Centre for Catalysis Research and Innovation & Department of Chemistry and Biomolecular Sciences, University of Ottawa , Ottawa, Ontario K1N 6N5, Canada.
Physical and Computational Science Directorate, Pacific Northwest National Laboratory , Richland, Washington 99354, United States.
J Am Chem Soc. 2017 Feb 8;139(5):1734-1737. doi: 10.1021/jacs.6b10455. Epub 2017 Jan 27.
Metal-organic frameworks (MOFs) have attracted significant attention as solid sorbents in gas separation processes for low-energy postcombustion CO capture. The parasitic energy (PE) has been put forward as a holistic parameter that measures how energy efficient (and therefore cost-effective) the CO capture process will be using the material. In this work, we present a nickel isonicotinate based ultramicroporous MOF, 1 [Ni-(4PyC)·DMF], that has the lowest PE for postcombustion CO capture reported to date. We calculate a PE of 655 kJ/kg CO, which is lower than that of the best performing material previously reported, Mg-MOF-74. Further, 1 exhibits exceptional hydrolytic stability with the CO adsorption isotherm being unchanged following 7 days of steam-treatment (>85% RH) or 6 months of exposure to the atmosphere. The diffusion coefficient of CO in 1 is also 2 orders of magnitude higher than in zeolites currently used in industrial scrubbers. Breakthrough experiments show that 1 only loses 7% of its maximum CO capacity under humid conditions.
金属-有机骨架（MOFs）作为固体吸附剂，在低能耗的燃烧后 CO2 捕集气体分离过程中引起了人们的广泛关注。寄生能（PE）已被提出作为一个整体参数，用于衡量使用该材料的 CO2 捕集过程的能量效率（因此也具有成本效益）。在这项工作中，我们提出了一种基于烟酰基镍的超微孔 MOF，1 [Ni-(4PyC)·DMF]，其在迄今为止报道的燃烧后 CO2 捕集中具有最低的 PE。我们计算出的 PE 为 655 kJ/kg CO，低于之前报道的性能最好的材料 Mg-MOF-74。此外，1 表现出优异的水解稳定性，在经过 7 天的蒸汽处理（>85% RH）或 6 个月的大气暴露后，CO 吸附等温线没有变化。CO 在 1 中的扩散系数也比目前工业洗涤器中使用的沸石高 2 个数量级。突破实验表明，1 在潮湿条件下仅失去其最大 CO 容量的 7%。
