Electrochemical Reactivity under Confinement Enabled by Molecularly Pillared 2D and Layered Materials

Abstract

This perspective presents an overview of how confinement can be used to tune electrochemical reactivity and the concept of using molecularly pillared 2D and layered materials to experimentally study this phenomenon. Many theoretical and computational studies have shown that the confinement of liquid-phase reactants to nano- or subnanometer spaces influences their electrochemical reactivity. While confinement is ubiquitous in various high surface area materials used as electrodes, experimental studies of this effect are scarce due to the challenge of deconvoluting the many competing influences on the measured electrochemical signal. This creates an exciting opportunity for the synthesis of well-defined materials platforms capable of confining liquid electrolytes and reactants for understanding electrochemical reactivity under confinement. In particular, a precise confinement geometry can be achieved with the use of 2D and layered materials whose interlayers have been tuned with the use of molecular pillars.