Boosting oxygen-reduction catalysis over mononuclear CuN2+2 moiety for rechargeable Zn-air battery

Endowing the transition-metal-nitrogen-carbon (M-N-Cs) electrocatalysts with high oxygen reduction activity for sustainable energy conversion, is a field of intense research while remains elusive. Here we exploit the variable configuration of atomically dispersed Cm centers on carbon support via rationally constructing prototypical CuN2+2 active sites to boost the kinetically sluggish electrochemical oxygen reduction. Density functional theory reveals the modified electronic structure of active Cu site and its derived orbital overlap through right symmetry with the degenerate pi* orbital of O-2 molecule, which more effectively facilitates O-2 activation compared with CuN4 counterpart. The targeted electrocatalyst delivers superior alkaline ORR activity with a half-wave potential of 0.88 V and superior kinetics with Tafel slope of 48 mV dec(-1), outperforming those of benchmark Pt/C. Remarkably, further demonstrated excellent peak power density and long-term durability in both primary liquid and flexible solid-state Zn-air battery assemblies signify the potential for practical applications.

Automated summary

This study explores the use of atomically dispersed active sites to enhance the activity of transition metal-nitrogen-carbon (M-N-Cs) electrocatalysts in oxygen reduction reactions, leading to a breakthrough in the field of oxygen reduction. The targeted electrocatalyst exhibits superior performance compared to Benchmark Pt/C, with excellent potential demonstrated in both liquid and solid-state Zn-air battery assemblies.