Complexity behind CO2 capture on NH2-MIL-53(Al).
Complexity behind CO2 capture on NH2-MIL-53(Al).
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DOI：
10.1021/la1045207
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发表时间：
2011-03
期刊：
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通讯作者：
E. Stavitski;E. Pidko;Sarah Couck;Tom Rémy;E. Hensen;B. Weckhuysen;J. Denayer;J. Gascón;F. Kapteijn
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文献类型：
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作者：
E. Stavitski;E. Pidko;Sarah Couck;Tom Rémy;E. Hensen;B. Weckhuysen;J. Denayer;J. Gascón;F. Kapteijn
一些金属有机框架（MOFs）在从不同气体混合物中提取二氧化碳方面表现出优异的性能。其分离能力增强的原因尚不清楚。在此，我们提出了一个相结合的实验和理论研究的氨基官能化的MIL-53（铝），以阐明其不寻常的高效率在CO（2）捕获背后的机制。光谱和DFT的研究指出，只有一个间接的作用，胺部分。与其他氨基官能化的CO（2）吸附剂相比，该结构的CO（2）和NH（2）基团之间没有形成化学键。我们表明，功能化调制的“呼吸”的材料的行为，也就是说，框架的灵活性和它的能力，改变结构后，引入特定的吸附物。不存在与CO（2）的强化学相互作用对于吸附剂的整体性能是非常重要的，因为在非常温和的条件下可以在几分钟内实现完全再生，证明了这种类型的吸附剂用于PSA类系统的高潜力。
Some Metal Organic Frameworks (MOFs) show excellent performance in extracting carbon dioxide from different gas mixtures. The origin of their enhanced separation ability is not clear yet. Herein, we present a combined experimental and theoretical study of the amino-functionalized MIL-53(Al) to elucidate the mechanism behind its unusual high efficiency in CO(2) capture. Spectroscopic and DFT studies point out only an indirect role of amine moieties. In contrast to other amino-functionalized CO(2) sorbents, no chemical bond between CO(2) and the NH(2) groups of the structure is formed. We demonstrate that the functionalization modulates the "breathing" behavior of the material, that is, the flexibility of the framework and its capacity to alter the structure upon the introduction of specific adsorbates. The absence of strong chemical interactions with CO(2) is of high importance for the overall performance of the adsorbent, since full regeneration can be achieved within minutes under very mild conditions, demonstrating the high potential of this type of adsorbents for PSA like systems.