Cu-BTC@GO復合材料的機械化學合成與成型及其吸附性能研究
發(fā)布時間：2018-08-15 19:45
【摘要】：烷烴、烯烴、芳香烴、有機醇類是油氣的重要組分,這些氣體的揮發(fā)不僅會造成經濟損失,還會對生態(tài)環(huán)境和人類的身體健康造成嚴重危害。因此對油氣的回收利用迫在眉睫。近年來,MOFs材料以其超高的比表面積和孔容、骨架結構多樣化以及易官能化等特點,在VOCs的吸附分離領域得到廣泛應用。本文主要研究Cu-BTC@GO復合材料的機械化學法合成與成型并測定材料的水穩(wěn)定性和VOCs的吸附性能,論文的工作涉及Cu-BTC@GO復合材料的機械化學法制備和表征,材料的水穩(wěn)定性測試,甲醇、乙烯、乙烷、丙烯、丙烷、C5、C6和C7正構烷烴、甲苯和苯十種VOCs組分的吸附性能研究,造粒成型和原位生長法制備Cu-BTC和Cu-BTC@GO復合材料成型體并測定材料對甲醇和苯的吸附等溫線,本文的研究內容屬于環(huán)境科學、化學工程和材料成型領域,具有重要的研究價值和工業(yè)應用背景。本文研究了合成條件包括球磨參數(shù)和純化試劑對Cu-BTC@GO復合材料的比表面積和孔隙結構的影響。研究表明:球磨珠數(shù)量為3顆,球磨時間為60 min,球磨轉速為1100 r/min,活化試劑為乙醇時,可合成大比表面積和高孔容的Cu-BTC@GO復合材料,其BET比表面積最高可達1362.0 m2/g,總孔容為0.8536 cm3/g,微孔孔容為0.4397 cm3/g。本文研究了氧化石墨烯復合對Cu-BTC@GO復合材料水穩(wěn)定性的影響。研究表明:Cu-BTC在水中浸泡5 h后,材料的XRD特征峰的強度明顯減弱,BET比表面積下降65%,中孔結構幾乎完全消失,微孔孔容減少62%,晶體表面出現(xiàn)很多細小的棒狀結構。浸泡10 h后,材料的BET比表面積和孔容幾乎完全消失,晶體表面出現(xiàn)大量棒狀結構。Cu-BTC@GO復合材料在水中浸泡10 h后BET比表面積仍在1000 m2/g以上,微孔孔容在0.4 cm3/g以上,Cu-BTC@GO復合材料的水穩(wěn)定性大大高于Cu-BTC。本文研究了Cu-BTC@GO對十種VOCs組分的吸附性能。研究表明:Cu-BTC@GO對這些VOCs組分具有很高的吸附性能,吸附量均大于本文和水熱法制備的Cu-BTC的吸附量,遠高于傳統(tǒng)吸附劑如分子篩、沸石等的吸附量;Cu-BTC@GO對丙烯和乙烯的吸附選擇性分別達到4.5和5.46,對C2~C3烷烴烯烴混合氣體具有很好的分離效果。本文研究了造粒成型和原位生長法制備Cu-BTC和Cu-BTC@GO成型體,并測定了甲醇和苯的吸附等溫線。研究表明:Cu-BTC@GO粒料的BET比表面積最高可達1059.2 m2/g,與成型前的粉末材料相比僅下降2.8%,保留了完整的MOFs粉末的晶體結構和熱穩(wěn)定性能,Cu-BTC@GO粒料對甲醇和苯的飽和吸附量分別為7.27 mmol/g和6.23 mmol/g,相比Cu-BTC@GO粉料,飽和吸附量分別下降12%和26.7%;Cu-BTC粒料對甲醇和苯的飽和吸附量分別為4.85 mmol/g和2.47 mmol/g,相比Cu-BTC粉料,飽和吸附量分別下降70%和58.8%,Cu-BTC@GO粒料對甲醇和苯均有良好的吸附性能。通過原位生長法可將Cu-BTC浸漬在堇青石表面,得到Cu-BTC@堇青石成型體,從SEM上可以看到堇青石表面生長了許多Cu-BTC晶體。
[Abstract]:Alkanes, olefins, aromatic hydrocarbons and organic alcohols are important components of oil and gas. The volatilization of these gases will not only cause economic losses, but also cause serious harm to the ecological environment and human health. Therefore, the recovery and utilization of oil and gas is imminent. In recent years, MOFs have been widely used in the field of adsorption and separation of VOCs due to their high specific surface area and pore volume, diverse skeleton structure and easy functionalization. In this paper, the synthesis and molding of Cu-BTC@GO composites by mechanochemical method and the determination of their water stability and the adsorption properties of VOCs were studied. Study on adsorption properties of ten VOCs components of ethylene, ethane, propylene, propane C _ 5N _ 6 and C _ 7 n-alkanes, toluene and benzene, granulation and in-situ growth method to prepare Cu-BTC and Cu-BTC@GO composite molds and determine the adsorption isotherms of methanol and benzene. The research content of this paper belongs to the field of environmental science, chemical engineering and material forming, which has important research value and industrial application background. The effects of synthesis conditions including ball milling parameters and purification reagents on the specific surface area and pore structure of Cu-BTC@GO composites were studied. The results