Zhao, XueruCheng, HaoChen, XiaoboZhang, QiLi, ChenzhaoXie, JianMarinkovic, NebojsaMa, LuZheng, Jin-ChengSasaki, Kotaro2024-06-122024-06-122024Zhao X, Cheng H, Chen X, et al. Multiple Metal-Nitrogen Bonds Synergistically Boosting the Activity and Durability of High-Entropy Alloy Electrocatalysts. J Am Chem Soc. 2024;146(5):3010-3022. doi:10.1021/jacs.3c08177https://hdl.handle.net/1805/41461The development of Pt-based catalysts for use in fuel cells that meet performance targets of high activity, maximized stability, and low cost remains a huge challenge. Herein, we report a nitrogen (N)-doped high-entropy alloy (HEA) electrocatalyst that consists of a Pt-rich shell and a N-doped PtCoFeNiCu core on a carbon support (denoted as N-Pt/HEA/C). The N-Pt/HEA/C catalyst showed a high mass activity of 1.34 A mgPt-1 at 0.9 V for the oxygen reduction reaction (ORR) in rotating disk electrode (RDE) testing, which substantially outperformed commercial Pt/C and most of the other binary/ternary Pt-based catalysts. The N-Pt/HEA/C catalyst also demonstrated excellent stability in both RDE and membrane electrode assembly (MEA) testing. Using operando X-ray absorption spectroscopy (XAS) measurements and theoretical calculations, we revealed that the enhanced ORR activity of N-Pt/HEA/C originated from the optimized adsorption energy of intermediates, resulting in the tailored electronic structure formed upon N-doping. Furthermore, we showed that the multiple metal-nitrogen bonds formed synergistically improved the corrosion resistance of the 3d transition metals and enhanced the ORR durability.en-USAttribution-NonCommercial-NoDerivatives 4.0 InternationalFuel cellsPt-based catalystsNitrogen (N)-doped high-entropy alloy (HEA) electrocatalystArticle