High-entropy materials are poised to revolutionize materials science and industrial applications due to their design flexibility, peculiar performance, and broad applicability. In this study, we present a proof-of-concept high-entropy engineered nanocarbon (HENC) co-doped with five nonmetal elements (B, F, P, S, and N), synthesized via in situ polymerization modification of ZIF-8 followed by pyrolysis. The HENC exhibits outstanding performance as a nonmetal electrocatalyst for the oxygen reduction reaction (ORR), with activity on par with benchmark Pt/C electrocatalysts and superior cyclic stability. Simulations and all-site calculations reveal that the synergistic effects of abundant heteroatoms and increased system entropy facilitate the formation of *O2 species, with N, P, and S acting as the key active elements, while co-doping with B and F further enhances stability. Notably, HENCs have been validated as cathode catalysts in zinc-air batteries, achieving an impressive peak power density of 604 mW cm-2 and demonstrating long-term stability over a 16-day period, outpacing the commercial Pt/C catalyst (542 mW cm-2). This work not only enriches the concept of high entropy and advances the understanding of high-entropy materials but also opens a new avenue for the development of high-performance low-cost catalysts.
Keywords: All‐site calculations; Electrocatalysts; Functionalized nanocarbon; High‐entropy doping; Oxygen reduction reaction.
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