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Curved Interfaces Enhanced Oxygen Reduction Reaction by PtCo Alloys Anchored MOF-Derived Carbon
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DOI：10.1039/D6NR01476C.png)
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Abstract
En 中文
The carbon supports employed in oxygen reduction reaction (ORR) catalysts frequently exhibit crumpled; curled; or other curved morphologies-features. The local microenvironment generated by such curved interfaces and its impact on the electronic structure of active sites as well as reaction kinetics; remain to be studied. Herein; the finite element method was employed to elucidate the evolution of the local catalytic microenvironment during the pyrolysis of ZIF-67 from the perspective of geometric distortion; the results revealed that moderate interfacial curvature can significantly enhance the local electric field strength and promote O 2 enrichment. Guided by the simulation results; MOF-derived carbon with an optimal curved configuration was constructed via control of the pyrolysis temperature. After etching; metal ion adsorption; and H 2 reduction; MOFderived carbon materials loaded with PtCo alloy were obtained (PtCo/NCs). As expected; the PtCo/NCs-900 sample with a moderately curved interface exhibited outstanding ORR performance; with a half-wave potential of 0.831 V; and 91.7% activity retention after 50000 s. Density functional theory calculations demonstrated that the curved interface in PtCo/NCs-900 induces electron redistribution; shifts the d-band center of Pt and optimizes *OH desorption behavior; thereby lowering the O 2 diffusion barrier; facilitating electron transfer; and ensuring sufficient O 2 supply.As an air-cathode catalyst; PtCo/NCs-900 sample delivered a peak power density of 159 mW cm -2 and a specific capacity of 837 mAh g -1 Zn ; demonstrating its potential for practical energy applications.
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