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Computational Modelling of Pyrrolic MN4 Motifs Embedded in Graphene for Catalyst Design

Low, Jian Liang and Paulus, Beate – 2023

Carbon-based materials doped with metal and nitrogen (M-N-Cs) have promising potential in electrocatalytic applications with the advantage of material sustainability. MN4 motifs incorporated into a carbon lattice are generally known to be responsible for the activity of these materials. While many computational studies assume the tetrapyridinic MN4 motifs, recent studies have elucidated the role of tetrapyrrolic MN4 motifs in electrocatalysis. Using density functional theory, we constructed and compared various structural models to study the incorporation of tetrapyrrolic and tetrapyridinic MN4 motifs in 2D carbon materials and analyzed the type of interactions between each metal species and the N4 site. We further quantified the relative affinity of various metal species to the two types of N4 site. Upon analysis of energies, bond lengths, electronic population and charges, we found that metals that exhibit highly ionic binding characters have a greater affinity towards tetrapyrrolic MN4 motifs compared to species that participate in covalent interactions with the π-system. Furthermore, the binding strength of each species in the N4 site depend on the electronegativity as well as the availability of orbitals for accepting electrons from the π-system.

Title
Computational Modelling of Pyrrolic MN4 Motifs Embedded in Graphene for Catalyst Design
Author
Low, Jian Liang and Paulus, Beate
Date
2023
Identifier
DOI: 10.3390/catal13030566
Source(s)
Citation
Catalysts 2023, 13, 566.