Despite the challenges on tuning the d-band structure of transition metals, the d-band is of great importance for promoting the interaction between catalytic and intermediates during the oxygen evolution reaction (OER) process. Herein, ultrafine Co nanoparticles embedded in the surface layer of nitrogen-doped carbon microspheres are prepared through an in-situ co-coordination strategy, and its d-band is modulated by introducing different Ni amounts. The introduction of Ni in the Co crystal lattice can tune the d-band center and unpaired electrons, which collectively result in an enhancement of OER activity and kinetics. By investigating the catalysts with Ni content from 0% to 75%, it is concluded that the catalyst with 25% Ni shows optimal OER activity, lower overpotential (285 mV at 10 mA cm-2) and higher current densities (73.75 mA cm-2 at 1.63 V). Moreover, the good stability is also demonstrated with the negligible decrease on current densities after 3000 CV cycles or 100 h of continuous test in alkaline media. This concept of modulating the d-band structure by introducing a transition metal with different contents in another transition metal crystal lattice could present an alternative pathway to the development of highly active catalytic materials for OER and beyond.
Keywords: D-band center; Electrocatalysis; Nitrogen-doped carbon; Oxygen evolution reaction; Unpaired electrons.
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