Ultrahigh-Loading Zinc Single-Atom Catalyst for Highly Efficient Oxygen Reduction in Both Acidic and Alkaline Media

摘要

Atomically dispersed Zn-N-C nanomaterials are promising platinum-free catalysts for the oxygen reduction reaction (ORR). However, the fabrication of Zn-N-C catalysts with a high Zn loading remains a formidable challenge owing to the high volatility of the Zn precursor during high-temperature annealing. Herein, we report that an atomically dispersed Zn-N-C catalyst with an ultrahigh Zn loading of 9.33wt% could be successfully prepared by simply adopting a very low annealing rate of 1 degrees min(-1). The Zn-N-C catalyst exhibited comparable ORR activity to that of Fe-N-C catalysts, and significantly better ORR stability than Fe-N-C catalysts in both acidic and alkaline media. Further experiments and DFT calculations demonstrated that the Zn-N-C catalyst was less susceptible to protonation than the corresponding Fe-N-C catalyst in an acidic medium. DFT calculations revealed that the Zn-N-4 structure is more electrochemically stable than the Fe-N-4 structure during the ORR process.