Design of Metal-Organic Framework Templated Materials Using High-Throughput Computational Screening

Area of Science:

• Materials Science
• Computational Chemistry
• Polymer Chemistry

Background:

• Metal-Organic Frameworks (MOFs) can be crosslinked to form "ideal network polymers".
• Synthesizing crystalline Covalent-Organic Frameworks (COFs) with diverse topologies is challenging using conventional methods.
• Previous MOF crosslinking utilized flexible linkers; rigid linkers require precise geometric matching, necessitating in silico design.

Purpose of the Study:

• To develop an effective computational method for identifying ideal rigid cross-linker/MOF pairs.
• To enable the synthesis of novel Covalent-Organic Frameworks (COFs) with unprecedented network flexibility.
• To provide a robust strategy for designing advanced network materials.

Main Methods:

• Developed a geometric high-throughput screening algorithm considering distances, angles, and rotations for MOF/cross-linker matching.
• Employed Molecular Dynamics (MD) simulations to quantitatively validate the geometric screening results.
• Screened MOF and cross-linker libraries to identify potential MOF-to-COF candidates.

Main Results:

• Successfully identified ideal rigid cross-linker/MOF combinations through computational screening.
• Validated the accuracy of the geometric matching algorithm using MD simulations.
• Discovered several promising MOF-to-COF candidate structures.

Conclusions:

• The presented geometric method is a powerful tool for designing MOF/cross-linker combinations.
• This approach facilitates the synthesis of Covalent-Organic Frameworks (COFs) with tunable network topologies.
• The methodology can be extended to design other complex network structures like mechanically interlocked materials.