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Highly Robust MOF Polymeric Beads with a Controllable Size for Molecular Separations
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2019-03-21 00:00:00 , DOI: 10.1021/acsami.9b00521 Julien Cousin-Saint-Remi , Stijn Van der Perre , Tiriana Segato 1 , Marie-Paule Delplancke 1 , Steven Goderis , Herman Terryn , Gino Baron , Joeri Denayer
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2019-03-21 00:00:00 , DOI: 10.1021/acsami.9b00521 Julien Cousin-Saint-Remi , Stijn Van der Perre , Tiriana Segato 1 , Marie-Paule Delplancke 1 , Steven Goderis , Herman Terryn , Gino Baron , Joeri Denayer
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Shaping metal–organic frameworks (MOFs) into robust particles with a controllable size is of large interest to the field of adsorption. Therefore, a method is presented here to produce robust MOF beads of different sizes, ranging from 250 μm to several millimeters, which, moreover, preserve the adsorption properties of the unformulated MOF. A simple, mild, and flexible method is demonstrated with the zeolitic imidazolate framework-8 (ZIF-8)/polyvinyl formal composite material. The properties of the composite material are determined via optical imaging, scanning electron microscopy, energy-dispersive X-ray spectroscopy, inductively coupled plasma mass spectrometry, X-ray diffraction, mercury intrusion, argon porosimetry and pycnometry as well as thermogravimetric analysis/differential scanning calorimetry, crush strength tests, and immersion experiments. The proposed method allows the production of resistant particles with a high MOF loading (up to 85 wt %) and remarkable structural and textural properties required for adsorptive separation processes, including a preserved ZIF-8 crystalline structure, microporosity, and a narrow macropore size distribution (1.27 μm average). The particles show a spherical shape with an average aspect ratio of 0.85. The stability tests demonstrated that the composite MOF material exhibits a high mechanical strength (3.09 N/Pc crushing strength) almost equivalent to that of a widely used commercial zeolite material. Furthermore, the material remains stable up to 200 °C and in most solvents. The adsorption properties are explored via static and dynamic experiments in the vapor and liquid phases. The results show that the adsorption capacities are only reduced in proportion to the binder content compared with the pristine material, indicating no binder intrusion in the ZIF-8 pores. Fixed-bed experiments demonstrate the remarkable separation performance in the vapor phase, whereas mass transfer limitations arise in the liquid phase with increasing flow rate. The mass transfer limitations are attributed to the diffusion in the macropores or through the ZIF-8 crystal outer layer.
中文翻译：
具有可控制大小的高度健壮的MOF聚合物珠粒，可用于分子分离
将金属有机框架（MOF）制成尺寸可控的坚固颗粒是吸附领域的一大兴趣。因此，在此提出了一种生产尺寸从250μm到几毫米不等的坚固MOF珠的方法，此外，该方法还保留了未配制的MOF的吸附性能。沸石咪唑酸酯骨架8（ZIF-8）/聚乙烯醇缩甲醛复合材料证明了一种简单，温和且灵活的方法。通过光学成像，扫描电子显微镜，能量色散X射线光谱，感应耦合等离子体质谱法，X射线衍射，压汞，氩气孔隙率法和比重瓶法以及热重分析/差示扫描法确定复合材料的性能。量热法，抗压强度测试，和沉浸实验。所提出的方法可以生产出具有高MOF含量（最高85 wt％）并且具有吸附分离过程所需的显着结构和质地特性的抗性颗粒，包括保留的ZIF-8晶体结构，微孔性和窄的大孔尺寸分布（平均1.27微米）。颗粒呈球形，平均长径比为0.85。稳定性测试表明，复合MOF材料具有很高的机械强度（3.09 N / Pc压碎强度），几乎与广泛使用的商业沸石材料相当。此外，该材料在最高200°C的温度下以及在大多数溶剂中均保持稳定。通过静态和动态实验在气相和液相中探索吸附性能。结果表明，与原始材料相比，吸附能力仅与粘合剂含量成比例降低，表明ZIF-8孔中没有粘合剂侵入。固定床实验表明，在气相中具有显着的分离性能，而随着流速的增加，在液相中会出现传质限制。传质限制归因于在大孔中或通过ZIF-8晶体外层的扩散。
更新日期：2019-03-21
中文翻译：
具有可控制大小的高度健壮的MOF聚合物珠粒，可用于分子分离
将金属有机框架（MOF）制成尺寸可控的坚固颗粒是吸附领域的一大兴趣。因此，在此提出了一种生产尺寸从250μm到几毫米不等的坚固MOF珠的方法，此外，该方法还保留了未配制的MOF的吸附性能。沸石咪唑酸酯骨架8（ZIF-8）/聚乙烯醇缩甲醛复合材料证明了一种简单，温和且灵活的方法。通过光学成像，扫描电子显微镜，能量色散X射线光谱，感应耦合等离子体质谱法，X射线衍射，压汞，氩气孔隙率法和比重瓶法以及热重分析/差示扫描法确定复合材料的性能。量热法，抗压强度测试，和沉浸实验。所提出的方法可以生产出具有高MOF含量（最高85 wt％）并且具有吸附分离过程所需的显着结构和质地特性的抗性颗粒，包括保留的ZIF-8晶体结构，微孔性和窄的大孔尺寸分布（平均1.27微米）。颗粒呈球形，平均长径比为0.85。稳定性测试表明，复合MOF材料具有很高的机械强度（3.09 N / Pc压碎强度），几乎与广泛使用的商业沸石材料相当。此外，该材料在最高200°C的温度下以及在大多数溶剂中均保持稳定。通过静态和动态实验在气相和液相中探索吸附性能。结果表明，与原始材料相比，吸附能力仅与粘合剂含量成比例降低，表明ZIF-8孔中没有粘合剂侵入。固定床实验表明，在气相中具有显着的分离性能，而随着流速的增加，在液相中会出现传质限制。传质限制归因于在大孔中或通过ZIF-8晶体外层的扩散。
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