Thermodynamic Preference for Atom Adsorption on versus Intercalation into Multilayer Graphene
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.
- Authors:
-
[1];
[2];
[2];
[2]
- Southern Univ. of Science and Technology, Guangdong (China)
- Ames Lab., Ames, IA (United States); Iowa State Univ., Ames, IA (United States)
- Publication Date:
- Research Org.:
- Ames Lab., Ames, IA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
- Sponsoring Org.:
- National Natural Science Foundation of China (NSFC); Shenzhen Basic Research Fund; USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; National Science Foundation (NSF)
- OSTI Identifier:
- 1727437
- Report Number(s):
- IS-J-10,371
Journal ID: ISSN 1948-7185
- Grant/Contract Number:
- AC02-07CH11358; 11774142; JCYJ20170817105132549; JCYJ20180504165817769; JCYJ20170817105201098; AC02-05CH11231; ACI-1548562
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Physical Chemistry Letters
- Additional Journal Information:
- Journal Volume: 11; Journal Issue: 22; Journal ID: ISSN 1948-7185
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Li, Wei, Huang, Li, Tringides, Michael C., Evans, James W., and Han, Yong. Thermodynamic Preference for Atom Adsorption on versus Intercalation into Multilayer Graphene. United States: N. p., 2020.
Web. doi:10.1021/acs.jpclett.0c02887.
Li, Wei, Huang, Li, Tringides, Michael C., Evans, James W., & Han, Yong. Thermodynamic Preference for Atom Adsorption on versus Intercalation into Multilayer Graphene. United States. https://doi.org/10.1021/acs.jpclett.0c02887
Li, Wei, Huang, Li, Tringides, Michael C., Evans, James W., and Han, Yong. Mon .
"Thermodynamic Preference for Atom Adsorption on versus Intercalation into Multilayer Graphene". United States. https://doi.org/10.1021/acs.jpclett.0c02887. https://www.osti.gov/servlets/purl/1727437.
@article{osti_1727437,
title = {Thermodynamic Preference for Atom Adsorption on versus Intercalation into Multilayer Graphene},
author = {Li, Wei and Huang, Li and Tringides, Michael C. and Evans, James W. and Han, Yong},
abstractNote = {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.},
doi = {10.1021/acs.jpclett.0c02887},
journal = {Journal of Physical Chemistry Letters},
number = 22,
volume = 11,
place = {United States},
year = {Mon Nov 02 00:00:00 EST 2020},
month = {Mon Nov 02 00:00:00 EST 2020}
}
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