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Enhanced CO2 adsorption on Al-MIL-53 by introducing hydroxyl groups into the framework

机译:通过将羟基引入框架中,增强了Al-MIL-53上的CO 2吸附

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摘要

A series of hydroxyl functionalized Al-MIL-53 materials (Al-MIL-53-OHx) containing varying hydroxyl molar ratios (x = 25%, 50%, 75%, and 100%) were synthesized via a mixed-linker approach, wherein x denotes the molar ratio of 2,5-dihydroxy terephthalic acid:(2,5-dihydroxy terephthalic acid + terephthalic acid). All Al-MIL-53-OHs exhibited an identical structure to that of Al-MIL-53. The thermal stability of Al-MIL-53 decreased after introducing hydroxyl groups. The hydroxyl functionalized Al-MIL-53 containing 25 mol% and 50 mol% of hydroxyl group showed higher surface areas (S-BET = 1270 and 1260 m(2) g(-1) for Al-MIL-53-OH25 and Al-MIL-53-OH50, respectively) than that of Al-MIL-53 (S-BET = 819 m(2) g(-1)). A further increase in the OH groups (75 mol% and 100 mol%) led to dramatical compromise of the framework. The presence of hydroxyl groups affected not only the CO2 adsorption capability but also the 'breathing effect' of MIL-53 resulting from the intraframework interaction. The CO2 adsorption capacities of Al-MIL-53-OH25 and Al-MIL-53-OH50 at 1 bar at 25 degrees C were 8.5 and 8.3 wt%, respectively, which are about 19% higher than that of Al-MIL-53 under the identical conditions. Moreover, pronounced improvement in CO2 adsorption was observed below 0.2 bar, especially for Al-MIL-53-OH25 (5.5 wt% for Al-MIL-53-OH25 vs. 1.7 wt% for Al-MIL-53). This behavior is due likely to the enhanced isosteric heat of CO2 adsorption. The hydroxyl group plays a positive role in the CO2 adsorption performance of Al-MIL-53, which is comparable to amino groups. Al-MIL-53-OHx (x = 75 and 100) displayed lower CO2 adsorption capacities despite the higher isosteric heat of CO2 adsorption, which might be due to the blocked pores in the presence of dense hydroxyl groups.
机译:一系列的羟基官能化含不同羟基摩尔比Al-MIL-53材料(铝MIL​​-53-OHX)(X = 25%,50%,75%和100%),通过混合体方法合成,其中x表示的2,5-二羟基对苯二甲酸的摩尔比:(2,5-二羟基对苯二甲酸+对苯二甲酸)。所有的Al-MIL-53-OHS表现出相同的结构,以使Al-MIL-53的。的Al-MIL-53的热稳定性引入羟基后下降。羟基官能化的Al-MIL-53含有25摩尔%和50摩尔%的羟基表现出较高的表面积(S-BET = 1270和1260米(2)克(-1)的Al-MIL-53-OH25和Al -MIL-53-OH50,分别地)比的铝MIL-53(S-BET =819米(2)克(-1))。进一步增加在OH基团(75摩尔%,100摩尔%)导致框架的显着的折衷。羟基基团的存在的影响不仅CO 2吸附能力,而且MIL-53的“呼吸效应”从intraframework相互作用而产生的。在1巴的Al-MIL-53-OH25和Al-MIL-53-OH50的CO 2吸附能力,在25℃下分别为8.5和8.3%(重量),分别,它们是约19%比Al-MIL-53的高在相同的条件下。此外,观察到的CO 2吸附着的改进低于0.2巴,尤其是对铝MIL-53-OH25(5.5%(重量)为的Al-MIL-53-OH25与1.7%(重量)为的Al-MIL-53)。这种现象是由于容易吸附CO2的增加等量的热量。羟基起着的Al-MIL-53,这相当于氨基的CO 2吸附性能的积极作用。尽管CO 2吸附的较高等量吸附热,这可能是由于在密羟基基团的存在堵塞毛孔的Al-MIL-53-OHX(X = 75和100)显示较低的CO 2吸附能力。

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  • 来源
    《RSC Advances》 |2016年第60期|共6页
  • 作者单位

    Shanghai Univ Elect Power Sch Math &

    Phys Shanghai 200090 Peoples R China;

    Shanghai Univ Elect Power Sch Math &

    Phys Shanghai 200090 Peoples R China;

    E China Normal Univ Sch Chem &

    Mol Engn Shanghai 200062 Peoples R China;

    Shanghai Univ Elect Power Sch Math &

    Phys Shanghai 200090 Peoples R China;

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  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类 化学;
  • 关键词

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