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N‐doped sites at carbon nanotubes and graphene trigger the spontaneous decoration of bimetal (Pt and Pd) particles by the facile electroless redox reaction. The created hybrid catalyst yields remarkable current density (≈2.44 mA cm−2), lower onset potential (≈0.13 V), higher electron transfer number ≈4), and long‐term stability for oxidation–reduction reactions.
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