Metal-organic frameworks offer a diverse landscape of building blocks to design high performance materials for implications in almost every major industry. With this diversity stems complex crystallization mechanisms with various pathways and intermediates. Crystallization studies have been key to the advancement of countless biological and synthetic systems, with MOFs being no exception. This review provides an overview of the current theories and fundamental chemistry used to decipher MOF crystallization. We then discuss how intrinsic and extrinsic synthetic parameters can be used as tools to modulate the crystallization pathway to produce MOF crystals with finely tuned physical and chemical properties. Experimental and computational methods are provided to guide the probing of MOF crystal formation on the molecular and bulk scale. Lastly, we summarize the recent major advances in the field and our outlook on the exciting future of MOF crystallization. 

Understanding and controlling the nucleation and growth of metal-organic frameworks.

Zeolite catalysts and adsorbents have been an integral part of many commercial processes and are projected to play a significant role in emerging technologies to address the changing energy and environmental landscapes. The ability to rationally design zeolites with tailored properties relies on a fundamental understanding of crystallization pathways to strategically manipulate processes of nucleation and growth. The complexity of zeolite growth media engenders a diversity of crystallization mechanisms that can manifest at different synthesis stages. In this review, we discuss the current understanding of classical and nonclassical pathways associated with the formation of (alumino)silicate zeolites. We begin with a brief overview of zeolite history and seminal advancements, followed by a comprehensive discussion of different classes of zeolite precursors with respect to their methods of assembly and physicochemical properties. The following two sections provide detailed discussions of nucleation and growth pathways wherein we emphasize general trends and highlight specific observations for select zeolite framework types. We then close with conclusions and future outlook to summarize key hypotheses, current knowledge gaps, and potential opportunities to guide zeolite synthesis toward a more exact science.

The Current Understanding of Mechanistic Pathways in Zeolite Crystallization.

With increasing environmental pollution, evolution of efficient adsorption materials has been increasing. Excellent adsorption properties of biomass and metal–organic framework (MOF) composites have received considerable importrance in environmental pollution control. Due to their surface-based functional groups and excellent void structures, biomass materials provide numerous loading sites for MOF as renewable resources. Considering their highly adjustable characteristics, MOFs can direct the adsorption of different pollutants by adjusting pore structures and ionic properties according to the pollutant to be adsorbed. Through synergistic effects, biomass/MOF composite materials can significantly advance adsorption efficiency and capacity of the pollutants by utilizing the respective advantages of biomass-MOF materials. This review covers recent advancements in the application of biomass/MOF composite materials for water restoration, air purification, and electromagnetic radiation adsorption. It discusses the pretreatment and modification of biomass materials, the synthesis and selection of MOFs, and the impact of various pollutant adsorption mechanisms on the performance of these composite materials. This review serves as a significant reference for improving environmental pollution adsorption by exploring the potential of biomass/MOF composite materials. 

Biomass-MOF composites in wastewater treatment, air purification, and electromagnetic radiation adsorption – A review

The immobilization protocol greatly alters the effects of metal phosphate modification on the activity/stability of immobilized lipases.

As one of the main components of solid propellant, ammonium perchlorate (AP) shows slow sluggish decomposition kinetics with unconcentrated heat release. To achieve efficient catalytical decomposition, it is a significant challenge to design reasonable catalyst structure and explore the interaction between catalyst and AP. Herein, a series of porous carbon supported spinel-typed homogeneous heterometallic composites CuxCo3-xO4/C via pyrolysis of MOF-74-Co doped Cu. On basis of precise electronic-structure-tuning through modulating Cu/Co ratio in MOF-74, Cu0.15Co2.85O4/C with 5% Cu-doping featuring oxygen vacancy concentration of 26.25% exhibits the decrease to 261.5 °C with heat release up to 1222.1 J g-1 (456.9 °C and 669.2 J g-1 for pure AP). The detail process of AP accelerated decomposition is approved by TG-DSC-FTIR-MS technique. Density functional theory calculation revealed that in the Cu0.15Co2.85O4/C, the distinctive ability for NH3 catalyzed oxidation assisted with absorption performance of active porous C boosts accelerating AP decomposition. The findings would provide an insight for perceiving and understanding AP catalytic decomposition.

In Situ MOF-74-Pyrolysis-Generated Porous Carbon Supporting Spinel Cu0.15Co2.85O4/C Boosts Ammonium Perchlorate Accelerating Decomposition: Precise Cu Doping Modulating Oxygen Vacancy Concentration.

Two steps must be satisfied to achieve high activity enzyme@MOFs: proper enzyme folding and low MOF crystallinity.

The role of protein folding in prenucleation clusters on the activity of enzyme@metal–organic frameworks

Metal–organic frameworks (MOFs) are a class of porous nanomaterials that have been extensively studied as enzyme immobilization substrates. During in situ immobilization, MOF nucleation is driven by biomolecules with low isoelectric points. Investigation of how biomolecules control MOF self-assembly mechanisms on the molecular level is key to designing nanomaterials with desired physical and chemical properties. Here, we demonstrate how molecular modifications of bovine serum albumin (BSA) with fluorescein isothiocyanate (FITC) can affect MOF crystal size, morphology, and encapsulation efficiency. Final crystal properties are characterized using scanning electron microscopy (SEM), powder X-ray diffraction (PXRD), fluorescent microscopy, and fluorescence spectroscopy. To probe MOF self-assembly, in situ experiments were performed using cryogenic transmission electron microscopy (cryo-TEM) and X-ray diffraction (XRD). Biophysical characterization of BSA and FITC-BSA was performed using ζ potential, mass spectrometry, circular dichroism studies, fluorescence spectroscopy, and Fourier transform infrared (FTIR) spectroscopy. The combined data reveal that protein folding and stability within amorphous precursors are contributing factors in the rate, extent, and mechanism of crystallization. Thus, our results suggest molecular modifications as promising methods for fine-tuning protein@MOFs’ nucleation and growth.

/pdf/role-of-molecular-modification-and-protein-folding-in-the-iewj11ug.pdf

Role of Molecular Modification and Protein Folding in the Nucleation and Growth of Protein–Metal–Organic Frameworks

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Understanding and controlling the nucleation and growth of metal-organic frameworks.

The role of protein folding in prenucleation clusters on the activity of enzyme@metal–organic frameworks

Role of Molecular Modification and Protein Folding in the Nucleation and Growth of Protein–Metal–Organic Frameworks