Ultrafast molecular transport on carbon surfaces: The diffusion of ammonia on graphite

Tamtögl, Anton; Sacchi, M.; Calvo-Almazán, I.; Zbiri, M.; Koza, M. M.; Ernst, W. E.; Fouquet, P.

doi:10.1016/j.carbon.2017.09.104

Title: Ultrafast molecular transport on carbon surfaces: The diffusion of ammonia on graphite

Journal Article · 30 September 2018 · Carbon

DOI: https://doi.org/10.1016/j.carbon.2017.09.104 · OSTI ID:1476645

^[1]; Sacchi, M. ^[2]; Calvo-Almazán, I. ^[3]; Zbiri, M. ^[4]; Koza, M. M. ^[4]; Ernst, W. E. ^[1]; Fouquet, P. ^[4]

Graz Univ. of Technology (Austria)
Univ. of Surrey, Guildford (United Kingdom)
Argonne National Lab. (ANL), Argonne, IL (United States); Univ. of Cambridge (United Kingdom). Cavendish Lab.
Inst. Laue-Langevin (ILL), Grenoble (France)

We present a combined experimental and theoretical study of the self-diffusion of ammonia on exfoliated graphite. Using neutron time-of-flight spectroscopy we are able to resolve the ultrafast diffusion process of adsorbed ammonia, NH₃, on graphite. Together with van der Waals corrected density functional theory calculations we show that the diffusion of NH₃ follows a hopping motion on a weakly corrugated potential energy surface with an activation energy of about 4 meV which is particularly low for this type of diffusive motion. The hopping motion includes further a significant number of long jumps and the diffusion constant of ammonia adsorbed on graphite is determined with D = 3.9•10^-8 m²/s at 94 K.

View Accepted Manuscript (DOE)

Cite

Export

Save

Research Organization:: Argonne National Lab. (ANL), Argonne, IL (United States)

Sponsoring Organization:: Engineering and Physical Sciences Research Council (EPSRC); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1476645

Journal Information:: Carbon, Journal Name: Carbon Journal Issue: C Vol. 126; ISSN 0008-6223

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

References (64)

