【摘要】：新型的多孔碳材料如高比表面積的活性炭和高疏水高吸油性能的大孔炭等由于其獨(dú)特的孔徑結(jié)構(gòu)而具有優(yōu)異的氣體吸附、油品吸收等性能,從而廣泛應(yīng)用于氣體存儲(chǔ)/分離、油水分離/溢油處理等方面。目前,如何高效、環(huán)保、經(jīng)濟(jì)的制備這些碳材料是當(dāng)今科學(xué)界面臨的一大挑戰(zhàn)。本論文以廉價(jià)易得且富含天然類石墨烯結(jié)構(gòu)的石油瀝青為碳源,制備了超高比表面積的瀝青基活性炭、高疏水高吸油性能的大孔炭,研究了他們?cè)跉怏w存儲(chǔ)和油水分離的應(yīng)用,另外,本論文還探討了液相物性對(duì)大孔炭材料吸油性能的影響。以乳化瀝青為碳源,KOH為活化劑,簡(jiǎn)便、高效的一步碳化法制備了以微孔結(jié)構(gòu)為主并含有一定量介孔結(jié)構(gòu)的超高比表面積的活性炭。制備的活性炭表現(xiàn)出優(yōu)越的CO2和CH4吸附能力,樣品AC4比表面積最大,高達(dá)2736m2/g,并且在高壓區(qū)內(nèi)表現(xiàn)出最大氣體吸附量,CO2和CH4分別為19.31mmol/g和9.85mmol/g。樣品AC2表現(xiàn)出低壓區(qū)內(nèi)最大的氣體吸附能力,CO2和CH4分別為3.97mmol/g和4.22mmol/g。本論文以廉價(jià)易得的石油瀝青為碳源,以商品化的密胺海綿為大孔模板,采用一種簡(jiǎn)單、高效的浸漬-碳化的工藝合成了三種高疏水和高親油的瀝青/密胺海綿基復(fù)合大孔炭材料(AMS)。其一,以富含瀝青質(zhì)的脫油瀝青DOA為碳源,制得了大孔炭AMS-d;其二,以瀝青質(zhì)含量較低的石油瀝青為碳源,制得了大孔炭AMS-a;其三,考慮到有機(jī)溶劑的揮發(fā)性,本文使用乳化瀝青為碳源,使整個(gè)制備過程在水相中進(jìn)行,避免了有機(jī)溶劑的使用,綠色、環(huán)保的制備了性能優(yōu)異的大孔炭AMS-e,吸油能力顯著高于以上兩種材料,吸油量可達(dá)自身重量的90~246倍。本論文考察了液相物性對(duì)瀝青/密胺海綿基復(fù)合大孔炭材料吸液性能的影響,結(jié)果證明,有機(jī)溶劑和表面活性劑都可以有效的降低水溶液的表面張力,降低液滴在海綿炭表面的接觸角,實(shí)現(xiàn)海綿炭在混合液中由疏水到吸液的改變。而鹽溶液的加入可以增加水溶液的表面張力和接觸角,不利于海綿炭吸液。因此,海綿炭對(duì)含有機(jī)溶劑和表面活性劑的污水具有良好的吸收效果,對(duì)高鹽廢水難以發(fā)揮作用。
[Abstract]:New porous carbon materials, such as activated carbon with high specific surface area and macroporous carbon with high hydrophobic and high oil absorption properties, have excellent gas adsorption and oil absorption properties due to their unique pore structure, so they are widely used in gas storage / separation. Oil / water separation / oil spill treatment. At present, how to prepare these carbon materials efficiently, environmentally and economically is a major challenge facing the scientific community. In this paper, asphalt-based activated carbon with ultra-high specific surface area and macroporous carbon with high hydrophobic and oil-absorbability were prepared by using petroleum asphalt which is cheap and easy to obtain and rich in natural graphene structure. Their applications in gas storage and oil-water separation were studied. In addition, the effects of liquid phase properties on the oil absorption properties of macroporous carbon materials were also discussed. Using emulsified asphalt as carbon source and Koh as activator, a simple and efficient one-step carbonization method was used to prepare ultrahigh specific surface area activated carbon with microporous structure and a certain amount of mesoporous structure. The prepared activated carbon showed excellent adsorption capacity of CO2 and CH4. The specific surface area of AC4 was the largest, up to 2736 m2 / g, and the maximum gas adsorption capacity of CO2 and CH4 were 19.31mmol/g and 9.85 mmol / g in high pressure region, respectively. The maximum adsorption capacity of CO _ 2 and CH4 was 3.97mmol/g and 4.22 mmol / g, respectively, in the low pressure region of AC2. In this paper, the cheap and easily available petroleum asphalt is used as carbon source, and the commercialized melamine sponge is used as a macroporous template. Three kinds of high hydrophobic and high oleophilic bitumen / melamine sponge based composite macroporous carbon materials (AMS). Were synthesized by high efficiency impregnation and carbonation process. First, macroporous carbon AMS-d; was prepared by using asphaltene rich deoiled asphalt DOA as carbon source. Secondly, macroporous carbon AMS-a; was prepared from asphaltene petroleum asphalt as carbon source, considering the volatility of organic solvents. In this paper, emulsified bitumen is used as carbon source to make the whole preparation process in water phase, avoiding the use of organic solvent, green, environmental protection of the preparation of excellent performance of macroporous carbon AMS-e, oil absorption ability is significantly higher than the above two materials. The oil absorption can reach 90 / 246 times of its own weight. In this paper, the effect of liquid phase properties on the absorbency of asphalt / melamine sponge composite macroporous carbon materials was investigated. The results show that both organic solvents and surfactants can effectively reduce the surface tension of aqueous solution. The contact angle of droplets on the surface of sponge carbon was reduced to change from hydrophobic to absorbent in the mixture. The addition of salt solution can increase the surface tension and contact angle of the solution, which is not conducive to the absorption of carbon sponge. Therefore, sponge carbon has a good absorption effect on wastewater containing organic solvents and surfactants, but it is difficult to play a role in high salt wastewater.
【學(xué)位授予單位】：青島科技大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2017
【分類號(hào)】：X703

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