The field of metal–organic frameworks (MOFs) has been incorrectly believed to be purely crystalline. However, non-crystalline MOFs (amorphous MOFs, MOF liquids, and MOF glasses) are starting to emerge as alternative materials, beyond the dictatorial domain of crystalline MOFs. Non-crystalline MOFs present many opportunities, either as novel functional materials themselves, or as vehicles to create other materials. In this extensive Review, we describe the two approaches to preparing amorphous MOFs: (1) the amorphization of crystalline MOFs and (2) the direct synthesis. Special attention is paid to the relationship between preparation method, properties and applications of amorphous MOFs. We also explore the field of MOF liquids and their applications, centering our attention to the phenomenon of melting. Finally, MOF glasses are explained. We highlight the properties and applications of the MOF glasses that are not usually found in crystalline MOFs. New related glass materials such as MOF-blends, flux melted MOFs, MOF crystal-glass composites, MOF and inorganic glass composites, and MOF glass membranes are also reviewed. We conclude the fields of amorphous MOFs, MOF liquids, and MOF glasses by presenting our thoughts on the possible future research directions.

Metal–organic frameworks (MOFs) beyond crystallinity: amorphous MOFs, MOF liquids and MOF glasses

The thermal stability of metal-organic frameworks

Two-dimensional conductive metal-organic frameworks (2D c-MOFs) as an emerging class of multifunctional materials have attracted extensive attention due to their predictable and diverse structures, intrinsic permanent porosity, high charge mobility, and excellent electrical conductivity. Such unique characteristics render them as a promising new platform for electrical related devices. This Minireview highlights the recent key progress of 2D c-MOFs with emphasis on the design strategies, unique electrical properties, and potential applications in electrochemical energy storage. The thorough elucidation of structure-function correlations may offer a guidance for the development of 2D c-MOFs based next-generation energy storage devices.

2D Conductive Metal–Organic Frameworks: An Emerging Platform for Electrochemical Energy Storage

The crystal-liquid-glass phase transition of coordination polymers (CPs) and metal-organic frameworks (MOFs) offers attractive opportunities as a new class of amorphous materials. Unlike conventional glasses, coordination chemistry allows the utilization of rational design concepts to fine-tune the desired properties. Although the glassy state has been rare in CPs/MOFs, it exhibits diverse advantages complementary to their crystalline counterparts, including improved mass transport, optical properties, mechanical properties, and the ability to form grain-boundary-free monoliths. This Review discusses the current achievements in improving the understanding of anomalous phase transitions in CPs/MOFs. We elaborate on the criteria for classifying CP/MOF glasses and comprehensively discuss the three common strategies employed to obtain a glassy state. We include all CP/MOF glass research progress since its inception, discuss the current challenges, and express our perspective on future research directions. 

https://pubs.acs.org/doi/pdf/10.1021/acs.chemrev.1c00826

Metal–Organic Network-Forming Glasses

Lead halide perovskite (LHP) semiconductors show exceptional optoelectronic properties. Barriers for their applications, however, lie in their polymorphism, instability to polar solvents, phase segregation, and susceptibility to the leaching of lead ions. We report a family of scalable composites fabricated through liquid-phase sintering of LHPs and metal-organic framework glasses. The glass acts as a matrix for LHPs, effectively stabilizing nonequilibrium perovskite phases through interfacial interactions. These interactions also passivate LHP surface defects and impart bright, narrow-band photoluminescence with a wide gamut for creating white light-emitting diodes (LEDs). The processable composites show high stability against immersion in water and organic solvents as well as exposure to heat, light, air, and ambient humidity. These properties, together with their lead self-sequestration capability, can enable breakthrough applications for LHPs.

Liquid-phase sintering of lead halide perovskites and metal-organic framework glasses.

The synthesis of four novel crystalline zeolitic imidazolate framework (ZIF) structures using a mixed-ligand approach is reported. The inclusion of both imidazolate and halogenated benzimidazolate-derived linkers leads to glass-forming behavior by all four structures. Melting temperatures are observed to depend on both electronic and steric effects. Solid-state NMR and terahertz (THz)/far-IR demonstrate the presence of a Zn-F bond for fluorinated ZIF glasses. In situ THz/far-IR spectroscopic techniques reveal the dynamic structural properties of crystal, glass, and liquid phases of the halogenated ZIFs, linking the melting behavior of ZIFs to the propensity of the ZnN4 tetrahedra to undergo thermally induced deformation. The inclusion of halogenated ligands within metal-organic framework (MOF) glasses improves their gas-uptake properties.

/pdf/halogenated-metal-organic-framework-glasses-and-liquids-1r49tvkvnr.pdf

Halogenated Metal-Organic Framework Glasses and Liquids.

High temperature superconducting (HTS) tape can be cut and stacked to generate large magnetic fields at cryogenic temperatures after inducing persistent currents in the superconducting layers. A field of 17.7 T was trapped between two stacks of HTS tape at 8 K with no external mechanical reinforcement. 17.6 T could be sustained when warming the stack up to 14 K. A new type of hybrid stack was used consisting of a 12 mm square insert stack embedded inside a larger 34.4 mm diameter stack made from different tape. The magnetic field generated is the largest for any trapped field magnet reported and 30% greater than previously achieved in a stack of HTS tapes. Such stacks are being considered for superconducting motors as rotor field poles where the cryogenic penalty is justified by the increased power to weight ratio. The sample reported can be considered the strongest permanent magnet ever created.

https://iopscience.iop.org/article/10.1088/1361-6668/aad34c/pdf

A trapped field of 17.7 T in a stack of high temperature superconducting tape

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Halogenated Metal-Organic Framework Glasses and Liquids.

A trapped field of 17.7 T in a stack of high temperature superconducting tape

A trapped field of 17.7 T in a stack of high temperature superconducting tape