Engineering the morphology and electronic structure of atomic cobalt-nitrogen-carbon catalyst with highly accessible active sites for enhanced oxygen reduction

Abstract

The stabilization of non-precious metals as isolated active sites with high loading density over nitrogen-doped carbon materials is essential for realizing the industrial application of single atom catalysts. However, achieving high loading of single cobalt active sites with greatly enhanced oxygen reduction reaction (ORR) activity and stability remains challenging. Here, an efficient approach was described to create a single atom cobalt electrocatalyst (Co SAs/NC) which possesses enhanced mesoporosity and specific surface area that greatly favor the mass transportation and exposure of accessible active sites. The electronic structure of the catalyst by the strong metal-support interaction has been elucidated through experimental characterizations and theoretical calculations. Due to dramatically enhanced mass transport and electron transfer endowed by morphology and electronic structure engineering, Co SAs/NC exhibits remarkable ORR performance with excellent activity (onset and half-wave potentials of 1.04 V (RHE) and 0.90 V (RHE), Tafel slope of 69.8 mV dec−1 and Jk of 18.8 mA cm−2 at 0.85 V) and stability (7 mV activity decay after 10,000 cycles). In addition, the catalyst demonstrates great promise as an alternative to traditional Pt/C catalyst in zinc-air batteries while maintaining high performance in terms of high specific capacity of (796.1 mAh/gZn), power density (175.4 mW/cm2), and long-term cycling stability (140 h). This study presents a facile approach to design SACs with highly accessible active sites for electrochemical transformations.