Optimal coordination-site exposure engineering in porous platinum for outstanding oxygen reduction performance

Abstract

In this study, we report that optimal coordination-site exposure engineering in porous platinum brings ultrahigh activity and durability for the fuel cell oxygen reduction reaction (ORR). The porous platinum with numerous grain boundaries (GBP-Pt) consisting of 3 nm crystals exhibits 7 times higher ORR activity than commercial Pt. For fuel-cell measurements, the GBP-Pt catalyst based MEA exhibits high power density (1.49 W cm⁻², 0.71 A mg⁻¹ Pt for mass activity) and stability (12.9% loss after 30 K cycles), all of which far surpass the U.S. DOE target in 2020 (0.44 A mg⁻¹ Pt for mass activity and 40% loss for stability). Density Functional Theory (DFT) calculation and X-ray Absorption Fine Structure (XAFS) results suggest that proper Pt coordination site exposure in grain boundaries provides optimal adsorption energies for oxygen species and high stability in the ORR, even superior to Pt(111) sites. We anticipated that coordination-site exposure engineering would open a new avenue to offer robust electrocatalysts for the fuel-cell oxygen reduction reaction.