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One of the great challenges facing atomically dispersed catalysts, includingsingle-atom catalyst (SAC) and double-atom catalyst (DAC) is their ultra-lowmetal loading (typically less than 5 wt%), basically limiting the practicalcatalytic application, such as oxygen reduction reaction (ORR) crucial tohydrogen fuel cell and metal-air battery. Although some important progresseshave been achieved on ultra-high-density (UHD) SACs, the reports on UHD-DACswith stable uniform dispersion is still lacking. Herein, based on theexperimentally synthesized M2N6 motif (M = Sc-Zn), we theoreticallydemonstrated the existence of the UHD-DACs with the metal loading > 40 wt%,which were confirmed by systematic analysis of dynamic, thermal, mechanical,thermodynamic, and electrochemical stabilities. Furthermore, ORR activities ofthe UHD-DACs are comparable with or even better than those of theexperimentally synthesized low-density (LD) counterparts, and the Fe2N6 andCo2N6 UHD-DACs locate at the peak of the activity volcano with ultra-lowoverpotentials of 0.31 and 0.33 V, respectively. Finally, spin magnetic momentof active center is found to be a catalytic descriptor for ORR on the DACs. Ourwork will stimulate the experimental exploration of the ultra-high-density DACsand provides the novel insight into the relationship between ORR activity ofthe DACs and their spin states.

Ultra-high-density double-atom catalyst with spin moment as activity descriptor for oxygen reduction reaction