Diffusion coefficients of small molecules at the gas-solid interface as measured by the nuclear magnetic resonance pulsed field gradient method Tabony, J.; Cosgrove, T. Chemical Physics Letters, Vol. 67, Issue 1 https://doi.org/10.1016/0009-2614(79)87115-8	journal	November 1979
Nuclear magnetic resonance studies of molecules physisorbed on homogeneous surfaces Tabony, J. Progress in Nuclear Magnetic Resonance Spectroscopy, Vol. 14, Issue 1 https://doi.org/10.1016/0079-6565(80)80001-X	journal	January 1980
Neutron scattering from adsorbed systems Thomas, R. K. Progress in Solid State Chemistry, Vol. 14, Issue 1-2 https://doi.org/10.1016/0079-6786(82)90002-4	journal	January 1982
Effects of low-dimensionality in solid-state protonic conductors Lechner, R. Solid State Ionics, Vol. 77 https://doi.org/10.1016/0167-2738(94)00308-F	journal	April 1995
Multiple hops in multidimensional activated surface diffusion Hershkovitz, Eli; Talkner, Peter; Pollak, Eli Surface Science, Vol. 421, Issue 1-2 https://doi.org/10.1016/S0039-6028(98)00820-6	journal	February 1999
Study of the Papyex structure using neutron Compton scattering Finkelstein, Y.; Nemirovsky, D.; Moreh, R. Physica B: Condensed Matter, Vol. 291, Issue 1-2 https://doi.org/10.1016/S0921-4526(99)01876-1	journal	August 2000
Neutron diffraction and incoherent neutron scattering from adsorbed layers Clarke, Stuart M. Current Opinion in Colloid & Interface Science, Vol. 6, Issue 2 https://doi.org/10.1016/S1359-0294(01)00069-3	journal	May 2001
Thermal desorption of gases and solvents from graphite and carbon nanotube surfaces Ulbricht, Hendrik; Zacharia, Renju; Cindir, Nesibe Carbon, Vol. 44, Issue 14 https://doi.org/10.1016/j.carbon.2006.05.040	journal	November 2006
Benzene diffusion on graphite described by a rough hard disk model Calvo-Almazán, I.; Bahn, E.; Koza, M. M. Carbon, Vol. 79 https://doi.org/10.1016/j.carbon.2014.07.058	journal	November 2014
Diffusion of molecular hydrogen in carbon aerogel Bahn, Emanuel; Czakkel, Orsolya; Nagy, Balázs Carbon, Vol. 98 https://doi.org/10.1016/j.carbon.2015.11.034	journal	March 2016
Structure and dynamics investigations of a partially hydrogenated graphene/Ni(111) surface Bahn, Emanuel; Tamtögl, Anton; Ellis, John Carbon, Vol. 114 https://doi.org/10.1016/j.carbon.2016.12.055	journal	April 2017
Linear response theory of activated surface diffusion with interacting adsorbates Martı´nez-Casado, R.; Sanz, A. S.; Vega, J. L. Chemical Physics, Vol. 370, Issue 1-3 https://doi.org/10.1016/j.chemphys.2010.02.013	journal	May 2010
Diffraction from physisorbed layers Arnold, Thomas; Clarke, Stuart M. Current Opinion in Colloid & Interface Science, Vol. 17, Issue 1 https://doi.org/10.1016/j.cocis.2011.11.003	journal	February 2012
Studies of physisorbed ammonia overlayers adsorbed on graphite Bolina, A. S.; Brown, W. A. Surface Science, Vol. 598, Issue 1-3 https://doi.org/10.1016/j.susc.2005.08.025	journal	December 2005
Graphene Nanomesh As Highly Sensitive Chemiresistor Gas Sensor Paul, Rajat Kanti; Badhulika, Sushmee; Saucedo, Nuvia M. Analytical Chemistry, Vol. 84, Issue 19 https://doi.org/10.1021/ac3012895	journal	September 2012
Repulsion-Induced Surface-Migration by Ballistics and Bounce Guo, Si Yue; Jenkins, Stephen J.; Ji, Wei The Journal of Physical Chemistry Letters, Vol. 6, Issue 20 https://doi.org/10.1021/acs.jpclett.5b01829	journal	September 2015
Ballistic Diffusion in Polyaromatic Hydrocarbons on Graphite Calvo-Almazán, Irene; Sacchi, Marco; Tamtögl, Anton The Journal of Physical Chemistry Letters, Vol. 7, Issue 24 https://doi.org/10.1021/acs.jpclett.6b02305	journal	November 2016
Adsorption of Water and Ammonia on Graphene: Evidence for Chemisorption from X-ray Absorption Spectra Böttcher, Stefan; Vita, Hendrik; Weser, Martin The Journal of Physical Chemistry Letters, Vol. 8, Issue 15 https://doi.org/10.1021/acs.jpclett.7b01085	journal	July 2017
Surface Self-Diffusion and Mean Displacement of Hydrogen on Graphite and a PEM Fuel Cell Catalyst Support Haas, Ole-Erich; Simon, Jean Marc; Kjelstrup, Signe The Journal of Physical Chemistry C, Vol. 113, Issue 47 https://doi.org/10.1021/jp902491s	journal	October 2009
Selectivity in vibrationally mediated single-molecule chemistry Pascual, J. I.; Lorente, N.; Song, Z. Nature, Vol. 423, Issue 6939 https://doi.org/10.1038/nature01649	journal	May 2003
Detection of individual gas molecules adsorbed on graphene Schedin, F.; Geim, A. K.; Morozov, S. V. Nature Materials, Vol. 6, Issue 9, p. 652-655 https://doi.org/10.1038/nmat1967	journal	July 2007
Ballistic nanofriction Guerra, Roberto; Tartaglino, Ugo; Vanossi, Andrea Nature Materials, Vol. 9, Issue 8 https://doi.org/10.1038/nmat2798	journal	July 2010
