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Abstract:
Co-based metal-organic frameworks (MOFs) as electrocatalysts for two-electron oxygen reduction reaction (2e(-) ORR) are highly promising for H2O2 production, but suffer from the intrinsic activity-selectivity trade-off. Herein, we report a ZnCo bimetal-triazole framework (ZnCo-MTF) as high-efficiency 2e(-) ORR electrocatalysts. The experimental and theoretical results demonstrate that the coordination between 1,2,3-triazole and Co increases the antibonding-orbital occupancy on the Co-N bond, promoting the activation of Co center. Besides, the adjacent Zn-Co sites on 1,2,3-triazole enable an asymmetric "side-on" adsorption mode of O-2, favoring the reduction of O-2 molecules and desorption of OOH* intermediate. By virtue of the unique ligand effect, the ZnCo-MTF exhibits a 2e(-) ORR selectivity of approximate to 100 %, onset potential of 0.614 V and H2O2 production rate of 5.55 mol g(cat)(-1) h(-1), superior to the state-of-the-art zeolite imidazole frameworks. Our work paves the way for the design of 2e(-) ORR electrocatalysts with desirable coordination and electronic structure.
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ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
ISSN: 1433-7851
Year: 2023
Issue: 2
Volume: 63
1 6 . 1
JCR@2023
1 6 . 1 0 0
JCR@2023
JCR Journal Grade:1
CAS Journal Grade:1
Cited Count:
WoS CC Cited Count: 27
SCOPUS Cited Count: 14
ESI Highly Cited Papers on the List: 0 Unfold All
WanFang Cited Count:
Chinese Cited Count:
30 Days PV: 0
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