In situ electrochemical redox tuning of Pd-Co hybrid electrocatalysts for high-performance methanol oxidation: Strong metal-support interaction

Abstract

Construction of strong metal-support interaction (SMSI) is of fundamental interest in the preparation of supported metal nanoparticle catalysts with enhanced catalytic activity. Herein, we report a facile in situ electrochemical redox tuning approach to build strong interactions between metals and supports. As for a typical example, a composite electrocatalyst of Pd-Co hybrid nanoparticles directly developed on Ni substrate is found to follow a distinct surface self-reconstruction process in alkaline media via an in situ electrochemical redox procedure, which results in structural transition from the original nanoparticles (NPs) to nanosheets (NSs) coupled with a phase transformation of the Co component, Co → CoO/Co(OH)2. The SMSI is observed in the electrochemically tuned Pd-Co hybrid system and leads to significantly enhanced catalytic activity for methanol oxidation reaction (MOR) due to the modified atomic/electronic structure, increased surface area, and more exposed electroactive sites. Compared with commercial Pd/C catalyst, the electrochemically tuned Pd-Co hybrid catalyst with SMSI exhibits superior catalytic activity (2330 mA∙mgPd−1) and much better stability (remains 503 mA∙mgPd−1 after 1000 cycles and 172 mA∙mgPd−1 after 5000 s), and therefore has great potential in practical applications.