Multimodal and Multiscale Interrogation of a Mechanically Tough Glass Forming Copper-Based Metal-Organic Framework

Abstract

A copper-based metal-organic framework, Cu(Im)2, was synthesized using a sol-gel process and subsequently melt-quenched into glass upon heating above 240 °C. In this paper, we present a multimodal, multiscale interrogation of the MOF nanocrystals and the resulting glasses. Structural characterization using X-ray diffraction, atomic force microscopy, and electron microscopy was performed to understand the morphology and size of the synthesized nanocrystals and glasses. Thermogravimetric analysis and differential scanning calorimetry were employed to understand the melting process of the crystals to form the glass. Synchrotron pair distribution function analysis was performed to verify that the framework structure is maintained upon melting, and nearfield infrared nanospectroscopy provided insight into the local chemical structure of the materials. The mechanical characterization via nanoindentation revealed that the resulting glasses exhibit an appreciably high elastic modulus (~10 GPa) and the highest fracture toughness (K_1c ~ 0.5 MPa m^1/2) yet reported for MOF glasses. This development is central to the emerging field of MOF-based materials processing and shaping, while upholding mechanical robustness and resistance to cracking.