close to 100%.. The synergistic effect of the self-assembled system was good, and the stripping method was simple and suitable for the recovery of Au. Finally, the double molecular two Pro ionic liquid 12-3-12 and sodium deoxycholate (SDC) were mixed with the double molecular layer vesicle self-assembly system. By adjusting the molar ratio of 12-3-12 to SDC, it could be regulated. By dynamic light scattering and zeta potential, it is determined by dynamic light scattering and zeta potential that when the molar ratio of 12-3-12 to SDC is 1:2, the surface of the vesicle is positive and stable, the size is about 240 nm, suitable for the extraction of Au in the HC1 medium. Compared with the vesicle extraction, the zeta potential decreases about 15 mV after the extraction, and the microstructure of the TEM photo shows no microstructure. The extraction mechanism of the mutual attraction between positive and negative charges is determined. This part also optimizes the process conditions for the extraction equilibrium. Under the optimal conditions, the extraction rate of Au can be as high as 99.67%. by the combination of step extraction and metal ligand improvement, and the separation of three metals (III), Cu (II), Fe (III) is completed. NaCl-NH3 (H20) was used to remove Au (III) from the vesicles and the dendritic Au nanoparticles were obtained by reducing agent.
【學(xué)位授予單位】：山東大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2017
【分類號】：TQ028.32

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