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Synthesis and Characterization of Functionalized Metal-organic Frameworks

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Structure sensitivity in gas sorption and conversion on metal-organic frameworks.

Guusje Delen¹, Matteo Monai¹, Katarina Stančiaková¹

¹Inorganic Chemistry and Catalysis, Institute for Sustainable and Circular Chemistry and Debye Institute for Nanomaterials Science, Utrecht University, Utrecht, The Netherlands.

Nature Communications

|January 9, 2023

Summary

This study reveals how formaldehyde adsorbs and converts on ZIF-8 crystal surfaces. In situ Photo-induced Force Microscopy (PiFM) and Density Functional Theory (DFT) show external surface termination dictates these processes, not defects.

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Area of Science:

Materials Science
Surface Chemistry
Catalysis

Background:

Catalytic processes rely on gas molecule interactions with functional materials.
Gaseous molecule sorption and conversion often occur at specific surface sites.

Purpose of the Study:

To investigate site-specific formaldehyde sorption and conversion on ZIF-8 microcrystals.
To understand the role of external surface termination and defects in these processes.
To demonstrate the utility of in situ Photo-induced Force Microscopy (PiFM) for studying porous materials.

Main Methods:

In situ Photo-induced Force Microscopy (PiFM) for nanoscale imaging.
Density Functional Theory (DFT) calculations for theoretical analysis.
Study of well-defined faceted ZIF-8 microcrystals.

Main Results:

Formaldehyde preferentially adsorbs on high-index planes of ZIF-8.
In situ PiFM visualized unsaturated nanodomains with enhanced sorption.
Structure-sensitive formaldehyde conversion via methoxy and formate pathways was observed on defective ZIF-8.
External surface termination, not defect concentration, primarily influenced sorption and conversion.

Conclusions:

Specific atomic arrangements on high-index surfaces drive formaldehyde interactions.
In situ PiFM is a powerful tool for structure sensitivity studies in porous materials.
Surface termination plays a critical role in catalytic events on ZIF-8.