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Electrically Conductive π-Intercalated Graphitic Metal-Organic Framework Containing Alternate π-Donor/Acceptor

Ashok Yadav¹, Shiyu Zhang¹, Paola A Benavides¹

¹Department of Chemistry, Clemson University, Clemson, SC 29634, USA.

Angewandte Chemie (International Ed. in English)

|April 5, 2023

Summary

We developed a novel π-intercalated graphitic metal-organic framework (iGMOF1) that significantly enhances electrical conductivity. This new material achieves higher bulk conductivity by enabling efficient charge transport both within layers and across them.

Keywords:

Bottom-up Synthesis Electrical Conductivity Graphitic Metal-Organic Frameworks π-Donor/Acceptor Interaction π-Intercalation

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Area of Science:

Materials Science
Nanotechnology
Electrochemistry

Background:

Two-dimensional graphitic metal-organic frameworks (GMOFs) exhibit good in-plane conductivity but suffer from poor out-of-plane charge transport.
This conductivity anisotropy limits the overall bulk electrical performance of GMOFs.

Purpose of the Study:

To engineer higher bulk electrical conductivity in 2D GMOFs.
To overcome the limitations of inefficient out-of-plane charge transport in stacked 2D GMOF layers.

Main Methods:

A bottom-up synthesis approach was employed to construct the first π-intercalated GMOF (iGMOF1).
The iGMOF1 features alternating stacks of π-donor/acceptor (π-D/A) components: Cu^II-coordinated hexaaminotriphenylene (HATP) ligands and hexacyano-triphenylene (HCTP) molecules.
This design facilitates both in-plane conduction through the Cu₃(HATP)₂ scaffold and out-of-plane conduction via the π-D/A stacks.

Main Results:

The synthesized iGMOF1 demonstrated an order of magnitude higher bulk electrical conductivity compared to the parent Cu₃(HATP)₂ material (25 S/m vs. 2 S/m).
iGMOF1 exhibited a significantly smaller activation energy (36 meV) than Cu₃(HATP)₂ (65 meV).
The enhanced conductivity is attributed to simultaneous in-plane (through-bond) and out-of-plane (through π-D/A stacks) charge transport.

Conclusions:

The successful construction of iGMOF1 validates the π-intercalation strategy for enhancing electrical conductivity in 2D GMOFs.
Simultaneous in-plane and out-of-plane charge transport pathways are crucial for achieving high bulk conductivity.
This work opens avenues for designing novel iGMOFs with superior electrical properties for advanced applications.