Issue 10, 2021

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

Abstract

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.

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

Supplementary files

Article information

Article type
Edge Article
Submitted
12 Okt 2020
Accepted
11 Jan 2021
First published
12 Jan 2021
This article is Open Access

All publication charges for this article have been paid for by the Royal Society of Chemistry
Creative Commons BY-NC license

Chem. Sci., 2021,12, 3551-3557

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

C. Choi, S. Yoon and Y. Jung, Chem. Sci., 2021, 12, 3551 DOI: 10.1039/D0SC05632D

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