Abstract

Regulation of the surface microenvironment is crucial for the development of highly active and durable OER/ORR bifunctional catalysts. In this study, a bifunctional m-CoSx@NSC electrocatalyst with dual electric field effects was designed and fabricated by synchronous pyrolysis of organic sulfur-rich cobalt compounds (Co-DC) and melem. The introduction of nitrogen-rich melem effectively induced the conversion of Co-DC and the growth of tentacles to form a hierarchical carbon skeleton. The interfacial micro-electric field between the carbon layer and CoSx active species improves the intrinsic activity and stability of m-CoSx@NSC. Finite element method simulation and in-situ measurements proved that the tentacle-induced external local electric field promotes the formation of Co(OH)2/CoOOH intermediates and mass transfer, thus accelerating the catalytic reaction kinetics. Through the synergistic effect of dual electric fields, the m-CoSx@NSC catalyst demonstrated a low overpotential of 340 mV for OER and a high half-wave potential of 0.85 V for ORR. Furthermore, the m-CoSx@NSC-based ZAB exhibited an open-circuit voltage of 1.42 V, a maximum power density of 87.38 mW cm−2, a specific capacity of 876.17 mAh gZn−1, and a cycling performance of 700 cycles. The synergistic regulation of the internal and external microenvironments provides a novel insight to improve the catalytic reaction kinetics of OER/ORR.

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