Making molecular machines work Browne, Wesley R.; Feringa, Ben L. Nature Nanotechnology, Vol. 1, Issue 1 https://doi.org/10.1038/nnano.2006.45	journal	October 2006
Measurement of single-molecule frictional dissipation in a prototypical nanoscale system Hedgeland, H.; Fouquet, P.; Jardine, A. P. Nature Physics, Vol. 5, Issue 8 https://doi.org/10.1038/nphys1335	journal	July 2009
Chemical doping of graphene Liu, Hongtao; Liu, Yunqi; Zhu, Daoben J. Mater. Chem., Vol. 21, Issue 10 https://doi.org/10.1039/C0JM02922J	journal	January 2011
Gas diffusion on graphene surfaces Sun, Chengzhen; Bai, Bofeng Physical Chemistry Chemical Physics, Vol. 19, Issue 5 https://doi.org/10.1039/C6CP06267A	journal	January 2017
Characterisation of a basal-plane-oriented graphite Gilbert, Elliot P.; Reynolds, Philip A.; White, John W. Journal of the Chemical Society, Faraday Transactions, Vol. 94, Issue 13 https://doi.org/10.1039/a801303i	journal	January 1998
The crystalline structures of the even alkanes hexane, octane, decane, dodecane and tetradecane monolayers adsorbed on graphite at submonolayer coverages and from the liquidElectronic Supplementary Information available. See http://www.rsc.org/suppdata/cp/b1/b108190j/ Arnold, Thomas; Thomas, Robert K.; Castro, Miguel A. Physical Chemistry Chemical Physics, Vol. 4, Issue 2 https://doi.org/10.1039/b108190j	journal	January 2002
The crystalline structures of the odd alkanes pentane, heptane, nonane, undecane, tridecane and pentadecane monolayers adsorbed on graphite at submonolayer coverages and from the liquidElectronic supplementary information (ESI) available: Fractional coordinates of single repeat units of some alkanes at sub-monolayer coverage and of the monolayer coexisting with the liquid. See http://www.suppdata/cp/b2/b201988b/ Arnold, Thomas; Dong, Chu Chuan; Thomas, Robert K. Physical Chemistry Chemical Physics, Vol. 4, Issue 14 https://doi.org/10.1039/b201988b	journal	June 2002
Graphene-based gas sensors Yuan, Wenjing; Shi, Gaoquan Journal of Materials Chemistry A, Vol. 1, Issue 35 https://doi.org/10.1039/c3ta11774j	journal	January 2013
Structure and dynamics of ammonia absorbed on graphitized carbon black. Part 3.—Neutron quasielastic and inelastic spectra Gamlen, Philip H.; Thomas, Robert K.; Trewern, Timothy D. Journal of the Chemical Society, Faraday Transactions 1: Physical Chemistry in Condensed Phases, Vol. 75, Issue 0 https://doi.org/10.1039/f19797501553	journal	January 1979
Effects of resolution and friction in the interpretation of QHAS measurements Jardine, A. P.; Ellis, J.; Allison, W. The Journal of Chemical Physics, Vol. 120, Issue 18 https://doi.org/10.1063/1.1695320	journal	May 2004
Generalized Chudley-Elliott vibration-jump model in activated atom surface diffusion Martínez-Casado, R.; Vega, J. L.; Sanz, A. S. The Journal of Chemical Physics, Vol. 126, Issue 19 https://doi.org/10.1063/1.2735586	journal	May 2007
Adsorption of nitrogen oxides on graphene and graphene oxides: Insights from density functional calculations Tang, Shaobin; Cao, Zexing The Journal of Chemical Physics, Vol. 134, Issue 4 https://doi.org/10.1063/1.3541249	journal	January 2011
Electron energy loss spectroscopy of ammonia on Ru(001) Parmeter, J. E.; Wang, Y.; Mullins, C. B. The Journal of Chemical Physics, Vol. 88, Issue 8 https://doi.org/10.1063/1.454597	journal	April 1988
The structure of ammonia overlayers physisorbed onto the surface of single crystal graphite, determined by means of atomic beam diffraction Rowntree, P.; Scoles, G.; Xu, J. The Journal of Chemical Physics, Vol. 92, Issue 6 https://doi.org/10.1063/1.457842	journal	March 1990
Adsorption capacity of H ₂ O, NH ₃ , CO, and NO ₂ on the pristine graphene Lin, Xianqing; Ni, Jun; Fang, Chao Journal of Applied Physics, Vol. 113, Issue 3 https://doi.org/10.1063/1.4776239	journal	January 2013
Atomic scale friction of molecular adsorbates during diffusion Lechner, B. A. J.; de Wijn, A. S.; Hedgeland, H. The Journal of Chemical Physics, Vol. 138, Issue 19 https://doi.org/10.1063/1.4804269	journal	May 2013
Diffusion, adsorption, and desorption of molecular hydrogen on graphene and in graphite Petucci, Justin; LeBlond, Carl; Karimi, Majid The Journal of Chemical Physics, Vol. 139, Issue 4 https://doi.org/10.1063/1.4813919	journal	July 2013
Graphene/mica based ammonia gas sensors Ben Aziza, Zeineb; Zhang, Qing; Baillargeat, Dominique Applied Physics Letters, Vol. 105, Issue 25 https://doi.org/10.1063/1.4905039	journal	December 2014
Neutron Scattering from a Liquid on a Jump Diffusion Model Chudley, C. T.; Elliott, R. J. Proceedings of the Physical Society, Vol. 77, Issue 2 https://doi.org/10.1088/0370-1328/77/2/319	journal	February 1961
