Gas Separation in Nanoporous Graphene from First Principle Calculations

Ambrosetti, Alberto; Silvestrelli, Pier Luigi

doi:10.1021/jp504914u

Cited by 68Membrane Separation and Gas TransportNanopore and Nanochannel Transport StudiesGraphene research and applications

Gas Separation in Nanoporous Graphene from First Principle Calculations

Ambrosetti, Alberto, Silvestrelli, Pier Luigi·2014·The Journal of Physical Chemistry C

DOI 10.1021/jp504914u

Open this paper in CoChat — free account

Abstract

Thanks to its single atom thickness and its mechanical strength, nanoporous graphene is currently being regarded as a promising candidate for efficient and reliable gas separation applications. Clearly, the accurate energetic characterization of the penetration processes involving relevant gas-phase molecules is a fundamental prerequisite for any possible application. Here we evaluate permeation barriers and adsorption energies of the H 2 O, CH 4, CO, CO 2, O 2, and H 2 molecules and of the Ar atom on two types of hydrogen saturated pores by means of ab initio simulations, based on the density functional theory (DFT), able to include dispersion corrections too. We find that, although the qualitative trend followed by the values of the permeation barriers of the considered molecules is independent of the adopted DFT functional, at a quantitative level the results are noticeably affected by the dispersion corrections and the chosen exchange contribution characterizing the different functionals, as well as by the allowed graphene sheet distortions. Interestingly, we observe that, due to the occurrence of nontrivial H-bond interactions with the pore-saturating H atoms, the permeation barrier of water remains low even considering a small-size pore. The barrier is further diminished when considering the interaction with a second water molecule on the opposite side of the pore. These observations, combined with the relatively strong binding of the water molecule with the defected surface, suggests that porous graphene could also represent a promising membrane for water filtration.

Integrity signals

Registry

Crossref · 10.1021/jp504914u

Cites

61 of 61 references verified0 citation errors · 0 not checkable

Statistics

Recomputing p-values needs the paper’s full text.

Claims the paper makes

This paper’s full text isn’t openly available, so its claims and self-check weren’t run. The registry and citation checks still apply.

