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Local geometric strain engineering is useful for modulating the performance of nitrogen-coordinated transition metal-carbon catalysts. However, realizing the nano-level strain is technically challenging. Additionally, the structure-property relationship between strain degree and performance remains poorly understood. Herein, it is conceptually predict that geometric bending induces more electron transfer from Zn to the coordinated N in ZnNC, leading to a positive shift of the d-band center of the Zn atom, which promotes the adsorption reduction process of the O-2 molecule and thus increases the intrinsic oxygen reduction reaction (ORR) activity. Moreover, a low-temperature non-saturated coordination strategy is proposed to prepare spherical porous carbon catalysts with surface-enriched geometrically bent (20-50(degrees)) ZnNC sites. Benefiting from the highly active ZnNC sites, large specific surface area and abundant pore structure, the optimized catalyst (SZnNC-950) exhibited excellent intrinsic alkaline ORR activity (half-wave potential E-1/2 = 0.89 V) and high zinc-air battery performance (peak power density of 229.2 mW cm(-2)), exceeding that of commercial Pt/C catalysts. Density functional theory (DFT) calculations show that when the geometrical bending angle is 30-45(degrees), Zn centers with suitable charge transfer to the surrounding N can produce a moderate adsorption strength to the oxygen intermediate state, resulting in optimal ORR activity.
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ADVANCED FUNCTIONAL MATERIALS
ISSN: 1616-301X
Year: 2024
Issue: 10
Volume: 34
1 8 . 5 0 0
JCR@2023
JCR Journal Grade:1
CAS Journal Grade:1
Cited Count:
WoS CC Cited Count: 19
SCOPUS Cited Count: 19
ESI Highly Cited Papers on the List: 0 Unfold All
WanFang Cited Count:
Chinese Cited Count:
30 Days PV: 2
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