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Densification-Induced Structure Changes in Basolite MOFs: Effect on Low-Pressure CH4 Adsorption

机译:致密化诱导Basolite MOF中的结构变化:对低压CH4吸附的影响

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摘要

Metal-organic frameworks’ (MOFs) adsorption potential is significantly reduced by turning the original powder into pellets or granules, a mandatory step for their use at industrial scale. Pelletization is commonly performed by mechanical compression, which often induces the amorphization or pressure-induced phase transformations. The objective of this work is the rigorous study of the impact of mechanical pressure (55.9, 111.8 and 186.3 MPa) onto three commercial materials (Basolite C300, F300 and A100). Phase transformations were determined by powder X-ray diffraction analysis, whereas morphological changes were followed by nitrogen physisorption. Methane adsorption was studied in an atmospheric fixed bed. Significant crystallinity losses were observed, even at low applied pressures (up to 69.9% for Basolite C300), whereas a structural change occurred to Basolite A100 from orthorhombic to monoclinic phases, with a high cell volume reduction (13.7%). Consequently, adsorption capacities for both methane and nitrogen were largely reduced (up to 53.6% for Basolite C300), being related to morphological changes (surface area losses). Likewise, the high concentration of metallic active centers (Basolite C300), the structural breathing (Basolite A100) and the mesopore-induced formation (Basolite F300) smooth the dramatic loss of capacity of these materials.
机译:通过将原始粉末转变为颗粒或颗粒,金属有机骨架(MOF)的吸附潜力将大大降低,这是工业规模使用它们的必不可少的步骤。造粒通常通过机械压缩进行,这通常会导致非晶化或压力诱导的相变。这项工作的目标是严格研究机械压力(55.9、111.8和186.3 MPa)对三种商业材料(Basolite C300,F300和A100)的影响。通过粉末X射线衍射分析确定相变,而通过氮物理吸附跟随形态变化。在大气固定床中研究了甲烷的吸附。即使在较低的施加压力下(Basolite C300高达69.9%),也观察到了明显的结晶度损失,而Basolite A100的结构发生了从正交晶相到单斜晶相的变化,单元体积减小了很多(13.7%)。因此,甲烷和氮气的吸附能力大大降低(Basolite C300高达53.6%),这与形态变化(表面积损失)有关。同样,高浓度的金属活性中心(Basolite C300),结构呼吸(Basolite A100)和介孔诱导的结构(Basolite F300)使这些材料的容量急剧下降。

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