Abstract

Developing active and stable non-precious metal bifunctional electrocatalysts towards the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) still remains a crucial challenge. Herein, we propose a simple strategy of integrating atomically dispersed and nanoscaled Co species embedded in micro-/mesoporous carbon nanosheet/nanotube architecture. Revealed by control and SCN- poisoning experiments, N species and atomically dispersed Co species are the main active centers for ORR; whereas the metal Co nanocrystals are the chief active species for OER. Additionally, the balanced micro/mesopore distribution offers fast mass diffusion, and carbon nanosheet/nanotube architecture supplies favorable 3D electrical conduct. As a result, the as-prepared CoNC (1:4) exhibits a positive half-wave potential of 0.87 V (vs RHE) for ORR, and a low potential of 1.55 V (vs RHE) at 10 mA cm−2 for the OER. Importantly, the flexible Zn-air battery using the catalyst exhibits a peak power density of 117 mW cm−2, a higher round-trip efficiency of 68% cycling at 2 mA/cm−2, and an excellent cycling stability with 3% decrease after 126 cycles test. This work provides a general strategy to design bifunctional catalysts by integrating atomically dispersed and nanoscaled transitional metal species together with N-doped micro-/mesoporous 3D carbon.

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