Generalized Gradient Approximation Made Simple
Perdew, J. P., Burke, K., & Ernzerhof, M. (1996) · Physical Review Letters · doi:10.1103/physrevlett.77.3865 · Cited by 215,824 · see citing works
Electric Field Effect in Atomically Thin Carbon Films
Novoselov, K. S., Geim, A. K., Morozov, S. V., Jiang, D., Zhang, Y., Dubonos, S. V., Grigorieva, I. V., & Firsov, A. A. (2004) · Science · doi:10.1126/science.1102896 · Cited by 66,834 · see citing works
A consistent and accurate <i>ab initio</i> parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-Pu
Grimme, S., Antony, J., Ehrlich, S., & Krieg, H. (2010) · The Journal of Chemical Physics · doi:10.1063/1.3382344 · Cited by 59,686 · see citing works
QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials
Giannozzi, P., Stefano Baroni, A., Bonini, N., Calandra, M., Car, R., Cavazzoni, C., Ceresoli, D., Chiarotti, G., Cococcioni, M., Dabo, I., et al. (2009) · Journal of Physics Condensed Matter · doi:10.1088/0953-8984/21/39/395502 · Cited by 29,336 · see citing works
Accurate and simple analytic representation of the electron-gas correlation energy
Perdew, J. P., & Wang, Y. (1992) · Physical review. B, Condensed matter · doi:10.1103/physrevb.45.13244 · Cited by 25,009 · see citing works
Toward reliable density functional methods without adjustable parameters: The PBE0 model
Adamo, C., & Barone, V. (1999) · The Journal of Chemical Physics · doi:10.1063/1.478522 · Cited by 19,137 · see citing works
Van der Waals Density Functional for General Geometries
Dion, M., Rydberg, H., Schröder, E., Langreth, D. C., & Lundqvist, B. I. (2004) · Physical Review Letters · doi:10.1103/physrevlett.92.246401 · Cited by 5,631 · see citing works
Van der Waals density functionals applied to solids
Klimeš, J., Bowler, D. R., & Michaelides, A. (2011) · Physical Review B · doi:10.1103/physrevb.83.195131 · Cited by 4,624 · see citing works
Chemical accuracy for the van der Waals density functional
Klimeš, J., Bowler, D. R., & Michaelides, A. (2010) · Journal of Physics: Condensed Matter · doi:10.1088/0953-8984/22/2/022201 · Cited by 3,587 · see citing works
Maximally localized Wannier functions: Theory and applications
Marzari, N., Mostofi, A. A., Yates, J. R., Souza, I., & Vanderbilt, D. (2012) · Reviews of Modern Physics · doi:10.1103/revmodphys.84.1419 · Cited by 3,283 · see citing works
Comment on “Generalized Gradient Approximation Made Simple”
Zhang, Y., & Yang, W. (1998) · Physical Review Letters · doi:10.1103/physrevlett.80.890 · Cited by 2,937 · see citing works
Impermeable Atomic Membranes from Graphene Sheets
Bunch, J. S., Verbridge, S. S., Alden, J. S., van der Zande, A. M., Parpia, J. M., Craighead, H. G., & McEuen, P. L. (2008) · Nano Letters · doi:10.1021/nl801457b · Cited by 2,929 · see citing works
Higher-accuracy van der Waals density functional
Lee, K., Murray, É., Kong, L., Lundqvist, B. I., & Langreth, D. C. (2010) · Physical Review B · doi:10.1103/physrevb.82.081101 · Cited by 2,765 · see citing works
Classical and Quantum Dynamics in Condensed Phase Simulations
(1998) · doi:10.1142/3816 · Cited by 2,284 · see citing works
Water Desalination across Nanoporous Graphene
Cohen‐Tanugi, D., & Grossman, J. C. (2012) · Nano Letters · doi:10.1021/nl3012853 · Cited by 2,206 · see citing works
Membrane Gas Separation: A Review/State of the Art
Bernardo, P., Drioli, E., & Golemme, G. (2009) · Industrial & Engineering Chemistry Research · doi:10.1021/ie8019032 · Cited by 2,160 · see citing works
Perspective on density functional theory
Burke, K. (2012) · The Journal of Chemical Physics · doi:10.1063/1.4704546 · Cited by 1,758 · see citing works
An improved simple model for the van der Waals potential based on universal damping functions for the dispersion coefficients
Tang, K. T., & Toennies, J. P. (1984) · The Journal of Chemical Physics · doi:10.1063/1.447150 · Cited by 1,630 · see citing works
Nonlocal van der Waals density functional: The simpler the better
Vydrov, O. A., & Voorhis, T. V. (2010) · The Journal of Chemical Physics · doi:10.1063/1.3521275 · Cited by 1,314 · see citing works
Porous Graphene as the Ultimate Membrane for Gas Separation
Jiang, D., Cooper, V. R., & Dai, S. (2009) · Nano Letters · doi:10.1021/nl9021946 · Cited by 946 · see citing works
Ultimate Permeation Across Atomically Thin Porous Graphene
Çelebi, K., Buchheim, J., Wyss, R. M., Droudian, A., Gasser, P., Shorubalko, I., Kye, J.-I., Lee, C.-H., & Park, H. G. (2014) · Science · doi:10.1126/science.1249097 · Cited by 912 · see citing works
Selective Ionic Transport through Tunable Subnanometer Pores in Single-Layer Graphene Membranes
O’Hern, S. C., Boutilier, M. S. H., Idrobo, J. C., et al. (2014) · Nano Letters · doi:10.1021/nl404118f · Cited by 819 · see citing works
