Issue 47, 2023

Electrocatalysis with molecules and molecular assemblies within gas diffusion electrodes

Abstract

Molecular catalysts and their assemblies are important model systems in electrocatalysis. This is largely because their active sites, secondary coordination spheres, and reaction environments can be rationally modulated. Such experiments yield important insights into the structure–activity relationships that can be used to design improved catalysts or translated to more technologically mature systems. However, in the context of electrocatalysis, molecular catalysts are often dissolved in an electrolyte or heterogenized on an electrode that is completely submersed in an electrolyte (e.g. H-cell) or reaction setups that are not used in practical systems and use poorly soluble gaseous reactants like CO2, CO, or O2. This is beginning to change, with a growing emphasis being placed on investigating molecular catalysts and catalytic assemblies (e.g. metal/covalent organic frameworks and polymers with molecular active sites) in gas-diffusion electrodes (GDEs) that feed the reactant directly from the gas phase to the catalytic sites and enable industrially viable current densities. Against this backdrop, this perspective first details the emerging set of molecular catalyst-embedded GDE-based systems and what the community has learned thus far from these efforts. We next identify the gaps in knowledge and performance that are yet to be closed and offer strategies for exploring in this direction. Finally, we conclude with a forward-looking discussion that highlights several new avenues to be pursued with molecule-based GDE platforms and how this can accelerate progress in the electrocatalysis field as a whole.

Graphical abstract: Electrocatalysis with molecules and molecular assemblies within gas diffusion electrodes

Article information

Article type
Perspective
Submitted
10 10 2023
Accepted
01 11 2023
First published
02 11 2023
This article is Open Access

All publication charges for this article have been paid for by the Royal Society of Chemistry
Creative Commons BY license

Chem. Sci., 2023,14, 13696-13712

Electrocatalysis with molecules and molecular assemblies within gas diffusion electrodes

H. Bemana, M. McKee and N. Kornienko, Chem. Sci., 2023, 14, 13696 DOI: 10.1039/D3SC05362H

This article is licensed under a Creative Commons Attribution 3.0 Unported Licence. You can use material from this article in other publications without requesting further permissions from the RSC, provided that the correct acknowledgement is given.

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