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用于25℃下二氧化碳吸附的氧化铝-介孔有机硅杂化材料的开发

Development of Alumina⁻Mesoporous Organosilica Hybrid Materials for Carbon Dioxide Adsorption at 25 °C.

作者信息

Gunathilake Chamila, Dassanayake Rohan S, Kalpage Chandrakantha S, Jaroniec Mietek

机构信息

Department of Chemical and Processing Engineering, Faculty of Engineering, University of Peradeniya, Peradeniya 20400, Sri Lanka.

Department of Chemistry and Biochemistry, Kent State University, Kent, OH 44242, USA.

出版信息

Materials (Basel). 2018 Nov 16;11(11):2301. doi: 10.3390/ma11112301.

Abstract

Two series of alumina (Al₂O₃)⁻mesoporous organosilica (Al⁻MO) hybrid materials were synthesized using the co-condensation method in the presence of Pluronic 123 triblock copolymer. The first series of Al⁻MO samples was prepared using aluminum nitrate nanahydrate (Al⁻NN) and aluminum isopropoxide (Al⁻IP) as alumina precursors, and organosilanes with three different bridging groups, namely tris[3-(trimethoxysilyl)propyl]isocyanurate, 1,4-bis(triethoxysilyl)benzene, and bis(triethoxysilyl)ethane. The second series was obtained using the aforementioned precursors in the presence of an amine-containing 3-aminopropyltriethoxysilane to introduce, also, hanging groups. The Al⁻IP-derived mesostructures in the first series showed the well-developed porosity and high specific surface area, as compared to the corresponding mesostructures prepared in the second series with 3-aminopropyltriethoxysilane. The materials obtained from Al⁻NN alumina precursor possessed enlarged mesopores in the range of 3⁻17 nm, whereas the materials synthesized from Al⁻IP alumina precursor displayed relatively low pore widths in the range of 5⁻7 nm. The Al⁻IP-derived materials showed high CO₂ uptakes, due to the enhanced surface area and microporosity in comparison to those observed for the samples of the second series with AP hanging groups. The Al⁻NN- and Al⁻IP-derived samples exhibited the CO₂ uptakes in the range of 0.73⁻1.72 and 1.66⁻2.64 mmol/g at 1 atm pressure whereas, at the same pressure, the Al⁻NN and Al⁻IP-derived samples with 3-aminopropyl hanging groups showed the CO₂ uptakes in the range of 0.72⁻1.51 and 1.70⁻2.33 mmol/g, respectively. These data illustrate that Al⁻MO hybrid materials are potential adsorbents for large-scale CO₂ capture at 25 °C.

摘要

在普朗尼克123三嵌段共聚物存在的情况下,采用共缩聚法合成了两系列氧化铝(Al₂O₃)-介孔有机硅(Al-MO)杂化材料。第一系列的Al-MO样品是使用硝酸铝九水合物(Al-NN)和异丙醇铝(Al-IP)作为氧化铝前驱体,以及带有三种不同桥连基团的有机硅烷制备的,这三种桥连基团分别是三[3-(三甲氧基硅基)丙基]异氰脲酸酯、1,4-双(三乙氧基硅基)苯和双(三乙氧基硅基)乙烷。第二系列是在含胺的3-氨丙基三乙氧基硅烷存在的情况下,使用上述前驱体制备的,目的是引入悬挂基团。与在第二系列中使用3-氨丙基三乙氧基硅烷制备的相应介孔结构相比,第一系列中由Al-IP衍生的介孔结构显示出发达的孔隙率和高比表面积。由Al-NN氧化铝前驱体制备的材料具有3至17纳米范围内扩大的介孔,而由Al-IP氧化铝前驱体制备的材料显示出相对较低的孔径,在5至7纳米范围内。与带有AP悬挂基团的第二系列样品相比,由Al-IP衍生的材料由于表面积和微孔率的增加而表现出较高的CO₂吸附量。在1个大气压下,由Al-NN和Al-IP衍生的样品的CO₂吸附量在0.73至1.72和1.66至2.64 mmol/g范围内,而在相同压力下,带有3-氨丙基悬挂基团的由Al-NN和Al-IP衍生的样品的CO₂吸附量分别在0.72至1.51和1.70至2.33 mmol/g范围内。这些数据表明,Al-MO杂化材料是在25℃下大规模捕获CO₂的潜在吸附剂。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/4669/6266018/48c3cdbb1d31/materials-11-02301-sch001.jpg

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