Atomistic simulations of plasma catalytic processes

doi:10.1007/s11705-017-1674-7

Front. Chem. Sci. Eng.

2018, Vol. 12

Issue (1) : 145-154 https://doi.org/10.1007/s11705-017-1674-7

RESEARCH ARTICLE

Atomistic simulations of plasma catalytic processes

Erik C. Neyts(

)

Research Group PLASMANT, Department of Chemistry, University of Antwerp, Universiteitsplein 1, 2610 Wilrijk-Antwerp, Belgium

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Abstract

There is currently a growing interest in the realisation and optimization of hybrid plasma/catalyst systems for a multitude of applications, ranging from nanotechnology to environmental chemistry. In spite of this interest, there is, however, a lack in fundamental understanding of the underlying processes in such systems. While a lot of experimental research is already being carried out to gain this understanding, only recently the first simulations have appeared in the literature. In this contribution, an overview is presented on atomic scale simulations of plasma catalytic processes as carried out in our group. In particular, this contribution focusses on plasma-assisted catalyzed carbon nanostructure growth, and plasma catalysis for greenhouse gas conversion. Attention is paid to what can routinely be done, and where challenges persist.

Keywords atomic scale simulation plasma-catalyst

Corresponding Author(s): Erik C. Neyts

Just Accepted Date: 04 July 2017 Online First Date: 08 November 2017 Issue Date: 26 February 2018

Cite this article:

Erik C. Neyts. Atomistic simulations of plasma catalytic processes[J]. Front. Chem. Sci. Eng., 2018, 12(1): 145-154.

URL:

https://academic.hep.com.cn/fcse/EN/10.1007/s11705-017-1674-7
https://academic.hep.com.cn/fcse/EN/Y2018/V12/I1/145

Fig.1 Effect of adding an electric field to the Ni-catalyzed CNT growth. (a) Vertical nucleation is observed in the E-field range 300?800 kV/cm; (b) charge separation in the Ni/C nanocluster. Reproduced with permission from ACS [31]

Fig.2 (a) Observed defect healing and enhanced cap formation by ion bombardment in the energy range 15?25 eV and destruction of the network at higher energies (>30 eV); (b) growth of the carbon network due to the ion bombardment at 15 eV, as seen in the MD simulations. The numbers in parentheses indicate the sum of the pentagons, hexagons and heptagons; the other numbers indicate the total number of rings in the patch. Reproduced with permission from [41]

Fig.3 Contribution of carbon atoms in the CNT network due to surface diffusion (SD) and bulk diffusion (BD), in ion-assisted growth. Reproduced with permission from [44]

Fig.4 Scatter plot of the time to first methanol to formaldehyde conversion in ms. Reproduced with permission from [53]

Fig.5 Effect of vibrational excitation of CH₄ molecules on a Ni(111) surface. (a) Comparison between simulated and experimental adsorption probability for CH₄ in the ground state as a function of the kinetic energy; (b) comparison between simulated and experimental adsorption probability for CH₄ excited in the ν₃ state as a function of the kinetic energy; (c) comparison of the simulated adsorption probability between CH₄ in the ground state and in the ν₃ state, as function of the translational energy

Fig.6 Reduction in activation energy for associative desorption of methanol due to an increase of the H-coverage. Side view and top view of H-transfer (pink atom) to previously formed CH₂OH fragments are shown in the insets for a coverage of 0.75 ML of H. The associative desorption of methanol (side view) will cause the associated H diffusion at the surface (green atoms). Reproduced with permission from [60]

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