Induced Magnetic Ordering by Proton Irradiation in Graphite
Esquinazi, P. D., Spemann, D., Höhne, R., Setzer, A., Han, K. ‐., & Butz, T. (2003) · Physical Review Letters · doi:10.1103/physrevlett.91.227201 · Cited by 815 · see citing works
Nonlocal van der Waals density functional made simple and efficient
Sabatini, R., Gorni, T., & de Gironcoli, S. (2013) · Physical Review B · doi:10.1103/physrevb.87.041108 · Cited by 717 · see citing works
Long-range correlation energy calculated from coupled atomic response functions
Ambrosetti, A., Reilly, A. M., DiStasio, R. A., & Tkatchenko, A. (2014) · The Journal of Chemical Physics · doi:10.1063/1.4865104 · Cited by 664 · see citing works
Self-citation
Irradiation-Induced Magnetism in Graphite: A Density Functional Study
Lehtinen, P. O., Foster, A. S., Ma, Y., Krasheninnikov, A. V., & Nieminen, R. M. (2004) · Physical Review Letters · doi:10.1103/physrevlett.93.187202 · Cited by 658 · see citing works
Selective Ion Passage through Functionalized Graphene Nanopores
Sint, K., Wang, B., & Král, P. (2008) · Journal of the American Chemical Society · doi:10.1021/ja804409f · Cited by 623 · see citing works
Electron beam nanosculpting of suspended graphene sheets
Fischbein, M. D., & Drndić, M. (2008) · Applied Physics Letters · doi:10.1063/1.2980518 · Cited by 608 · see citing works
Long-range correlation energy calculated from coupled atomic response functions
Ambrosetti, A., Reilly, A., DiStasio, R., & Tkatchenko, A. (2014) · Max Planck Digital Library · Cited by 580 · see citing works
Self-citation
Density-Functional Theory with Screened van der Waals Interactions for the Modeling of Hybrid Inorganic-Organic Systems
Ruiz, V. G., Liu, W., Zojer, E., Scheffler, M., & Tkatchenko, A. (2012) · Physical Review Letters · doi:10.1103/physrevlett.108.146103 · Cited by 558 · see citing works
From Microporous Regular Frameworks to Mesoporous Materials with Ultrahigh Surface Area: Dynamic Reorganization of Porous Polymer Networks
Kuhn, P., Forget, A., Su, D., et al. (2008) · Journal of the American Chemical Society · doi:10.1021/ja803708s · Cited by 556 · see citing works
Long-range–short-range separation of the electron-electron interaction in density-functional theory
Toulouse, J., Colonna, F., & Savin, A. (2004) · Physical Review A · doi:10.1103/physreva.70.062505 · Cited by 465 · see citing works
Separation of Hydrogen and Nitrogen Gases with Porous Graphene Membrane
Du, H., Li, J., Zhang, J., Su, G., Li, X., & Zhao, Y. (2011) · The Journal of Physical Chemistry C · doi:10.1021/jp206258u · Cited by 383 · see citing works
Porous Graphene as an Atmospheric Nanofilter
Blankenburg, S., Bieri, M., Fasel, R., Müllen, K., Pignedoli, C. A., & Passerone, D. (2010) · Small · doi:10.1002/smll.201001126 · Cited by 372 · see citing works
Investigation of Exchange Energy Density Functional Accuracy for Interacting Molecules
Murray, É., Lee, K., & Langreth, D. C. (2009) · Journal of Chemical Theory and Computation · doi:10.1021/ct900365q · Cited by 323 · see citing works
Benchmarking Density Functional Methods against the S66 and S66x8 Datasets for Non‐Covalent Interactions
Goerigk, L., Kruse, H., & Grimme, S. (2011) · ChemPhysChem · doi:10.1002/cphc.201100826 · Cited by 321 · see citing works
Scaling laws for van der Waals interactions in nanostructured materials
Gobre, V. V., & Tkatchenko, A. (2013) · Nature Communications · doi:10.1038/ncomms3341 · Cited by 301 · see citing works
Benzene adsorbed on metals: Concerted effect of covalency and van der Waals bonding
Liu, W., Carrasco, J., Santra, B., et al. (2012) · Physical Review B · doi:10.1103/physrevb.86.245405 · Cited by 285 · see citing works
Helium Separation Using Porous Graphene Membranes
Schrier, J. (2010) · The Journal of Physical Chemistry Letters · doi:10.1021/jz100748x · Cited by 257 · see citing works
Van der Waals Interactions in DFT Made Easy by Wannier Functions
Silvestrelli, P. L. (2008) · Physical Review Letters · doi:10.1103/physrevlett.100.053002 · Cited by 213 · see citing works
Self-citation
Theory of hydrogen permeability in nonporous silica membranes
Oyama, S. T., Lee, D., Hacarlioglu, P., et al. (2004) · Journal of Membrane Science · doi:10.1016/j.memsci.2004.06.046 · Cited by 199 · see citing works
Hard Numbers for Large Molecules: Toward Exact Energetics for Supramolecular Systems
Ambrosetti, A., Alfè, D., DiStasio, R. A., & Tkatchenko, A. (2014) · The Journal of Physical Chemistry Letters · doi:10.1021/jz402663k · Cited by 184 · see citing works
Self-citation
Insight into the description of van der Waals forces for benzene adsorption on transition metal (111) surfaces
