Highly Surface-Distorted Pt Superstructures for Multifunctional Electrocatalysis

Platinum (Pt) catalysts play a key role in energy conversion and storage processes, but the realization of further performance enhancement remains challenging. Herein, we report a new class of Pt superstructures (SSs) with surface distortion engineering by electrochemical leaching of PtTe_x SSs that can largely boost the oxygen reduction reaction (ORR), the methanol oxidation reaction (MOR), and the hydrogen evolution reaction (HER). In particular, the high-distortion (H)-Pt SSs achieve a mass activity of 2.24 A mg^–1 at 0.90 V_RHE for the ORR and 2.89 A mg^–1 for the MOR as well as a low overpotential of 25.3 mV at 10 mA cm^–2 for the HER. Moreover, the distorted surface features of Pt SSs can be preserved by mitigating the detrimental effects of agglomeration/degradation during long-time electrocatalysis. A multiscale modeling demonstrates that surface compressions, defects, and nanopores act in synergy for the enhanced ORR performance. This work highlights the advances of stable superstructure and distortion engineering for realizing high-performance Pt nanostructures.