showed that the Cu-BTC@GO composites with large specific surface area and high pore volume could be synthesized when the number of ball balls was 3, the milling time was 60 minutes, the rotational speed of ball milling was 1100 r / min, and the activation reagent was ethanol. The highest specific surface area of BET is 1362.0 m2 / g, the total pore volume is 0.8536 cm 3 / g, and the micropore volume is 0.4397 cm 3 / g. The effect of graphene oxide composite on the water stability of Cu-BTC@GO composites was studied in this paper. The results show that the specific surface area of XRD decreases by 65%, the mesoporous structure almost disappears, the micropore volume decreases 62%, and many fine rod-like structures appear on the crystal surface after being immersed in water for 5 h. After immersion for 10 h, the BET specific surface area and pore volume of the composites almost disappeared, and a large number of rod-like structure. Cu-BTCCGO composites were immersed in water for 10 hours. The specific surface area of BET was still over 1000 m2 / g. The water stability of Cu-BTCCgo composites with micropore volume above 0.4 cm3/g is much higher than that of Cu-BTC-based composites. In this paper, the adsorption properties of ten VOCs components by Cu-BTC@GO have been studied. The results showed that the adsorptive capacity of VOCs components was higher than that of Cu-BTC prepared by hydrothermal method and higher than that of traditional adsorbents such as molecular sieve, and the adsorption capacity of Cu-BTC was much higher than that of Cu-BTC prepared by hydrothermal method, and the adsorption capacity of these components was much higher than that of traditional adsorbents such as molecular sieve. The adsorption selectivity of Cu-BTCgo on propylene and ethylene reached 4.5 and 5.46 respectively, which showed good separation effect on C2~C3 alkenes. In this paper, Cu-BTC and Cu-BTC@GO molds were prepared by granulation and in situ growth, and the adsorption isotherms of methanol and benzene were determined. The results show that the BET specific surface area of the w / Cu-BTCCgo particles can reach 1059.2 m2 / g, which is only 2.8m / g lower than that of the powder materials before molding. The crystal structure and thermal stability of the whole MOFs powder are preserved. The saturated adsorption of methanol and benzene by Cu-BTCCgo particles are respectively. 7.27 mmol/g and 6.23 mmol / g, compared to Cu-BTC@GO powder, The saturated adsorption capacity of Cu-BTC particles for methanol and benzene was 4.85 mmol/g and 2.47 mmol / g, respectively. Compared with Cu-BTC powder, the saturated adsorption capacity of Cu-BTC particles decreased by 70% and 58.8% respectively. Cu-BTC can be impregnated on cordierite surface by in situ growth method, and Cu-BTC @ cordierite forming body can be obtained. A lot of Cu-BTC crystals can be seen on the surface of cordierite from SEM.
