發(fā)布時(shí)間：2018-08-19 15:32

【摘要】：隨著世界人口的增長(zhǎng)和工業(yè)化水平的提高,人們?cè)趯?duì)能源不斷索取之余,淡水資源這一人類生存必需品也列入各國(guó)爭(zhēng)取的目標(biāo)。在天災(zāi)、人為等因素的影響下,本就儲(chǔ)量很少的淡水資源更加匱乏,非洲、中東地區(qū)尤為嚴(yán)重。我國(guó)部分省市也長(zhǎng)期處于干旱情況,嚴(yán)重地區(qū)已經(jīng)影響到人民的日常飲用水問(wèn)題。解決水資源問(wèn)題迫在眉睫。海水淡化技術(shù)是一種有效獲得淡水資源的工藝,龐大的海水資源為海水淡化提供了足夠的原材料。在二十世紀(jì)中期開(kāi)始使用以來(lái)獲得蓬勃發(fā)展,美國(guó)在1954年建成的海水淡化工廠至今仍在運(yùn)行,源源不斷的提供著日常用水。近年來(lái),海水淡化工業(yè)在中東地區(qū)發(fā)展迅速。蓬勃的石油交易為其提供了大量的研究資金，極度水資源匱乏也迫使當(dāng)?shù)厝送度氪罅咳肆ξ锪?lái)發(fā)展海水淡化這一淡水資源開(kāi)源增量工程。膜蒸餾過(guò)程是一種有效的海水淡化工藝,但是自從1963年被人發(fā)現(xiàn)以來(lái),依舊未完全在工業(yè)中實(shí)施。最近,膜蒸餾膜工程(比如膜的設(shè)計(jì)、制備和膜蒸餾性能測(cè)試)越來(lái)越受到大家的關(guān)注,膜蒸餾技術(shù)發(fā)展迅速。膜蒸餾技術(shù)的關(guān)鍵點(diǎn)就是分離膜材料的研究,尋找一種有效、高效、長(zhǎng)效的分離膜蒸餾膜材料是其發(fā)展的重中之重。本文的宗旨是探索一種能夠穩(wěn)定運(yùn)行的有發(fā)展?jié)摿Φ哪げ牧?在前人的研究中了解到,有機(jī)膜在高溫海水這種環(huán)境下穩(wěn)定性存在問(wèn)題,基于本實(shí)驗(yàn)室的前期研究成果,本文研究重點(diǎn)為高度穩(wěn)定的非氧化物陶瓷膜。分別從陶瓷膜的制備、表面修飾改性、膜蒸餾性能等方面進(jìn)行穩(wěn)定膜蒸餾用陶瓷膜的探索。具體分為以下幾個(gè)部分。第一章介紹當(dāng)前水資源現(xiàn)狀,淡水需求的迫切性；海水淡化工藝的工業(yè)化情況及當(dāng)前海水淡化工藝的缺陷；膜蒸餾技術(shù)的工作原理及阻礙膜蒸餾工藝實(shí)現(xiàn)工業(yè)化的障礙；陶瓷膜的制備及改性方法。最后闡述了整個(gè)研究思路。第二章簡(jiǎn)單介紹了實(shí)驗(yàn)過(guò)程中用到的原料和儀器。第三章介紹兩部分的研究：一是β-Sialon陶瓷纖維管膜的成型和燒結(jié)。使用相轉(zhuǎn)化擠出成型配合燒結(jié)的方法成功獲得纖維管膜,通過(guò)有效漿料中分散劑種類、含量和漿料組分配比獲得穩(wěn)定均一的漿料,并且通過(guò)調(diào)節(jié)燒結(jié)溫度等條件對(duì)陶瓷膜的性質(zhì)進(jìn)行了表征和優(yōu)化；二是氮化硅和β-Sialon陶瓷平板膜制備和表征。使用相轉(zhuǎn)化流延和燒結(jié)的放法制備了氮化硅平板膜。通過(guò)優(yōu)化陶瓷膜的漿料配比、燒結(jié)溫度等條件,成功獲得了高強(qiáng)度和高孔隙率的氮化硅和β-Sialon陶瓷平板膜。第四章介紹陶瓷膜的表面修飾改性,并且對(duì)于已經(jīng)改性好的陶瓷膜進(jìn)行膜蒸餾過(guò)程測(cè)試。陶瓷膜的天然親水性使其不適用于膜蒸餾過(guò)程,其表面改性過(guò)程是提高其使用壽命,使其具有投入工業(yè)生產(chǎn)淡水潛力的一個(gè)關(guān)鍵步驟,主要包括三種改性方法：(1)表面嫁接氟硅烷分子；(2)表面氯硅烷氨解聚合熱解無(wú)機(jī)納米顆粒修飾；(3)表面聚二甲基硅氧烷熱解修飾。三種修飾方法都成功達(dá)到表面改性的目標(biāo),并且都在膜蒸餾過(guò)程中具有分離作用獲得了純水。但是其長(zhǎng)期穩(wěn)定性卻不相同,氟硅烷有機(jī)分子嫁接穩(wěn)定性明顯劣于熱解修飾。第五章在獲得穩(wěn)定實(shí)用的陶瓷膜基礎(chǔ)上盡可能的提高陶瓷膜膜蒸餾的通量。通過(guò)改進(jìn)陶瓷膜的成型過(guò)程,使用石墨犧牲層的雙層流延以及熱壓工藝,有效地提高了陶瓷膜的物質(zhì)傳輸通量,使膜蒸餾過(guò)程中的水通量提高了50%以上。提高了陶瓷膜膜蒸餾過(guò)程的效率,使其工業(yè)化應(yīng)用更進(jìn)一步。第六章介紹氮化硅陶瓷在其作為支撐體材料的一種應(yīng)用,在氮化硅中空纖維管膜的外表面成功合成了一層致密的ZIF-8氣體分離膜,并且證明了其在二氧化碳吸附和分離方面的應(yīng)用。氫氣和二氧化碳的分離因子為11.67。第七章對(duì)本文的工作進(jìn)行了總結(jié),并且指出了工作的不足之處和發(fā)展前景。
[Abstract]:With the growth of world population and the improvement of industrialization level, people are constantly demanding energy, freshwater resources as a human survival necessities are also included in the goals of all countries. The long-term drought has affected people's daily drinking water problems in serious areas. It is urgent to solve the problem of water resources. Seawater desalination technology is an effective way to obtain fresh water resources. The huge seawater resources provide sufficient raw materials for seawater desalination. In recent years, the desalination industry has developed rapidly in the Middle East. The booming oil trade has provided it with a large amount of research funds. The extreme shortage of water resources has also forced the local people to invest a lot of manpower and resources to develop desalination. Membrane distillation process is an effective seawater desalination process, but it has not been fully implemented in industry since it was discovered in 1963. Recently, membrane engineering (such as membrane design, preparation and performance testing of membrane distillation) has attracted more and more attention, and membrane distillation technology has developed rapidly. The key point of distillation technology is the study