Jiahui Song, Yutao Ni, Chaoqi Han, Huiying Lan, Xue Jing, Mengxue Huang, Lifang Chen, Qi Wang, Wenwen Shi, Ruimin Ding, Xi Yin
ABSTRACT Rational carbon support engineering is a critical yet underexplored strategy for modulating the activity and durability of Pt‐based oxygen reduction reaction (ORR) electrocatalysts in proton exchange membrane fuel cells (PEMFCs). Here, we show that dual‐atom‐site‐rich carbon supports constitute an unique and highly promising architecture, playing a decisive role in electronic metal‐support interactions (EMSI) and catalyst stability. Comparing single‐atom‐site‐rich (M‐NC, M = Co or Fe) and dual‐atom‐site‐rich (CoFe‐NC) supports for PtZn intermetallic nanoparticles (iNPs) reveals that conventional M‐NC suffers from metal leaching, whereas cooperative CoFe‐N 8 sites remain intact, enabling strong and persistent EMSI. Density functional theory (DFT) calculations reveal that the dual‐atom‐site configuration promotes electron donation to Pt, downshifts the Pt d ‐band center, reduces the kinetic barrier for the final * OH desorption step, and reinforcing nanoparticle anchoring, collectively enhancing ORR activity and stability. Consequently, PtZn@CoFe‐NC catalyst achieves a mass activity of 1.93 A mg Pt −1 at 0.9 V vs. RHE in rotating disc electrode (RDE) tests. Membrane electrode assembly (MEA) delivers peak power density 2.18 W cm −2 (H 2 ─O 2 ), retaining ∼95% performance after 30k cycles accelerated stress test (AST). This work highlights that dual‐atom‐site‐rich support engineering can serve as an effective approach to enhance performance of PtZn catalysts.