【學位授予單位】：華南理工大學
【學位級別】：碩士
【學位授予年份】：2015
【分類號】：O647.3;TB33
本文編號：2185222
[Abstract]:Alkanes, olefins, aromatic hydrocarbons and organic alcohols are important components of oil and gas. The volatilization of these gases will not only cause economic losses, but also cause serious harm to the ecological environment and human health. Therefore, the recovery and utilization of oil and gas is imminent. In recent years, MOFs have been widely used in the field of adsorption and separation of VOCs due to their high specific surface area and pore volume, diverse skeleton structure and easy functionalization. In this paper, the synthesis and molding of Cu-BTC@GO composites by mechanochemical method and the determination of their water stability and the adsorption properties of VOCs were studied. Study on adsorption properties of ten VOCs components of ethylene, ethane, propylene, propane C _ 5N _ 6 and C _ 7 n-alkanes, toluene and benzene, granulation and in-situ growth method to prepare Cu-BTC and Cu-BTC@GO composite molds and determine the adsorption isotherms of methanol and benzene. The research content of this paper belongs to the field of environmental science, chemical engineering and material forming, which has important research value and industrial application background. The effects of synthesis conditions including ball milling parameters and purification reagents on the specific surface area and pore structure of Cu-BTC@GO composites were studied. The results showed that the Cu-BTC@GO composites with large specific surface area and high pore volume could be synthesized when the number of ball balls was 3, the milling time was 60 minutes, the rotational speed of ball milling was 1100 r / min, and the activation reagent was ethanol. The highest specific surface area of BET is 1362.0 m2 / g, the total pore volume is 0.8536 cm 3 / g, and the micropore volume is 0.4397 cm 3 / g. The effect of graphene oxide composite on the water stability of Cu-BTC@GO composites was studied in this paper. The results show that the specific surface area of XRD decreases by 65%, the mesoporous structure almost disappears, the micropore volume decreases 62%, and many fine rod-like structures appear on the crystal surface after being immersed in water for 5 h. After immersion for 10 h, the BET specific surface area and pore volume of the composites almost disappeared, and a large number of rod-like structure. Cu-BTCCGO composites were immersed in water for 10 hours. The specific surface area of BET was still over 1000 m2 / g. The water stability of Cu-BTCCgo composites with micropore volume above 0.4 cm3/g is much higher than that of Cu-BTC-based composites. In this paper, the adsorption properties of ten VOCs components by Cu-BTC@GO have been studied. The results showed that the adsorptive capacity of VOCs components was higher than that of Cu-BTC prepared by hydrothermal method and higher than that of traditional adsorbents such as molecular sieve, and the adsorption capacity of Cu-BTC was much higher than that of Cu-BTC prepared by hydrothermal method, and the adsorption capacity of these components was much higher than that of traditional adsorbents such as molecular sieve. The adsorption selectivity of Cu-BTCgo on propylene and ethylene reached 4.5 and 5.46 respectively, which showed good separation effect on C2~C3 alkenes. In this paper, Cu-BTC and Cu-BTC@GO molds were prepared by granulation and in situ growth, and the adsorption isotherms of methanol and benzene were determined. The results show that the BET specific surface area of the w / Cu-BTCCgo particles can reach 1059.2 m2 / g, which is only 2.8m / g lower than that of the powder materials before molding. The crystal structure and thermal stability of the whole MOFs powder are preserved. The saturated adsorption of methanol and benzene by Cu-BTCCgo particles are respectively. 7.27 mmol/g and 6.23 mmol / g, compared to Cu-BTC@GO powder, The saturated adsorption capacity of Cu-BTC particles for methanol and benzene was 4.85 mmol/g and 2.47 mmol / g, respectively. Compared with Cu-BTC powder, the saturated adsorption capacity of Cu-BTC particles decreased by 70% and 58.8% respectively. Cu-BTC can be impregnated on cordierite surface by in situ growth method, and Cu-BTC @ cordierite forming body can be obtained. A lot of Cu-BTC crystals can be seen on the surface of cordierite from SEM.
【學位授予單位】：華南理工大學
【學位級別】：碩士
【學位授予年份】：2015
【分類號】：O647.3;TB33
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