Isolation of pseudocapacitive surface processes at monolayer MXene flakes reveals delocalized charging mechanism

Marc Brunet Cabré, Dahnan Spurling, Pietro Martinuz, Mariangela Longhi, Christian Schröder, Hugo Nolan, Valeria Nicolosi, Paula E. Colavita and Kim McKelvey ()
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Marc Brunet Cabré: Trinity College Dublin
Dahnan Spurling: Trinity College Dublin
Pietro Martinuz: Trinity College Dublin
Mariangela Longhi: Università degli Studi di Milano, Dipartimento di Chimica
Christian Schröder: Trinity College Dublin
Hugo Nolan: Trinity College Dublin
Valeria Nicolosi: Trinity College Dublin
Paula E. Colavita: Trinity College Dublin
Kim McKelvey: Trinity College Dublin

Nature Communications, 2023, vol. 14, issue 1, 1-7

Abstract: Abstract Pseudocapacitive charge storage in Ti3C2Tx MXenes in acid electrolytes is typically described as involving proton intercalation/deintercalation accompanied by redox switching of the Ti centres and protonation/deprotonation of oxygen functional groups. Here we conduct nanoscale electrochemical measurements in a unique experimental configuration, restricting the electrochemical contact area to a small subregion (0.3 µm2) of a monolayer Ti3C2Tx flake. In this unique configuration, proton intercalation into interlayer spaces is not possible, and surface processes are isolated from the bulk processes, characteristic of macroscale electrodes. Analysis of the pseudocapacitive response of differently sized MXene flakes indicates that entire MXene flakes are charged through electrochemical contact of only a small basal plane subregion, corresponding to as little as 3% of the flake surface area. Our observation of pseudocapacitive charging outside the electrochemical contact area is suggestive of a fast transport of protons mechanism across the MXene surface.

Date: 2023
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DOI: 10.1038/s41467-023-35950-1

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