of membrane materials. It is very important to find an effective, efficient and long-term membrane material for membrane distillation. Based on the previous research results of our laboratory, this paper focuses on highly stable non-oxide ceramic membranes. The preparation of ceramic membranes, surface modification, membrane distillation performance and other aspects of stable membrane distillation ceramic membranes are explored. It is divided into the following parts. The first chapter introduces the current situation of water resources, light. The urgency of water demand, the industrialization of seawater desalination process and the shortcomings of current seawater desalination process, the working principle of membrane distillation technology and the obstacles hindering the industrialization of membrane distillation process, the preparation and modification methods of ceramic membranes are described. Finally, the whole research idea is elaborated. Materials and instrumentation. Chapter 3 introduces the study of two parts: one is the formation and sintering of the membrane of the beta-Sialon ceramic fibers. Fiber membranes are successfully obtained by phase inversion extrusion molding with sintering. The stable and uniform slurry is obtained by the type, content and proportion of dispersants in the effective slurry, and the sintering temperature is adjusted. Silicon nitride and beta-Sialon ceramic flat membranes with high strength and high porosity were successfully obtained by optimizing the slurry ratio and sintering temperature. In the fourth chapter, the surface modification of ceramic membrane is introduced, and the membrane distillation process is tested for the modified ceramic membrane. The natural hydrophilicity of ceramic membrane makes it unsuitable for membrane distillation process. The surface modification process is a key step to improve its service life and make it have the potential of industrial production of fresh water. Suddenly, there are three modification methods: (1) surface grafting of fluorosilane molecules; (2) surface modification of chlorosilane pyrolysis pyrolysis pyrolysis inorganic nanoparticles; (3) surface polydimethylsiloxane pyrolysis modification. All three modification methods have successfully achieved the goal of surface modification, and all of them have the separation effect in the process of membrane distillation to obtain pure water. The grafting stability of fluorosilane is obviously inferior to that of pyrolysis modification. In the fifth chapter, the distillation flux of ceramic membrane is increased as much as possible on the basis of obtaining stable and practical ceramic membrane. The material transfer flux of ceramic membrane was increased by more than 50% during membrane distillation. The efficiency of membrane distillation was improved and the industrial application was further improved. In chapter 6, silicon nitride ceramics was successfully synthesized on the outer surface of silicon nitride hollow fiber tube membrane. The dense ZIF-8 gas separation membrane has been proved to be suitable for carbon dioxide adsorption and separation. The separation factors of hydrogen and carbon dioxide are 11.67. Chapter 7 summarizes the work in this paper and points out the shortcomings and prospects of the work.
【學(xué)位授予單位】：中國(guó)科學(xué)技術(shù)大學(xué)
【學(xué)位級(jí)別】：博士
【學(xué)位授予年份】：2016
【分類號(hào)】：TQ051.893

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