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Metal single-atom materials with their high atom utilization efficiency and unique electronic structures usually show remarkable catalytic performances in many crucial chemical reactions. Herein, a facile and easily scalable "impregnation-carbonization-acidification" strategy for fabricating a class of single-atom-anchored (including cobalt and nickel single atoms) monolith as superior binder-free electrocatalysts for developing high-performance wearable Zn-air batteries is reported. The as-prepared single atoms, supported by N-doped carbon flake arrays grown on carbon nanofibers assembly (M SA@NCF/CNF), demonstrate the dual characteristics of excellent catalytic activity (reversible oxygen overpotential of 0.75 V) and high stability, owing to the greatly improved active sites' accessibility and optimized single-sites/pore-structures correlations. Furthermore, wearable Zn-air battery based on Co SA@NCF/CNF air electrode displays superior stability under deformation, satisfactory energy storage capacity, and good practicality to be utilized as an integrated battery system. Theoretical calculations reveal a mechanism for the promotion of the catalytic performances on single atomic sites by lowering the overall oxygen reduction/evolution reaction barriers comparing to metal cluster co-existing configuration. These findings provide a facile strategy for constructing free-standing single-atom materials as well as the engineering of high-performance binder-free catalytic electrodes.
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