Carrasco, J., Liu, W., Michaelides, A., et al. (2014) · The Journal of Chemical Physics · doi:10.1063/1.4866175 · Cited by 183 · see citing works
Interatomic methods for the dispersion energy derived from the adiabatic connection fluctuation-dissipation theorem
Tkatchenko, A., Ambrosetti, A., & DiStasio, R. A. (2013) · The Journal of Chemical Physics · doi:10.1063/1.4789814 · Cited by 170 · see citing works
Self-citation
Nanoporous Graphene Membranes for Efficient 3 He/ 4 He Separation
Hauser, A., & Schwerdtfeger, P. (2011) · The Journal of Physical Chemistry Letters · doi:10.1021/jz201504k · Cited by 166 · see citing works
Fluorine-Modified Porous Graphene as Membrane for CO2/N2 Separation: Molecular Dynamic and First-Principles Simulations
Wu, T., Xue, Q., Ling, C., et al. (2014) · The Journal of Physical Chemistry C · doi:10.1021/jp4096776 · Cited by 134 · see citing works
Methane-selective nanoporous graphene membranes for gas purification
Hauser, A., & Schwerdtfeger, P. (2012) · Physical Chemistry Chemical Physics · doi:10.1039/c2cp41889d · Cited by 133 · see citing works
Adsorption of Rare-Gas Atoms and Water on Graphite and Graphene by van der Waals-Corrected Density Functional Theory
Ambrosetti, A., & Silvestrelli, P. L. (2011) · The Journal of Physical Chemistry C · doi:10.1021/jp110669p · Cited by 121 · see citing works
Self-citation
Interatomic methods for the dispersion energy derived from the adiabatic connection fluctuation-dissipation theorem
Tkatchenko, A., Ambrosetti, A., & DiStasio, R. (2013) · MPG.PuRe (Max Planck Society) · Cited by 109 · see citing works
Self-citation
Penetration Barrier of Water through Graphynes’ Pores: First-Principles Predictions and Force Field Optimization
Bartolomei, M., Carmona-Novillo, E., Hernández, M. I., et al. (2014) · The Journal of Physical Chemistry Letters · doi:10.1021/jz4026563 · Cited by 97 · see citing works
Molecular switches from benzene derivatives adsorbed on metal surfaces
Liu, W., Filimonov, S. N., Carrasco, J., & Tkatchenko, A. (2013) · Nature Communications · doi:10.1038/ncomms3569 · Cited by 88 · see citing works
Separation of the hydrogen sulfide and methane mixture by the porous graphene membrane: Effect of the charges
Lei, G., Liu, C., Xie, H., et al. (2014) · Chemical Physics Letters · doi:10.1016/j.cplett.2014.03.040 · Cited by 71 · see citing works
Including screening in van der Waals corrected density functional theory calculations: the case of atoms and small molecules physisorbed on graphene.
Silvestrelli, P., & Ambrosetti, A. (2014) · Journal of Chemical Physics · doi:10.1063/1.4869330 · Cited by 58 · see citing works
Self-citation
Graphene with line defect as a membrane for gas separation: Design via a first-principles modeling
Qin, X., Meng, Q., Feng, Y. P., et al. (2012) · Surface Science · doi:10.1016/j.susc.2012.08.024 · Cited by 54 · see citing works
van der Waals interactions in density functional theory using Wannier functions: Improved C6 and C3 coefficients by a different approach
Ambrosetti, A., & Silvestrelli, P. L. (2012) · Physical Review B · doi:10.1103/physrevb.85.073101 · Cited by 44 · see citing works
Self-citation
Van der Waals interactions in density functional theory by combining the quantum harmonic oscillator-model with localized Wannier functions
Silvestrelli, P. L. (2013) · The Journal of Chemical Physics · doi:10.1063/1.4816964 · Cited by 40 · see citing works
Self-citation
Hydrogen saturation stabilizes vacancy-induced ferromagnetic ordering in graphene
Li, W., Zhao, M., Zhao, X., et al. (2010) · Physical Chemistry Chemical Physics · doi:10.1039/c003524f · Cited by 35 · see citing works
Geometry, Energetics, and Dynamics of Hydrogen Bonds in Proteins: Structural Information Derived from NMR Scalar Couplings
Gsponer, J., Hopearuoho, H., Cavalli, A., et al. (2006) · Journal of the American Chemical Society · doi:10.1021/ja0614722 · Cited by 32 · see citing works
van der Waals-Corrected Ab Initio Study of Water Ice–Graphite Interaction
Ambrosetti, A., Ancilotto, F., & Silvestrelli, P. L. (2012) · The Journal of Physical Chemistry C · doi:10.1021/jp309617f · Cited by 29 · see citing works
Self-citation
Creation and dynamics of remote spin-entangled pairs in the expansion of strongly correlated fermions in an optical lattice
Keßler, S., McCulloch, I. P., & Marquardt, F. (2013) · New Journal of Physics · doi:10.1088/1367-2630/15/5/053043 · Cited by 21 · see citing works
First-Principles Study of Water Ice Adsorption on the Methyl-Terminated Si(111) Surface
Ambrosetti, A., Costanzo, F., & Silvestrelli, P. L. (2011) · The Journal of Physical Chemistry C · doi:10.1021/jp202704c · Cited by 9 · see citing works
Self-citation

