Stability and Electronic
Structure of Nitrogen-Doped
Graphene-Supported Cun (n = 1–5) Clusters in Vacuum and under Electrochemical Conditions:
Toward Sensor and Catalyst Design
posted on 2024-03-08, 15:38authored byMárton Guba, Tibor Höltzl
Here, we present a detailed computational study of the
stability
and the electronic structure of nitrogen-doped graphene (N4V2) supported Cun (n = 1–5) clusters, which are promising carbon-dioxide
electroreduction catalysts. The binding of the clusters to the nitrogen-doped
graphene and the electronic structure of these systems were investigated
under vacuum and electrochemical conditions. The stability analysis
showed that among the systems, the nitrogen-doped graphene bound Cu4 is the most stable in vacuum, while in an electrolyte, and
at a negative potential, the N4V2–Cu3 is energetically more favorable. The ground state electronic
structure of the nitrogen-doped graphene substrate undergoes topological
phase transition, from a semimetallic state, and we observed a metallic
and topologically trivial state after the clusters are deposited.
The electrode potential adjusts the type and density of the charge
carriers in the semimetallic models, while the structures containing
copper exhibit bands which are deformed and relaxed by the modified
number of electrons.