Electrically conductive 2D metal–organic frameworks (MOFs) have emerging applications in electrocatalysis, energy storage, and electronic devices. However, their formation mechanisms are poorly understood, resulting in limited control over particle size and shape. I hypothesize that a critical barrier to their synthesis is uncontrolled ligand oxidation, as conductive MOFs often contain redox-active catechol, o-phenylenediamine, and dithiolene building units that are oxidized in situ during synthesis in air. Here, I will describe a new synthetic strategy for the 2D framework Cu3(HHTP)2 (HHTP = 2,3,6,7,10,11-hexahydroxytriphenylene) that relies on controlled chemical oxidation performed under an inert atmosphere. By varying the strength and rate of introduction of chemical oxidant, I have produced three distinct morphologies of Cu3(HHTP)2: long, narrow rods; short, thick particles; and large intergrown flakes. How particle morphology influences capacitive performance will be described. Ultimately, this new synthetic approach will enable deeper insight into the formation mechanisms of this important class of frameworks.

Controlled oxidative synthesis of triphenylene-based 2D metal–organic frameworks

ACS Spring 2022

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