Flagged first, then by citations

Slowing single-stranded DNA translocation through a solid-state nanopore by decreasing the nanopore diameter
Akahori, R., Haga, T., Hatano, T., et al. (2014) · Nanotechnology · doi:10.1088/0957-4484/25/27/275501 · Cited by 77 · see citing works
Selectively detecting attomolar concentrations of proteins using gold lined nanopores in a nanopore blockade sensor
Wu, Y., Yao, Y., Cheong, S., et al. (2020) · Chemical Science · doi:10.1039/d0sc04552g · Cited by 41 · see citing works
Nanoporous Metal Template Methods
Qin, K. (2022) · doi:10.1002/9783527822089.ch3
SDS-assisted protein transport through solid-state nanopores
Restrepo-Pérez, L., John, S., Aksimentiev, A., et al. (2017) · Nanoscale · doi:10.1039/c7nr02450a · Cited by 84 · see citing works
Effect of nanopore size on poly(dT)30 translocation through silicon nitride membrane
Si, W., Sha, J., Liu, L., et al. (2013) · Science China Technological Sciences · doi:10.1007/s11431-013-5330-2 · Cited by 22 · see citing works

Authors: Ambrosetti, A., & Silvestrelli, P. L.
Affiliations: University of Padua (IT)
Corresponding author: Ambrosetti, Alberto
ORCID: Ambrosetti, Alberto
Silvestrelli, Pier Luigi
Venue: The Journal of Physical Chemistry C
Publisher: American Chemical Society (ACS)
Published: 2014-08-13
Volume: 118
Issue: 33
Pages: 19172-19179
ISSN: 1932-7447 (ISSN-L)
1932-7455
DOI: 10.1021/jp504914u
OpenAlex: W2073625297
Cited by: 68
References: 61
Citations by year: 2026: 1 · 2025: 3 · 2024: 1 · 2023: 4 · 2022: 5 · 2021: 7 · 2020: 4 · 2019: 9 · 2018: 5 · 2017: 9 · 2016: 10 · 2015: 8 · 2014: 2
FWCI: 11.28
Type: journal article
Language: en
Open access: closed
Locations: The Journal of Physical Chemistry C (publishedVersion)
Padua Research Archive (University of Padova) (submittedVersion)
Funders: Ministero dell'Istruzione, dell'Universit? e della Ricerca
Topics: Physical Sciences › Engineering › Mechanical Engineering › Membrane Separation and Gas Transport
Physical Sciences › Engineering › Biomedical Engineering › Nanopore and Nanochannel Transport Studies
Physical Sciences › Materials Science › Materials Chemistry › Graphene research and applications
Keywords: nanoporous graphene, gas separation, adsorption energy, water permeation, water filtration membranes, dispersion correction, exchange-correlation functionals, hydrogen bonding, methane, carbon dioxide, oxygen, hydrogen, argon

About these checks

Registry, retraction, Cites and statistics results are computed, not judged, with one exception: a printed reference that no index lists is read once by a model before it counts as a citation error. Claims are extracted by a model and kept only when their quote appears verbatim in the text; each cited source is then checked, with a model’s help, for whether it says what the claim relies on. Those verdicts can be wrong — read the claim’s quote and the cited source before relying on one.

Statistics and arithmetic are recomputed, not judged.

Confidence bands are shown only for fields calibrated on our annotated test set. None is calibrated yet, so no band is shown.

What counts as a claim ›How we measure confidence ›How we check this ›

Are you an author, or do you see a problem with this page? Request a review

Gas Separation in Nanoporous Graphene from First Principle Calculations

Abstract

Integrity signals

Claims the paper makes

Cites

Related

Record

About these checks