Qiao, ZhiWang, ChenyuLi, ChenzhaoZeng, YachaoHwang, SooyeonLi, BoyangKarakalos, StavrosPark, JaehyungKropf, A. JeremyWegener, Evan C.Gong, QingXu, HuiWang, GuofengMyers, Deborah J.Xie, JianSpendelow, Jacob S.Wu, Gang2023-02-142023-02-142021-09Qiao, Z., Wang, C., Li, C., Zeng, Y., Hwang, S., Li, B., Karakalos, S., Park, J., Kropf, A. J., Wegener, E. C., Gong, Q., Xu, H., Wang, G., Myers, D. J., Xie, J., Spendelow, J. S., & Wu, G. (2021). Atomically dispersed single iron sites for promoting Pt and Pt3Co fuel cell catalysts: Performance and durability improvements. Energy & Environmental Science, 14(9), 4948–4960. https://doi.org/10.1039/D1EE01675Jhttps://hdl.handle.net/1805/31243Significantly reducing platinum group metal (PGM) loading while improving catalytic performance and durability is critical to accelerating proton-exchange membrane fuel cells (PEMFCs) for transportation. Here we report an effective strategy to boost PGM catalysts through integrating PGM-free atomically-dispersed single metal active sites in the carbon support toward the cathode oxygen reduction reaction (ORR). We achieved uniform and fine Pt nanoparticle (NP) (∼2 nm) dispersion on an already highly ORR-active FeN4 site-rich carbon (FeN4–C). Furthermore, we developed an effective approach to preparing a well-dispersed and highly ordered L12 Pt3Co intermetallic nanoparticle catalyst on the FeN4–C support. DFT calculations predicted a synergistic interaction between Pt clusters and surrounding FeN4 sites through weakening O2 adsorption by 0.15 eV on Pt sites and reducing activation energy to break O–O bonds, thereby enhancing the intrinsic activity of Pt. Experimentally, we verified the synergistic effect between Pt or Pt3Co NPs and FeN4 sites, leading to significantly enhanced ORR activity and stability. Especially in a membrane electrode assembly (MEA) with a low cathode Pt loading (0.1 mgPt cm−2), the Pt/FeN4–C catalyst achieved a mass activity of 0.451 A mgPt−1 and retained 80% of the initial values after 30 000 voltage cycles (0.60 to 0.95 V), exceeding DOE 2020 targets. Furthermore, the Pt3Co/FeN4 catalyst achieved significantly enhanced performance and durability concerning initial mass activity (0.72 A mgPt−1), power density (824 mW cm−2 at 0.67 V), and stability (23 mV loss at 1.0 A cm−2). The approach to exploring the synergy between PGM and PGM-free Fe–N–C catalysts provides a new direction to design advanced catalysts for hydrogen fuel cells and various electrocatalysis processes.enCC0 1.0 Universalfuel cell electric vehiclesmembrane electrode assemblyPGM loadingsArticle