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Proton exchange membrane fuel cells convert hydrogen and oxygen into electricity without emissions. The high cost and low durability of Pt-based electrocatalysts for the oxygen reduction reaction hinder their wide application, and the development of non-precious metal electrocatalysts is limited by their low performance. Here we design a hybrid electrocatalyst that consists of atomically dispersed Pt and Fe single atoms and Pt–Fe alloy nanoparticles. Its Pt mass activity is 3.7 times higher than that of commercial Pt/C in a fuel cell. More importantly, the fuel cell with a low Pt loading in the cathode (0.015 mgPt cm−2) shows an excellent durability, with a 97% activity retention after 100,000 cycles and no noticeable current drop at 0.6 V for over 200 hours. These results highlight the importance of the synergistic effects among active sites in hybrid electrocatalysts and provide an alternative way to design more active and durable low-Pt electrocatalysts for electrochemical devices.

The intrinsic poor thermal stability of layered LiNi x Co y Mn 1−x−y O 2 (NCM) cathodes and the exothermic side reactions triggered by the associated oxygen release are the main safety threats for their large-scale implantation. In the NCM family, it is widely accepted that Ni is the stability troublemaker, while Mn has long been considered as a structure stabilizer, whereas the role of Co remains elusive. Here, via Co/Mn exchange in a Ni-rich LiNi 0.83 Co 0.11 Mn 0.06 O 2 cathode, we demonstrate that the chemical and structural stability of the deep delithiated NCM cathodes are significantly dominated by Co rather than the widely reported Mn. Operando synchrotron X-ray characterization coupling with in situ mass spectrometry reveal that the Co 4+ reduces prior to the reduction of Ni 4+ and could thus prolong the Ni migration by occupying the tetrahedra sites and, hence, postpone the oxygen release and thermal failure. In contrast, the Mn itself is stable, but barely stabilizes the Ni 4+ . Our results highlight the importance of evaluating the intrinsic role of compositional tuning on the Ni-rich/Cofree layered oxide cathode materials to guarantee the safe operation of high-energy Li-ion batteries.