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整体支撑的胺功能化 Mg(dobpdc) 吸附剂用于 CO 捕获。

Monolith-Supported Amine-Functionalized Mg(dobpdc) Adsorbents for CO Capture.

机构信息

School of Chemical & Biomolecular Engineering, Georgia Institute of Technology , 311 Ferst Drive, Atlanta, Georgia 30332, United States.

出版信息

ACS Appl Mater Interfaces. 2017 May 24;9(20):17042-17050. doi: 10.1021/acsami.7b02035. Epub 2017 May 9.

Abstract

The potential of using an amine-functionalized metal organic framework (MOF), mmen-M(dobpdc) (M = Mg and Mn), supported on a structured monolith contactor for CO capture from simulated flue gas is explored. The stability of the unsupported MOF powders under humid conditions is explored using nitrogen physisorption and X-ray diffraction analysis before and after exposure to humidity. Based on its superior stability to humidity, mmen-Mg(dobpdc) is selected for further growth on a honeycomb cordierite monolith that is wash-coated with α-alumina. A simple approach for the synthesis of an Mg(dobpdc) MOF film using MgO nanoparticles as the metal precursor is used. Rapid drying of MgO on the monolith surface followed by a hydrothermal treatment is demonstrated to allow for the synthesis of a MOF film with good crystallite density and favorable orientation of the MOF crystals. The CO adsorption behavior of the monolith-supported mmen-Mg(dobpdc) material is assessed using 10% CO in helium and 100% CO, demonstrating a CO uptake of 2.37 and 2.88 mmol/g, respectively. Excellent cyclic adsorption/desorption performance over multiple cycles is also observed. This is one of the first examples of the deployment of an advanced MOF adsorbent in a scalable, low-pressure drop gas-solid contactor. Such demonstrations are critical to the practical application of MOF materials in adsorptive gas separations, as structured contactors have many practical advantages over packed or fluidized beds.

摘要

探索了在结构化整体式接触器上负载胺功能化金属有机骨架(MOF)mmen-M(dobpdc)(M = Mg 和 Mn),以用于从模拟烟道气中捕获 CO。在暴露于湿度之前和之后,使用氮气物理吸附和 X 射线衍射分析来探索无载体 MOF 粉末在潮湿条件下的稳定性。基于其对湿度的优异稳定性,选择 mmen-Mg(dobpdc)进一步在蜂窝堇青石整体式上生长,堇青石整体式用α-氧化铝进行了涂覆。使用 MgO 纳米颗粒作为金属前体制备了 Mg(dobpdc)MOF 膜的简单方法。在整体式表面上快速干燥 MgO,然后进行水热处理,证明可以合成具有良好结晶密度和 MOF 晶体有利取向的 MOF 膜。使用氦气中的 10%CO 和 100%CO 评估了负载在整体式上的 mmen-Mg(dobpdc)材料的 CO 吸附行为,分别证明了 2.37 和 2.88 mmol/g 的 CO 吸收量。还观察到多次循环的出色循环吸附/解吸性能。这是将先进的 MOF 吸附剂应用于可扩展、低压降气固接触器的首批实例之一。这种演示对于 MOF 材料在吸附性气体分离中的实际应用至关重要,因为结构化接触器相对于填充床或流化床具有许多实际优势。

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