UNLEASH: Ultralow Nanocluster Loading of Pt via Electro-Acoustic Seasoning of Heterocatalysts

The shift toward sustainable energy has fueled the development of advanced electrocatalysts to enable green fuel production and chemical synthesis. To date, no material outperforms Pt-group catalysts for key electrocatalytic reactions, necessitating advanced catalysts that minimize use of these rare and expensive constituents (i.e., Pt) to reduce cost without sacrificing activity. Whilst a myriad of routes involving co-synthesis of Pt with other elements have been reported, the Pt is often buried within the bulk of the composite, rendering a large proportion of it inaccessible to the interfacial electrocatalytic reaction. Surface decoration of Pt on arbitrary substrates is therefore desirable to maximize catalytic activity; nevertheless, Pt electrodeposition suffers from clustering and ripening effects that result in large ( $⌀0.1-1\mu m$ ) aggregates that hinder electrocatalytic activity. Herein, an unconventional synthesis method is reported that utilizes high-frequency (10 MHz) acoustic waves to electrochemically 'season' a gold working electrode with an ultralow loading of Pt nanoclusters. The UNLEASH platform is shown to facilitate high-density dispersion of nanometer-order clusters at the bimetallic interface to enable superior atomic utilization of Pt. This is exemplified by its utility for methanol oxidation reaction (MOR), wherein a mass activity of 5.28 A ${\mathrm{mg}}_{\mathrm{Pt}}^{-1}$ is obtained, outperforming all other Au/Pt bimetallic electrocatalysts reported to date.