The logic of chemical synthesis

Because of their efficiency, selectivity, and environmental sustainability, there are significant opportunities for enzymes in chemical synthesis and biotechnology. However, as the three-dimensional active structure of enzymes is predominantly maintained by weaker noncovalent interactions, thermal, pH, and chemical stressors can modify or eliminate activity. Metal-organic frameworks (MOFs), which are extended porous network materials assembled by a bottom-up building block approach from metal-based nodes and organic linkers, can be used to afford protection to enzymes. The self-assembled structures of MOFs can be used to encase an enzyme in a process called encapsulation when the MOF is synthesized in the presence of the biomolecule. Alternatively, enzymes can be infiltrated into mesoporous MOF structures or surface bound via covalent or noncovalent processes. Integration of MOF materials and enzymes in this way affords protection and allows the enzyme to maintain activity in challenge conditions (e.g., denaturing agents, elevated temperature, non-native pH, and organic solvents). In addition to forming simple enzyme/MOF biocomposites, other materials can be introduced to the composites to improve recovery or facilitate advanced applications in sensing and fuel cell technology. This review canvasses enzyme protection via encapsulation, pore infiltration, and surface adsorption and summarizes strategies to form multicomponent composites. Also, given that enzyme/MOF biocomposites straddle materials chemistry and enzymology, this review provides an assessment of the characterization methodologies used for MOF-immobilized enzymes and identifies some key parameters to facilitate development of the field.

Metal-Organic Framework-Based Enzyme Biocomposites.

Metal-organic frameworks (MOFs), constructed from organic linkers and inorganic building blocks, are well-known for their high crystallinity, high surface areas, and high component tunability. The stability of MOFs is a key prerequisite for their potential practical applications in areas including storage, separation, catalysis, and biomedicine since it is essential to guarantee the framework integrity during utilization. However, MOFs are prone to destruction under external stimuli, considerably hampering their commercialization. In this Review, we provide an overview of the situations where MOFs undergo destruction due to external stimuli such as chemical, thermal, photolytic, radiolytic, electronic, and mechanical factors and offer guidelines to avoid unwanted degradation happened to the framework. Furthermore, we discuss possible destruction mechanisms and their varying derived products. In particular, we highlight cases that utilize MOF instability to fabricate varying materials including hierarchically porous MOFs, monolayer MOF nanosheets, amorphous MOF liquids and glasses, polymers, metal nanoparticles, metal carbide nanoparticles, and carbon materials. Finally, we provide a perspective on the utilization of MOF destruction to develop advanced materials with a superior hierarchy for various applications.

Destruction of Metal-Organic Frameworks: Positive and Negative Aspects of Stability and Lability.

Metal-organic frameworks (MOFs) are a class of porous materials with immense chemical tunability derived from their organic and inorganic building blocks Presynthetic approaches have been used to construct tailor-made MOFs, but with a rather restricted functional group scope limited by the typical MOF solvothermal synthesis conditions Postsynthetic modification (PSM) of MOFs has matured into an alternative strategy to broaden the functional group scope of MOFs PSM has many incarnations, but two main avenues include (1) covalent PSM, in which the organic linkers of the MOF are modified with a reagent resulting in new functional groups, and (2) coordinative PSM, where organic molecules containing metal ligating groups are introduced onto the inorganic secondary building units (SBUs) of the MOF These methods have evolved from simple efforts to modifying MOFs to demonstrate proof-of-concept, to becoming key synthetic tools for advancing MOFs for a range of emerging applications, including selective gas sorption, catalysis, and drug delivery Moreover, both covalent and coordinative PSM have been used to create hierarchal MOFs, MOF-based porous liquids, and other unusual MOF materials This Outlook highlights recent reports that have extended the scope of PSM in MOFs, some seminal reports that have contributed to the advancement of PSM in MOFs, and our view on future directions of the field

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Postsynthetic Modification: An Enabling Technology for the Advancement of Metal-Organic Frameworks

The authors gratefully acknowledge financial support from the King Abdullah University of Science and Technology (KAUST) and thank V. Guillerm for helpful comments and suggestions.

A reticular chemistry guide for the design of periodic solids

Sequence-defined nucleic acids and proteins with internal monomer sequences and arrangement are vital components in the living world, as a result of billions of years of molecular evolution. These ...

Hierarchy in Metal-Organic Frameworks.

The production of two-dimensional (2D) ultrathin metal-organic framework (MOF) nanosheets with functionalized surfaces is significant for extending their applications. To date, no protocol has been developed yet to solve this problem. Herein, we report a facile, mild, and efficient method to produce 2D monolayer MOF nanosheets with hydrophobic surfaces from layer-pillared 3D MOFs. This approach is based on the replacement of weaker coordinating pillar ligands with stronger coordinating capping ligands with the assistance of a high concentration gradient of the latter. Utilizing this method, the replacement of the 4,4'-bipyridine (bpy) pillars in two cadmium-based layer-pillared MOFs with alkylpyridine derivatives has been achieved, producing 2D MOF nanosheets with monolayer thickness and double-sided hydrophobic surfaces. The resulting hydrophobic 2D MOF nanosheets exhibit good performance for the separation of oil and water.

Facile Exfoliation of 3D Pillared Metal-Organic Frameworks (MOFs) to Produce MOF Nanosheets with Functionalized Surfaces.

Sophisticated chemical processes widely observed in biological cells require precise apportionment regulation of building units, which inspires researchers to develop tailorable architectures with ...

Imprinted Apportionment of Functional Groups in Multivariate Metal-Organic Frameworks

Improving Alkylamine Incorporation in Porous Polymer Networks through Dopant Incorporation

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Hierarchy in Metal-Organic Frameworks.

Facile Exfoliation of 3D Pillared Metal-Organic Frameworks (MOFs) to Produce MOF Nanosheets with Functionalized Surfaces.

Imprinted Apportionment of Functional Groups in Multivariate Metal-Organic Frameworks

Improving Alkylamine Incorporation in Porous Polymer Networks through Dopant Incorporation