.png){kind=icon}
.png){kind=icon}
Return
Dual modulation of coordination asymmetry and curvature unlocks record-level Zn-air battery performance with Fe-N-C single-atom catalysts
.png){kind=icon}
PRE
AI
Q
L
B
C
Z
H
D
W
J
Z
黄
Y
DOI：10.1039/D5EE04648C.png)
.png){kind=icon}
Original request for help.png){kind=icon}
Share.png){kind=icon}
Save
Abstract
En 中文
The coordination environment of single-atom catalysts (SACs) plays a pivotal role in determining their electronic structure and catalytic performance. Conventional planar Fe-N4 motifs; however; often bind oxygen intermediates too strongly; limiting their activity in oxygen electrocatalysis. Here; we report a symmetry-breaking strategy coupled with nanoscale surface curvature engineering to tailor the electronic and spatial configuration of isolated Fe sites anchored on a sulfur/nitrogen co-doped highly concave carbon polyhedron (Fe-N4S1/SNhcC). This dual-scale structural design delivers outstanding bifunctional activity for the oxygen reduction and evolution reactions (ORR/OER); achieving a high half-wave potential of 0.933 V and a small ORR/OER potential gap (ΔE) of 0.695 V. Density functional theory calculations reveal that the asymmetric Fe-N4S1 coordination; modulated by surface curvature; weakens *OH binding and lowers the energy barrier for ORR. Finite element simulations further show that the local electric field generated by the concave surface enhances the adsorption of O2 and OH-; thereby accelerating reaction kinetics. When applied as a cathode in quasi-solid-state Zn-air batteries; Fe-N4S1/SNhcC demonstrates exceptional performance across a wide temperature range (-60 to 80 °C); including a high peak power density of 181 mW cm-2 and extended cycling stability of 210/120/80 h at 20/50/100 mA cm-2; respectively. Notably; it delivers a discharge capacity of 1.56 Ah and a cycling lifespan exceeding 2000 h at -40 °C and 2 mA cm-2. This work highlights the importance of dual-scale structural modulation in SACs and opens new avenues for rechargeable Zn-air batteries operating under extreme conditions.
Journal
IF:
30.8
Papers:
6.9K
Citations:
12.4W
Organization
No organization information available
Cited Papers