Shifting the scaling relations of single-atom catalysts for facile methane activation by tuning the coordination number

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We investigate oxidative methane activation on a wide range of single transition metal atom catalysts embedded on N-doped graphene derivatives using density functional theory calculations. An inverse scaling relationship between *O formation and its hydrogen affinity is observed, consistent with a previous report. However, we find that the latter scaling line can be shifted towards a more reactive region by tuning the coordination number (CN) of the active metal sites. Specifically, we find that lowering the CN plays an important role in increasing the reactivity for methane activation via a radical-like transition state by moving the scaling lines. Thus, in the new design strategy suggested here, different from the conventional efforts focusing mainly on breaking the scaling relations, one maintains the scaling relations but moves them towards more reactive regions by controlling the coordination number of the active sites. With this design principle, we suggest several single atom catalysts with lower C-H activation barriers than some of the most active methane activation catalysts in the literature such as Cu-based zeolites.
Publisher
ROYAL SOC CHEMISTRY
Issue Date
2021-03
Language
English
Article Type
Article
Citation

CHEMICAL SCIENCE, v.12, no.10, pp.3551 - 3557

ISSN
2041-6520
DOI
10.1039/d0sc05632d
URI
http://hdl.handle.net/10203/282378
Appears in Collection
CBE-Journal Papers(저널논문)
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