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Enhancing catalytic activity through modulating the interaction between N-doped carbon and metal phosphides clusters is an effective approach. Herein, the electronic structure modulation of CoP2 supported N-modified carbon (CoP2/NC) has been designed and prepared as efficient electrocatalysts for oxygen reduction reaction (ORR), oxygen evolution reaction (OER), and hydrogen evolution reaction (HER). Notably, CoP2/NC-1 catalyst exhibits impressive performance in alkaline media, with an ORR half-wave potential of 0.84 V, as well as OER and HER overpotentials of 290 and 129 mV (at 10 mA·cm−2), respectively. In addition, CoP2/NC-1 produces a power density as high as 172.9 mW·cm−2, and excellent reversibility of 100 h at 20 mA·cm−2 in home-made Zn-air batteries. The experimental results demonstrate that the synergistic interactions between N modified carbon substrate and CoP2 material significantly enhance the kinetics of ORR, OER, and HER. Density functional theory (DFT) calculations reveal the strong electrons redistribution of CoP2 induced by high-density N atoms at the interface, thus optimizing the key intermediates and significantly lower the energy barrier of reactions. These electronic adjustments of CoP2 greatly enhance its kinetics of ORR/OER/HER, leading to faster reactions. This study provides profound insights into the specific modification of CoP2 by N-doped carbon, enabling the construction of efficient catalysts.
This work was supported by the National Natural Science Foundation of China (Nos. 51872209, 52171145, 21972106, and 22105146), Zhejiang Province Natural Science Foundation project key project (No. LZ20B030001), and Zhejiang Provincial Special Support Program for High-level Talents (No. 2019R52042).