Controlling 3d orbital energy level via local structure engineering in single atom electrocatalyst
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초록
내용
Transition metal single atom catalysts (SACs) have emerged as promising electrocatalysts due to their maximum atomic efficiency. However, due to poor metal-ligand (M-L) coordination, their catalytic performance is often weak. Herein, we first reveal the effects of pyrrolic nitrogen (N) ligand structure with cobalt (Co) single atomic sites for oxygen evolution reaction (OER) and the relationship between M-L distance and O* intermediate adsorption behavior. Density functional theory calculations show that the pyrrolic N4 symmetry which exhibits long M-L distance causes the enhancement of the adsorption strength of intermediates by reducing the electrons in sigma-antibonding (σ*), and Operando X-ray absorption spectroscopy measurements reveal that the Co single atomic sites in Co–pyrrolic N4 shows rapid electrostatic OH- adsorption behavior. This work provides a new avenue for the rational design of SACs with pyrrolic N4 structure and fundamental insight into the OER catalytic origin.