Molecular Engineering of Noble Metal Aerogels Boosting Electrocatalytic Oxygen Reduction

Abstract Developing robust oxygen reduction reaction (ORR) electrocatalysts with high activity and durability remains great challenging while noble metal aerogels (NMAs) hold great potential because of their hierarchically porous morphology, excellent activity, and self‐supported characteristic. Herein, a general molecular engineering strategy to synthesize molecule‐noble metal aerogels (M‐NMAs) via 3D assembly of metal nanoparticles (e.g., Pt, Pd, Au, Ag, and PtPd NPs) induced by metalloporphyrin as cross‐linkers is reported. Due to the well synergy of NMAs and porphyrin molecule in creating the facile reaction pathway for ORR catalysis, these M‐NMAs demonstrate boosted ORR activity and durability in different electrolytes. Particularly, the best PtPd‐based M‐NMA delivers 1.47 A mg_Pt⁻¹ and 2.13 mA cm⁻² in mass and specific activities, which are 11.3 and 14.2 times higher than those of the commercial Pt/C catalyst, respectively. Thus, this work not only provides a simple and universal functional engineering approach of NMAs with catalytic molecules, but also opens an avenue of the rational design for superior ORR electrocatalysts.