Campus Units

Physics and Astronomy, Ames Laboratory

Document Type

Article

Publication Version

Submitted Manuscript

Publication Date

11-19-2020

Journal or Book Title

The Journal of Physical Chemistry Letters

Volume

11

Issue

22

First Page

9725

Last Page

9730

DOI

10.1021/acs.jpclett.0c02887

Abstract

The thermodynamic preference of a foreign atom for adsorption on versus intercalation into a graphitic surface is of fundamental and widespread interest. From an exhaustive first-principles density functional theory investigation for 38 typical elements over the periodic table, we reveal a quasilinear correlation between the Shannon effective ionic radius and the chemical-potential difference for a single atom from adsorption to intercalation at multilayer graphene surfaces. A critical Shannon radius is found to be around 0.10 nm, below (above) which intercalation (adsorption) is more favorable for elements with ionic-like bonding after intercalation. Single atoms with van der Waals-biased bonding show some deviation from the linear relationship, while single atoms for the elements with covalent-like bonding do not favor intercalation relative to adsorption. An energy decomposition analysis indicates that the chemical-potential difference determining the thermodynamic preference of a foreign atom for adsorption versus intercalation results from the competition between the electronic and elastic strain effects.

Comments

This document is the unedited Author’s version of a Submitted Work that was subsequently accepted for publication in The Journal of Physical Chemistry Letters, copyright © American Chemical Society after peer review. To access the final edited and published work see DOI: 10.1021/acs.jpclett.0c02887. Posted with permission.

Copyright Owner

American Chemical Society

Language

en

File Format

application/pdf

Published Version

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