The dynamics of activated surface diffusion Miret-Artés, Salvador; Pollak, Eli Journal of Physics: Condensed Matter, Vol. 17, Issue 49 https://doi.org/10.1088/0953-8984/17/49/009	journal	November 2005
Vibration and diffusion of Cs atoms on Cu(001) Jardine, A. P.; Alexandrowicz, G.; Hedgeland, H. Journal of Physics: Condensed Matter, Vol. 19, Issue 30 https://doi.org/10.1088/0953-8984/19/30/305010	journal	July 2007
Adsorption of ammonia on graphene Romero, Hugo E.; Joshi, Prasoon; Gupta, Awnish K. Nanotechnology, Vol. 20, Issue 24 https://doi.org/10.1088/0957-4484/20/24/245501	journal	May 2009
Single-molecule manipulation experiments to explore friction and adhesion Pawlak, R.; Kawai, S.; Meier, T. Journal of Physics D: Applied Physics, Vol. 50, Issue 11 https://doi.org/10.1088/1361-6463/aa599d	journal	February 2017
Dynamics of adatoms on solid surfaces Chen, L. Y.; Ying, S. C. Physical Review B, Vol. 49, Issue 19 https://doi.org/10.1103/PhysRevB.49.13838	journal	May 1994
Self-diffusion on low-index metallic surfaces: Ag and Au (100) and (111) Boisvert, Ghyslain; Lewis, Laurent J. Physical Review B, Vol. 54, Issue 4 https://doi.org/10.1103/PhysRevB.54.2880	journal	July 1996
Isotopic ordering in adsorbed hydrogen monolayers Bienfait, M.; Zeppenfeld, P.; Ramos, R. C. Physical Review B, Vol. 60, Issue 16 https://doi.org/10.1103/PhysRevB.60.11773	journal	October 1999
Adsorption of H 2 O , N H 3 , CO, N O 2 , and NO on graphene: A first-principles study Leenaerts, O.; Partoens, B.; Peeters, F. M. Physical Review B, Vol. 77, Issue 12 https://doi.org/10.1103/PhysRevB.77.125416	journal	March 2008
Atomic jumps during surface diffusion Ferrón, J.; Miranda, R.; de Miguel, J. J. Physical Review B, Vol. 79, Issue 24 https://doi.org/10.1103/PhysRevB.79.245407	journal	June 2009
Adsorption and diffusion of water on graphene from first principles Ma, Jie; Michaelides, Angelos; Alfè, Dario Physical Review B, Vol. 84, Issue 3 https://doi.org/10.1103/PhysRevB.84.033402	journal	July 2011
Internal degrees of freedom and transport of benzene on graphite de Wijn, Astrid S. Physical Review E, Vol. 84, Issue 1 https://doi.org/10.1103/PhysRevE.84.011610	journal	July 2011
Accurate Molecular Van Der Waals Interactions from Ground-State Electron Density and Free-Atom Reference Data Tkatchenko, Alexandre; Scheffler, Matthias Physical Review Letters, Vol. 102, Issue 7 https://doi.org/10.1103/PhysRevLett.102.073005	journal	February 2009
Experimental Observation of Fast Diffusion of Large Antimony Clusters on Graphite Surfaces Bardotti, Laurent; Jensen, Pablo; Hoareau, Alain Physical Review Letters, Vol. 74, Issue 23 https://doi.org/10.1103/PhysRevLett.74.4694	journal	June 1995
Generalized Gradient Approximation Made Simple Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868 https://doi.org/10.1103/PhysRevLett.77.3865	journal	October 1996
Surface Diffusion of Pt on Pt(110): Arrhenius Behavior of Long Jumps Linderoth, T. R.; Horch, S.; Lægsgaard, E. Physical Review Letters, Vol. 78, Issue 26 https://doi.org/10.1103/PhysRevLett.78.4978	journal	June 1997
C 60 Molecular Bearings Miura, K.; Kamiya, S.; Sasaki, N. Physical Review Letters, Vol. 90, Issue 5 https://doi.org/10.1103/PhysRevLett.90.055509	journal	February 2003
Nonstochastic Behavior of Atomic Surface Diffusion on Cu(111) down to Low Temperatures Ferrón, J.; Gómez, L.; de Miguel, J. J. Physical Review Letters, Vol. 93, Issue 16 https://doi.org/10.1103/PhysRevLett.93.166107	journal	October 2004
Progress in the measurement and modeling of physisorbed layers Bruch, L. W.; Diehl, R. D.; Venables, J. A. Reviews of Modern Physics, Vol. 79, Issue 4 https://doi.org/10.1103/RevModPhys.79.1381	journal	November 2007
N-Doping of Graphene Through Electrothermal Reactions with Ammonia Wang, Xinran; Li, Xiaolin; Zhang, Li Science, Vol. 324, Issue 5928, p. 768-771 https://doi.org/10.1126/science.1170335	journal	May 2009
Superlubricity of graphene nanoribbons on gold surfaces Kawai, S.; Benassi, A.; Gnecco, E. Science, Vol. 351, Issue 6276 https://doi.org/10.1126/science.aad3569	journal	February 2016
Graphene on ferromagnetic surfaces and its functionalization with water and ammonia Böttcher, Stefan; Weser, Martin; Dedkov, Yuriy S. Nanoscale Research Letters, Vol. 6, Issue 1 https://doi.org/10.1186/1556-276X-6-214	journal	January 2011
Study on adsorption and desorption of ammonia on graphene Zhang, Zhengwei; Zhang, Xinfang; Luo, Wei Nanoscale Research Letters, Vol. 10, Issue 1 https://doi.org/10.1186/s11671-015-1060-7	journal	September 2015
First principles methods using CASTEP Clark, Stewart J.; Segall, Matthew D.; Pickard, Chris J. Zeitschrift für Kristallographie - Crystalline Materials, Vol. 220, Issue 5/6 https://doi.org/10.1524/zkri.220.5.567.65075	journal	January 2005

