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金屬—有機(jī)骨架MOF-74系列吸附捕集低濃度二氧化碳的研究

發(fā)布時(shí)間:2018-05-20 02:07

  本文選題:金屬-有機(jī)骨架MOF-74 + CO_2吸附; 參考:《大連理工大學(xué)》2016年碩士論文


【摘要】:各種人類(lèi)活動(dòng)所排放的CO2正通過(guò)溫室效應(yīng)而致使全球變暖,該觀點(diǎn)被廣泛認(rèn)同;厥誄02有利于緩解溫室效應(yīng),實(shí)現(xiàn)資源的優(yōu)化利用。因此,迫切需要開(kāi)發(fā)高效的C02吸附劑。金屬-有機(jī)骨架材料是一種新型多孔材料,其在氣體吸附分離領(lǐng)域表現(xiàn)出巨大的應(yīng)用前景。MOF-74系列材料擁有蜂窩狀網(wǎng)絡(luò)拓?fù)浣Y(jié)構(gòu),其一維六方孔道內(nèi)布滿(mǎn)了裸露的金屬離子吸附位點(diǎn),因而MOF-74對(duì)C02的吸附性能良好。以Mg-MOF-74為吸附劑,考察了原料氣流速及吸附溫度對(duì)C02吸附性能的影響。結(jié)果發(fā)現(xiàn)穿透時(shí)間與吸附量隨著原料氣流速以及吸附溫度的升高而降低。Mg-MOF-74的吸附量隨著溫度的升高而下降,說(shuō)明其對(duì)C02的吸附屬于物理吸附,低溫有利于C02的吸附。本文采用溶劑熱法合成M-MOF-74系列材料(M=Cu, Zn, Co, Mn,Mg, Cd等),探究不同金屬離子合成的MOF-74材料對(duì)CO2吸附能力的差異。在該系列材料中,Cu-MOF-74的吸附效果最差;Mg-MOF-74的吸附效果最佳,吸附性能遠(yuǎn)優(yōu)于其他材料。對(duì)于溶劑熱合成法制備的Mg-MOF-74,采用不同濃度的氨水溶液對(duì)其進(jìn)行浸漬負(fù)載,探究不同濃度的浸漬氨水對(duì)改性后材料的CO2吸附性能的影響規(guī)律。結(jié)果表明氨水負(fù)載能夠有效降低CO2濃度對(duì)材料吸附性能的影響,雖然氨負(fù)載導(dǎo)致材料比表面積減小,但是卻提高了材料的單位表面積吸附量。氨負(fù)載有利于材料對(duì)低濃度CO2的吸附。在改性材料中,0.2mol/L氨水浸漬負(fù)載后的材料的吸附性能要優(yōu)于原材料,其吸附量為200.5mg/g,與未浸漬原材料相比,吸附量提高5.6%。本文在常溫常壓下通過(guò)多組份的自組裝合成出兩種在一維孔道內(nèi)含有-OH官能團(tuán)的MOF-74衍生物,分別命名為Zn(OCA-OH)2(4,4'-bipy)0.5與Zn(MCA-OH)2(4,4'-bipy)0.5。衍生物的結(jié)構(gòu)以及孔道尺寸與MOF-74一致。探究?jī)煞N衍生物以及Zn-MOF-74對(duì)C02吸附能力的差異。結(jié)果表明,Zn(OCA-OH)2(4,4'-bipy)0.5與Zn(MCA-OH)2(4,4'-bipy)0.5材料對(duì)C02尤其是低濃度的C02的吸附性能,均優(yōu)于Zn-MOF-74.并且對(duì)于3%CO2的吸附性能,Zn(MCA-OH)2(4,4'-bipy)0.5要略?xún)?yōu)于Zn(OCA-OH)2(4,4'-bipy)0.5。
[Abstract]:The idea that CO2 emissions from various human activities are warming the globe through Greenhouse Effect is widely accepted. Recovery of CO2 is helpful to alleviate Greenhouse Effect and realize optimal utilization of resources. Therefore, there is an urgent need to develop an efficient adsorbent C _ 2. The metal-organic skeleton material is a new porous material, which shows great application prospect in the field of gas adsorption and separation. The MOF-74 series of materials have honeycomb network topology. One dimensional hexagonal pore is filled with bare metal ion adsorption sites, so MOF-74 has good adsorption performance for CO2. The effects of gas flow rate and adsorption temperature on the adsorption properties of CO2 were investigated with Mg-MOF-74 as adsorbent. The results show that the adsorption capacity of Mg-MOF-74 decreases with the increase of gas velocity and adsorption temperature, indicating that the adsorption of CO2 is physical, and the low temperature is favorable to the adsorption of CO2. In this paper, M-MOF-74 series of materials, such as Cu, Zn, Co, MNO, mg, CD and so on, were synthesized by solvothermal method. The difference of the adsorption ability of MOF-74 materials synthesized by different metal ions to CO2 was investigated. The adsorption efficiency of Cu-MOF-74 is the worst and the adsorption performance of Mg-MOF-74 is much better than that of other materials. For Mg-MOF-74 prepared by solvothermal synthesis, different concentrations of ammonia solution were used to impregnate Mg-MOF-74, and the influence of different concentration of impregnated ammonia on the adsorption properties of modified CO2 was investigated. The results show that ammonia loading can effectively reduce the effect of CO2 concentration on the adsorption performance of the material. Although ammonia loading can reduce the specific surface area of the material, the adsorption amount per unit surface area of the material is increased. Ammonia loading is beneficial to the adsorption of CO2 with low concentration. The adsorption capacity of the modified material was better than that of the raw material after impregnated with ammonia water (0.2 mol / L). The adsorption capacity of the modified material was 200.5mg / g, which was increased by 5.6g / g compared with the unimpregnated raw material. In this paper, two kinds of MOF-74 derivatives containing -OH functional groups in one-dimensional channels have been synthesized by multicomponent self-assembly at room temperature and atmospheric pressure. The two derivatives are named ZnOCA-OHH2OH2OH2OH2OH2OH2OH2OH2OH2OH2OH2OHOH2OH2OH2OH2OH2OH2 and ZnMCA-OHH 2OHH 2OHP2OH2OH2OH2OH@@ The structure and pore size of the derivatives are consistent with that of MOF-74. To explore the difference of adsorption ability of two derivatives and Zn-MOF-74 for CO2. The results show that the adsorptive properties of ZnOCA-OHH2OH2OHH2OHH2OH2OHH2OH2OHH2OH2OH2OH2OH2OH2OH2OH2OH2OH2OH2OH2 and ZnMCA-OHH2OH2OHH2OH2OHH2OH2OHH2 and ZnM@@ Moreover, the adsorption property of 3%CO2 is slightly better than that of OCA-OH2OH2OH2OH2OH2 (OHH2OH2) and 4K4 (4 / 4) -bipyrue (0.5) for the adsorption properties of 3%CO2 (Zn-OCA-OHH ~ (2 +).
【學(xué)位授予單位】:大連理工大學(xué)
【學(xué)位級(jí)別】:碩士
【學(xué)位授予年份】:2016
【分類(lèi)號(hào)】:O647.3

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