Clustering of metal dopants in defect sites of graphene-based materials

Single-atom catalysts are promising candidates for many industrial reactions. However, making true single-atom catalysts is an experimental dilemma, due to the difficulty of keeping dopant single atoms stable at temperature and under pressure. This difficulty can lead to clustering of the metal dopa...

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Bibliographic Details
Published in:Physical chemistry chemical physics : PCCP 2021-12, Vol.24 (1), p.98-111
Main Authors: Lambie, Stephanie, Steenbergen, Krista G, Gaston, Nicola, Paulus, Beate
Format: Article
Language:English
Subjects:
Clustering
Dopants
Electronic structure
Graphene
Single atom catalysts
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Summary:Single-atom catalysts are promising candidates for many industrial reactions. However, making true single-atom catalysts is an experimental dilemma, due to the difficulty of keeping dopant single atoms stable at temperature and under pressure. This difficulty can lead to clustering of the metal dopant atoms in defect sites. However, the electronic and geometric structure of sub-nanoscale clusters in single-atom defects has not yet been explored. Furthermore, recent studies have proven sub-nanoscale clusters of dopants in single-atom defect sites can be equally good or better catalysts than their single-atom counterparts. Here, a comprehensive DFT study is undertaken to determine the geometric and electronic structure effects that influence clustering of noble and p-block dopants in C 3 - and N 4 -defect sites in graphene-based systems. We find that the defect site is the primary driver in determining clustering dynamics in these systems. Selected defect sites in graphene thermodynamically favour single atom doping over clustering, when doped with noble and p-block elements.
ISSN:1463-9076
1463-9084
DOI:10.1039/d1cp05008g