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Published on: February 1, 2022
Cooperative Spin Transition of Monodispersed FeN3 Sites within Graphene Induced by CO Adsorption
Qin-Kun Li1, Xiao-Fei Li2, Guozhen Zhang1
1Hefei National Laboratory for Physical Sciences at the Microscale, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), CAS Center for Excellence in Nanoscience, School of Chemistry and Materials Science , University of Science and Technology of China , Hefei , Anhui 230026 , China.
Abstract:
The significance of identifying the fundamental mechanism of interactions between adjacent catalytic active centers has long been underestimated. Utilizing density functional theory calculations, we demonstrate controllable cooperative interaction between two nearby Fe centers embedded on nitrogenated graphene aided by CO adsorption. The interconnected adjacent Fe atoms respond cooperatively to CO molecules with communicative structural self-adaption and electronic transformation. The adsorbed CO changes not only the spin of the active site it is attached to but also that of its adjacent site. Consequently, the two adjacent Fe atoms feature unique oscillatory long-range spin coupling. Our theoretical investigation suggests cooperative communication between adjacent active sites on a single-atom catalyst is nontrivial.
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