Recent advances in process engineering and upcoming applications of metal-organic frameworks.

Metal-organic frameworks (MOFs) have emerged as an important and unique class of functional crystalline hybrid porous materials in the past two decades. Due to their modular structures and adjustable pore system, such distinctive materials have exhibited remarkable prospects in key applications pertaining to adsorption such as gas storage, gas and liquid separations, and trace impurity removal. Evidently, gaining a better understanding of the structure-property relationship offers great potential for the enhancement of a given associated MOF property either by structural adjustments via isoreticular chemistry or by the design and construction of new MOF structures via the practice of reticular chemistry. Correspondingly, the application of isoreticular chemistry paves the way for the microfine design and structure regulation of presented MOFs. Explicitly, the microfine tuning is mainly based on known MOF platforms, focusing on the modification and/or functionalization of a precise part of the MOF structure or pore system, thus providing an effective approach to produce richer pore systems with enhanced performances from a limited number of MOF platforms. Here, the latest progress in this field is highlighted by emphasizing the differences and connections between various methods. Finally, the challenges together with prospects are also discussed.

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Recent Progress on Microfine Design of Metal-Organic Frameworks: Structure Regulation and Gas Sorption and Separation.

Challenges to developing materials for the transport and storage of hydrogen

Isoreticular principle has been employed to realize a flexible-robust metal-organic framework (MOF) with extended pore structure for the adsorptive removal of trace acetylene from ethylene under ambient conditions. The substitution from zinc(II) to copper(II) of high coordination distortion leads to elongated Cu-F bonds that expand the closed pore cavities in the prototypical MOF from 3.5 × 3.9 × 4.1 to 3.6 × 4.3 × 4.2 A3. The optimal cavity size together with strong binding sites thus endows the new Cu analogue to possess open pore space accessible for trace C2H2 within a substantial low-pressure range while excluding C2H4 molecules, as validated by gas isotherms and single-crystal structure of its partially C2H2-loading phase. In contrast to the Zn prototype, at 298 K and 1.0 bar, the guest-free Cu analogue shows significant C2H2 uptake increase with a total capacity of 4.57 mmol g-1, and gains an over two orders of magnitude jump in IAST selectivity for C2H2/C2H4 (1/99, v/v). These results are higher than the benchmark MOFs for molecular sieving of C2H2/C2H4, leading a high C2H4 productivity of 14.9 mmol g-1. Crystallography studies, molecular modeling, selectivity evaluation, and breakthrough experiments have comprehensively demonstrated this flexible-robust MOF as an efficient adsorbent for C2H2/C2H4 separation.

Optimizing Pore Space for Flexible-Robust Metal-Organic Framework to Boost Trace Acetylene Removal.

Rational design and synthesis of ultramicroporous metal-organic frameworks for gas separation

Industrial processes prominently feature π-acidic gases, and an adsorbent capable of selectively interacting with these molecules could enable important chemical separations1-4. Biological systems use accessible, reducing metal centres to bind and activate weakly π-acidic species, such as N2, through backbonding interactions5-7, and incorporating analogous moieties into a porous material should give rise to a similar adsorption mechanism for these gaseous substrates8. Here, we report a metal-organic framework featuring exposed vanadium(II) centres capable of back-donating electron density to weak π acids to successfully target π acidity for separation applications. This adsorption mechanism, together with a high concentration of available adsorption sites, results in record N2 capacities and selectivities for the removal of N2 from mixtures with CH4, while further enabling olefin/paraffin separations at elevated temperatures. Ultimately, incorporating such π-basic metal centres into porous materials offers a handle for capturing and activating key molecular species within next-generation adsorbents.

/pdf/selective-nitrogen-adsorption-via-backbonding-in-a-metal-1i9xn57mx6.pdf

Selective nitrogen adsorption via backbonding in a metal-organic framework with exposed vanadium sites

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Selective nitrogen adsorption via backbonding in a metal-organic framework with exposed vanadium sites