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      Pyrazine‐interior‐embodied MOF‐74 for selective CO 2 adsorption

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          Abstract

          A series of pyrazine‐interior‐embodied metal–organic framework‐74 composites (py‐MOF‐74) were successfully synthesized by a post‐synthetic vapor modification method. Here, pyrazine molecules occupy the cavity to block the wide pores of MOF‐74, which accentuates the difference in adsorption of a pair of gases on MOFs and consequently reinforces the adsorption selectivity. Different from the “physical confinement” of occupants, the pyrazine molecule with dual “para‐nitrogen” atoms donates one N atom to bond with the open metal ion of MOF‐74 for stability and the other N atom for potential CO 2 trapping. Typically, py‐MOF‐74c with the highest pyrazine insertion ratio displays selectivity greatly superior to that of MOF‐74 in equimolar CO 2/CH 4 (598 vs. 35) and in simulated CO 2/N 2 flue gas (471 vs. 49). Py‐MOF‐74 entities are long‐lived adsorbents, and their CO 2 capacity can be maintained even after storage for 1 year in air. Py‐MOF‐74 also showed a sharp molecular sieve property in fixed‐bed cycle adsorption tests, which implies its great potential in real applications.

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          Selective gas adsorption and separation in metal-organic frameworks.

          Jian-Rong Li, Ryan J Kuppler, Hong-Cai Zhou (2009)
          Adsorptive separation is very important in industry. Generally, the process uses porous solid materials such as zeolites, activated carbons, or silica gels as adsorbents. With an ever increasing need for a more efficient, energy-saving, and environmentally benign procedure for gas separation, adsorbents with tailored structures and tunable surface properties must be found. Metal-organic frameworks (MOFs), constructed by metal-containing nodes connected by organic bridges, are such a new type of porous materials. They are promising candidates as adsorbents for gas separations due to their large surface areas, adjustable pore sizes and controllable properties, as well as acceptable thermal stability. This critical review starts with a brief introduction to gas separation and purification based on selective adsorption, followed by a review of gas selective adsorption in rigid and flexible MOFs. Based on possible mechanisms, selective adsorptions observed in MOFs are classified, and primary relationships between adsorption properties and framework features are analyzed. As a specific example of tailor-made MOFs, mesh-adjustable molecular sieves are emphasized and the underlying working mechanism elucidated. In addition to the experimental aspect, theoretical investigations from adsorption equilibrium to diffusion dynamics via molecular simulations are also briefly reviewed. Furthermore, gas separations in MOFs, including the molecular sieving effect, kinetic separation, the quantum sieving effect for H2/D2 separation, and MOF-based membranes are also summarized (227 references).
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            Metal-organic framework nanosheets in polymer composite materials for gas separation

            Tania Rodenas, Ignacio Luz, Gonzalo Prieto … (2015)
            Composites incorporating two-dimensional nanostructures within polymeric matrices hold potential as functional components for several technologies, including gas separation. Prospectively, employing metal-organic-frameworks (MOFs) as versatile nanofillers would notably broaden the scope of functionalities. However, synthesizing MOFs in the form of free standing nanosheets has proven challenging. We present a bottom-up synthesis strategy for dispersible copper 1,4-benzenedicarboxylate MOF lamellae of micrometer lateral dimensions and nanometer thickness. Incorporating MOF nanosheets into polymer matrices endows the resultant composites with outstanding CO2 separation performance from CO2/CH4 gas mixtures, together with an unusual and highly desired increment in the separation selectivity with pressure. As revealed by tomographic focused-ion-beam scanning-electron-microscopy, the unique separation behaviour stems from a superior occupation of the membrane cross-section by the MOF nanosheets as compared to isotropic crystals, which improves the efficiency of molecular discrimination and eliminates unselective permeation pathways. This approach opens the door to ultrathin MOF-polymer composites for various applications.
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              Colossal cages in zeolitic imidazolate frameworks as selective carbon dioxide reservoirs.

              Bo Wang, Adrien P Côté, Hiroyasu Furukawa … (2008)
              Zeolitic imidazolate frameworks (ZIFs) are porous crystalline materials with tetrahedral networks that resemble those of zeolites: transition metals (Zn, Co) replace tetrahedrally coordinated atoms (for example, Si), and imidazolate links replace oxygen bridges. A striking feature of these materials is that the structure adopted by a given ZIF is determined by link-link interactions, rather than by the structure directing agents used in zeolite synthesis. As a result, systematic variations of linker substituents have yielded many different ZIFs that exhibit known or predicted zeolite topologies. The materials are chemically and thermally stable, yet have the long-sought-after design flexibility offered by functionalized organic links and a high density of transition metal ions. Here we report the synthesis and characterization of two porous ZIFs-ZIF-95 and ZIF-100-with structures of a scale and complexity previously unknown in zeolites. The materials have complex cages that contain up to 264 vertices, and are constructed from as many as 7,524 atoms. As expected from the adsorption selectivity recently documented for other members of this materials family, both ZIFs selectively capture carbon dioxide from several different gas mixtures at room temperature, with ZIF-100 capable of storing 28 litres per litre of material at standard temperature and pressure. These characteristics, combined with their high thermal and chemical stability and ease of fabrication, make ZIFs promising candidate materials for strategies aimed at ameliorating increasing atmospheric carbon dioxide levels.
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                Author and article information

                Contributors
                Journal
                Title: AIChE Journal
                Abbreviated Title: AIChE Journal
                Publisher: Wiley
                ISSN (Print): 0001-1541
                ISSN (Electronic): 1547-5905
                Publication date Created: March 2022
                Publication date (Electronic): November 30 2021
                Publication date (Print): March 2022
                Volume: 68
                Issue: 3
                Affiliations
                [1 ] State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics Chinese Academy of Sciences Dalian China
                [2 ] University of Chinese Academy of Sciences Beijing China
                [3 ] Dalian National Laboratory for Clean Energy Dalian China
                [4 ] School of Materials Science and Engineering, National Institute for Advanced Materials TKL of Metal and Molecule‐Based Material Chemistry, Nankai University Tianjin China
                [5 ] Collaborative Innovation Center of Chemical Science and Engineering (Tianjin) Tianjin China
                Article
                DOI: 10.1002/aic.17528
                SO-VID: 6014fe56-3794-4cca-ae54-95d9b4b4b796
                Copyright © © 2022
                License:

                http://onlinelibrary.wiley.com/termsAndConditions#vor

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