dc.contributor.author
Low, Jian Liang
dc.contributor.author
Paulus, Beate
dc.date.accessioned
2023-03-30T15:34:12Z
dc.date.available
2023-03-30T15:34:12Z
dc.identifier.uri
https://refubium.fu-berlin.de/handle/fub188/38690
dc.identifier.uri
http://dx.doi.org/10.17169/refubium-38406
dc.description.abstract
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.
en
dc.format.extent
12 Seiten
dc.rights.uri
https://creativecommons.org/licenses/by/4.0/
dc.subject
single-atom catalyst
en
dc.subject
carbon material
en
dc.subject
density functional theory
en
dc.subject
pyrrolic and pyridinicMN4
en
dc.subject.ddc
500 Naturwissenschaften und Mathematik::540 Chemie::540 Chemie und zugeordnete Wissenschaften
dc.title
Computational Modelling of Pyrrolic MN4 Motifs Embedded in Graphene for Catalyst Design
dc.type
Wissenschaftlicher Artikel
dcterms.bibliographicCitation.articlenumber
566
dcterms.bibliographicCitation.doi
10.3390/catal13030566
dcterms.bibliographicCitation.journaltitle
Catalysts
dcterms.bibliographicCitation.number
3
dcterms.bibliographicCitation.originalpublishername
MDPI
dcterms.bibliographicCitation.volume
13
dcterms.bibliographicCitation.url
https://doi.org/10.3390/catal13030566
refubium.affiliation
Biologie, Chemie, Pharmazie
refubium.affiliation.other
Institut für Chemie und Biochemie
refubium.resourceType.isindependentpub
no
dcterms.accessRights.openaire
open access
dcterms.isPartOf.eissn
2073-4344