Cited By (6)

Nanoscopic diffusion of water on a topological insulator. Tamtögl, Anton; Sacchi, Marco; Avidor, Nadav Apollo - University of Cambridge Repository https://doi.org/10.17863/cam.48374	text	January 2020
Nanoscopic diffusion of water on a topological insulator Tamtögl, Anton; Sacchi, Marco; Avidor, Nadav Nature Communications, Vol. 11, Issue 1 https://doi.org/10.1038/s41467-019-14064-7	journal	January 2020
Polarisation in spin-echo experiments: Multi-point and lock-in measurements Tamtögl, Anton; Davey, Benjamin; Ward, David J. Review of Scientific Instruments, Vol. 89, Issue 2 https://doi.org/10.1063/1.5017276	journal	February 2018
Activated quantum diffusion in a periodic potential above the crossover temperature Ianconescu, Reuven; Pollak, Eli The Journal of Chemical Physics, Vol. 151, Issue 2 https://doi.org/10.1063/1.5100010	journal	July 2019
Polarisation in spin-echo experiments: Multi-point and lock-in measurements. Tamtögl, Anton; Davey, Benjamin; Ward, David Apollo - University of Cambridge Repository https://doi.org/10.17863/cam.23001	text	January 2018
Nanoscopic diffusion of water on a topological insulator. Tamtögl, Anton; Sacchi, Marco; Avidor, Nadav Apollo - University of Cambridge Repository https://doi.org/10.17863/cam.48374	text	January 2020

Similar Records

Controlling the number of graphene sheets exfoliated from graphite by designed normal loading and frictional motion

Journal Article · 2014 · Journal of Applied Physics · OSTI ID:22308981

Lee, Seungjun; Lu, Wei

Binding and Diffusion of Lithium in Graphite: Quantum Monte Carlo Benchmarks and Validation of van der Waals Density Functional Methods

Journal Article · 2014 · Journal of Chemical Theory and Computation · OSTI ID:1185355

Ganesh, P.; Kim, Jeongnim; Park, Changwon; +3 more

Interaction of Ti with the (0001) surface of highly oriented pyrolitic graphite

Journal Article · 1999 · Physical Review, B: Condensed Matter · OSTI ID:355452

Ma, Q; Rosenberg, R A

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Adsorption
Ammonia
DFT
Diffusion
Graphite
Neutron scattering

Title: Ultrafast molecular transport on carbon surfaces: The diffusion of ammonia on graphite

Citation Formats

References (64)

Cited By (6)

Similar Records

Related Subjects