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Modulating a1g-b1g-orbital occupied states of planar square-coordinated cobalt single-atom electrocatalyst for oxygen
1School of Integrated Circuits, Hubei University, Wuhan 430062, PR China.
Abstract:
Exploiting low-cost electrocatalysts for the oxygen evolution reaction (OER) is significantly important for rechargeable Zn-air batteries. Herein, we modulate the a1g-b1g-orbital occupied states of planar square-coordinated copper oxide by introducing the single-atom cobalt (denoted as Co-CuO). As expected, the resultant Co-CuO catalyst achieves excellent OER catalytic activity with a low overpotential of only 280 mV and 320 mV at 10 mA cm-2 and 50 mA cm-2, respectively, and maintains a stable performance for over 130 h at 50 mA cm-2, manifesting its high potential for practical application in rechargeable Zn-air battery and water splitting Experiments and theoretical calculations reveal that its high activity originates from the electron redistribution and the optimization of the electron spin states of the dz2 and dx2-y2 orbitals of single-atom cobalt in the planar square crystal field. This study provides a valuable research paradigm for the efficient regulation of surface adsorption of oxygen-containing intermediates in OER.
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