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Probing Metal–Organic Framework Design for Adsorptive Natural Gas Purification
Langmuir ( IF 3.7 ) Pub Date : 2018-06-26 00:00:00 , DOI: 10.1021/acs.langmuir.8b00889 Jayraj N. Joshi 1 , Guanghui Zhu 1 , Jason J. Lee 1 , Eli A. Carter 1 , Christopher W. Jones 1 , Ryan P. Lively 1 , Krista S. Walton 1
Langmuir ( IF 3.7 ) Pub Date : 2018-06-26 00:00:00 , DOI: 10.1021/acs.langmuir.8b00889 Jayraj N. Joshi 1 , Guanghui Zhu 1 , Jason J. Lee 1 , Eli A. Carter 1 , Christopher W. Jones 1 , Ryan P. Lively 1 , Krista S. Walton 1
Affiliation
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Parent and amine-functionalized analogues of metal–organic frameworks (MOFs), UiO-66(Zr), MIL-125(Ti), and MIL-101(Cr), were evaluated for their hydrogen sulfide (H2S) adsorption efficacy and post-exposure acid gas stability. Adsorption experiments were conducted through fixed-bed breakthrough studies utilizing multicomponent 1% H2S/99% CH4 and 1% H2S/10% CO2/89% CH4 natural gas simulant mixtures. Instability of MIL-101(Cr) materials after H2S exposure was discovered through powder X-ray diffraction and porosity measurements following adsorbent pelletization, whereas other materials retained their characteristic properties. Linker-based amine functionalities increased H2S breakthrough times and saturation capacities from their parent MOF analogues. Competitive CO2 adsorption effects were mitigated in mesoporous MIL-101(Cr) and MIL-101–NH2(Cr), in comparison to microporous UiO-66(Zr) and MIL-125(Ti) frameworks. This result suggests that the installation of H2S binding sites in large-pore MOFs could potentially enhance H2S selectivity. In situ Fourier transform infrared measurements in 10% CO2 and 5000 ppm H2S environments suggest that framework hydroxyl and amine moieties serve as H2S physisorption sites. Results from this study elucidate design strategies and stability considerations for engineering MOFs in sour gas purification applications.
中文翻译：
探究吸附性天然气净化的金属有机框架设计
评估了金属有机骨架（MOF），UiO-66（Zr），MIL-125（Ti）和MIL-101（Cr）的母体和胺官能化类似物的硫化氢（H 2 S）吸附功效以及暴露后酸性气体的稳定性。吸附实验是通过使用多组分1％H 2 S / 99％CH 4和1％H 2 S / 10％CO 2 /89％CH 4天然气模拟混合物的固定床穿透研究进行的。H 2之后MIL-101（Cr）材料的不稳定性通过吸附剂造粒后的粉末X射线衍射和孔隙率测量发现了S暴露，而其他材料则保留了它们的特征。基于连接基的胺官能团与其母体MOF类似物相比，增加了H 2 S的穿透时间和饱和能力。与微孔UiO-66（Zr）和MIL-125（Ti）骨架相比，在中孔MIL-101（Cr）和MIL-101-NH 2（Cr）中，竞争性CO 2吸附作用得以减轻。该结果表明，在大孔MOF中安装H 2 S结合位点可以潜在地提高H 2 S的选择性。在10％CO 2和5000 ppm H 2中进行原位傅立叶变换红外测量S环境表明骨架的羟基和胺部分充当H 2 S的物理吸附位点。这项研究的结果阐明了酸性气体净化应用中工程MOF的设计策略和稳定性考虑。
更新日期：2018-06-26
中文翻译：
探究吸附性天然气净化的金属有机框架设计
评估了金属有机骨架（MOF），UiO-66（Zr），MIL-125（Ti）和MIL-101（Cr）的母体和胺官能化类似物的硫化氢（H 2 S）吸附功效以及暴露后酸性气体的稳定性。吸附实验是通过使用多组分1％H 2 S / 99％CH 4和1％H 2 S / 10％CO 2 /89％CH 4天然气模拟混合物的固定床穿透研究进行的。H 2之后MIL-101（Cr）材料的不稳定性通过吸附剂造粒后的粉末X射线衍射和孔隙率测量发现了S暴露，而其他材料则保留了它们的特征。基于连接基的胺官能团与其母体MOF类似物相比，增加了H 2 S的穿透时间和饱和能力。与微孔UiO-66（Zr）和MIL-125（Ti）骨架相比，在中孔MIL-101（Cr）和MIL-101-NH 2（Cr）中，竞争性CO 2吸附作用得以减轻。该结果表明，在大孔MOF中安装H 2 S结合位点可以潜在地提高H 2 S的选择性。在10％CO 2和5000 ppm H 2中进行原位傅立叶变换红外测量S环境表明骨架的羟基和胺部分充当H 2 S的物理吸附位点。这项研究的结果阐明了酸性气体净化应用中工程MOF的设计策略和稳定性考虑。
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