Enhanced gas adsorption on graphitic substrates via defects and local curvature: A density functional theory study
Abstract
Using van-der-Waals-corrected density functional theory calculations, we explore the possibility of engineering the local structure and morphology of high-surface-area graphene-derived materials to improve the uptake of methane and carbon dioxide for gas storage and sensing. We test the sensitivity of the gas adsorption energy to the introduction of native point defects, curvature, and the application of strain. The binding energy at topological point defect sites is inversely correlated with the number of missing carbon atoms, causing Stone–Wales defects to show the largest enhancement with respect to pristine graphene (~20%). Improvements of similar magnitude are observed at concavely curved surfaces in buckled graphene sheets under compressive strain, whereas tensile strain tends to weaken gas binding. Trends for CO2 and CH4 are similar, although CO2 binding is generally stronger by ~4 to 5 kJ mol–1. Furthermore, the differential between the adsorption of CO2 and CH4 is much higher on folded graphene sheets and at concave curvatures; this could possibly be leveraged for CH4/CO2 flow separation and gas-selective sensors.
- Authors:
-
- Indian Institute of Science, Bangalore (India)
- Jawaharlal Nehru Centre for Advanced Scientific Research, Bangalore (India); Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
- Jawaharlal Nehru Centre for Advanced Scientific Research, Bangalore (India)
- Publication Date:
- Research Org.:
- Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1325864
- Report Number(s):
- LLNL-JRNL-643967
Journal ID: ISSN 1932-7447
- Grant/Contract Number:
- AC52-07NA27344
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Physical Chemistry. C
- Additional Journal Information:
- Journal Volume: 118; Journal Issue: 15; Journal ID: ISSN 1932-7447
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; 77 NANOSCIENCE AND NANOTECHNOLOGY; 03 NATURAL GAS; 37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; 25 ENERGY STORAGE
Citation Formats
Dutta, Debosruti, Wood, Brandon C., Bhide, Shreyas Y., Ayappa, K. Ganapathy, and Narasimhan, Shobhana. Enhanced gas adsorption on graphitic substrates via defects and local curvature: A density functional theory study. United States: N. p., 2014.
Web. doi:10.1021/jp411338a.
Dutta, Debosruti, Wood, Brandon C., Bhide, Shreyas Y., Ayappa, K. Ganapathy, & Narasimhan, Shobhana. Enhanced gas adsorption on graphitic substrates via defects and local curvature: A density functional theory study. United States. https://doi.org/10.1021/jp411338a
Dutta, Debosruti, Wood, Brandon C., Bhide, Shreyas Y., Ayappa, K. Ganapathy, and Narasimhan, Shobhana. Mon .
"Enhanced gas adsorption on graphitic substrates via defects and local curvature: A density functional theory study". United States. https://doi.org/10.1021/jp411338a. https://www.osti.gov/servlets/purl/1325864.
@article{osti_1325864,
title = {Enhanced gas adsorption on graphitic substrates via defects and local curvature: A density functional theory study},
author = {Dutta, Debosruti and Wood, Brandon C. and Bhide, Shreyas Y. and Ayappa, K. Ganapathy and Narasimhan, Shobhana},
abstractNote = {Using van-der-Waals-corrected density functional theory calculations, we explore the possibility of engineering the local structure and morphology of high-surface-area graphene-derived materials to improve the uptake of methane and carbon dioxide for gas storage and sensing. We test the sensitivity of the gas adsorption energy to the introduction of native point defects, curvature, and the application of strain. The binding energy at topological point defect sites is inversely correlated with the number of missing carbon atoms, causing Stone–Wales defects to show the largest enhancement with respect to pristine graphene (~20%). Improvements of similar magnitude are observed at concavely curved surfaces in buckled graphene sheets under compressive strain, whereas tensile strain tends to weaken gas binding. Trends for CO2 and CH4 are similar, although CO2 binding is generally stronger by ~4 to 5 kJ mol–1. Furthermore, the differential between the adsorption of CO2 and CH4 is much higher on folded graphene sheets and at concave curvatures; this could possibly be leveraged for CH4/CO2 flow separation and gas-selective sensors.},
doi = {10.1021/jp411338a},
journal = {Journal of Physical Chemistry. C},
number = 15,
volume = 118,
place = {United States},
year = {Mon Mar 24 00:00:00 EDT 2014},
month = {Mon Mar 24 00:00:00 EDT 2014}
}
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