The melting phenomenon in metal-organic frameworks (MOFs) has been recognised as one of the fourth generation MOF paradigm behaviours. Molten MOFs have high processibility for producing mechanically robust glassy MOF macrostructures, and they also offer highly tunable interfacial characteristics when combined with other types of functional materials, such as crystalline MOFs, inorganic glass and metal halide perovskites. As a result, MOF glass composites have emerged as a family of functional materials with dynamic properties and hierarchical structural control. These nanocomposites allow for sophisticated materials science studies as well as the fabrication of next-generation separation, catalysis, optical, and biomedical devices. Here, we review the approaches for designing, fabricating, and characterising MOF glass composites. We determine the key application opportunities enabled by these composites and explore the remaining hurdles, such as improving thermal and chemical compatibility, regulating interfacial properties, and scalability.

Metal-organic framework glass composites.

New opportunities and challenges associated with amorphous MOFs for energy storage. 

Amorphous MOFs for next generation supercapacitors and batteries

The detailed understanding of the microscopic structure of amorphous phases of metal-organic frameworks (MOFs) remains a widely open question: characterization of these systems is very difficult, both from the experimental...

Machine Learning Interatomic Potentials for Amorphous Zeolitic Imidazolate Frameworks

Defect engineering has developed over the last decade to become an inimitable tool with which to shape Metal-Organic Framework (MOF) chemistry; part of an evolution in the perception of MOFs from perfect, rigid matrices to dynamic materials whose chemistry is shaped as much by imperfections as it is by their molecular components. However, challenges in defect characterisation and reproducibility persist and, coupled with an as-yet opaque role for synthetic parameters in defect formation, deny chemists the full potential of reticular synthesis. Herein we map the broad implications defects have on MOF properties, highlight key challenges and explore the remarkable ways imperfection enriches MOF chemistry. Engineering defects into metal-organic frameworks is a strategy to grant additional properties but there are still challenges with their reproducibility. Here, this Perspective presents the benefits of defects in metal-organic framework properties and key challenges in the field. 

Benefits and complexity of defects in metal-organic frameworks

Disordered and defective semi-crystalline Fe-MOF as a high-power and high-energy anode material for lithium-ion batteries

Abstract Intentionally disordered metal–organic frameworks (MOFs) display rich functional behaviour. However, the characterisation of their atomic structures remains incredibly challenging. X-ray pair distribution function techniques have been pivotal in determining their average local structure but are largely insensitive to spatial variations in the structure. Fe-BTC (BTC = 1,3,5-benzenetricarboxylate) is a nanocomposite MOF, known for its catalytic properties, comprising crystalline nanoparticles and an amorphous matrix. Here, we use scanning electron diffraction to first map the crystalline and amorphous components to evaluate domain size and then to carry out electron pair distribution function analysis to probe the spatially separated atomic structure of the amorphous matrix. Further Bragg scattering analysis reveals systematic orientational disorder within Fe-BTC’s nanocrystallites, showing over 10° of continuous lattice rotation across single particles. Finally, we identify candidate unit cells for the crystalline component. These independent structural analyses quantify disorder in Fe-BTC at the critical length scale for engineering composite MOF materials. 

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Mapping nanocrystalline disorder within an amorphous metal–organic framework

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Mapping nanocrystalline disorder within an amorphous metal–organic framework