LAUSR

For current single-atom catalysts (SACs), modulating the coordination environments of rare earth (RE) single atoms with complex electronic orbital and flexible chemical states is still limited. Herein, we report cerium (Ce) SAs supported on the P, S, and N co-doped hollow carbon substrate (Ce SAs/PSNC) for oxygen reduction reaction (ORR). The as-prepared Ce SAs/PSNC possessed a half-wave potential of 0.90 V, a turnover frequency value of 52.2 s-1 at 0.85 V, and excellent stability for ORR, which far exceeds the commercial Pt/C and most recent SACs. The Ce SAs/PSNC-based liquid zinc-air batteries (ZABs) exhibited a high and stable open circuit voltage of 1.49 V and a maximum power density of 212 mW cm-2 . As the catalyst of air cathode, it also displayed remarkable performances in flexible electronic devices. Theoretical calculations have revealed that the introduction of S and P sites has induced significant electronic modulations to the Ce SA active sites. The P and S dopings promote the electroactivity of Ce SAs and improve the overall site-to-site electron transfer within the Ce SAs/PSNC. This work can offer a unique perspective for modulating RE-based SACs in a complex coordination environment towards superior electrocatalysis and broad applications in energy conversion and storage devices. This article is protected by copyright. All rights reserved.