Publication
Title
A comparative DFT study on CO oxidation reaction over Si-doped BC2N nanosheet and nanotube
Author
Abstract
In this study, we performed density functional theory (DFT) calculations to investigate different reaction mechanisms of CO oxidation catalyzed by the Si atom embedded defective BC2N nanostructures as well as the analysis of the structural and electronic properties. The structures of all the complexes are optimized and characterized by frequency calculations at the M062X/6-31G* computational level. Also, The electronic structures and thermodynamic parameters of adsorbed CO and O-2 molecules over Si-doped BC2N nanostructures are examined in detail. Moreover, to investigate the curvature effect on the CO oxidation reaction, all the adsorption and CO oxidation reactions on a finite-sized armchair (6,6) Si-BC2NNT are also studied. Our results indicate that there can be two possible pathways for the CO oxidation with O-2 molecule: O-2(g) + CO(g) -> O-2(ads) + CO(ads) -> CO2(g) + O-(ads) and O-(ads) + CO(g) -> CO2(g). The first reaction proceeds via the Langmuir-Hinshelwood (LH) mechanism while the second goes through the Eley-Rideal (ER) mechanism. On the other hand, by increasing the tube diameter, the energy barrier increases due to the strong adsorption energy of the O-2 molecule which is related to its dissociation over the tube surface. Our calculations indicate that the two step energy barrier of the oxidation reaction over Si-BC2NNS is less than that over the Si-BC2NNT. Hence, Si-BC2NNS may serve as an efficient and highly activated substrate to CO oxidation rather than (4,4) Si-BC2NNT. (C) 2018 Elsevier B.V. All rights reserved.
Language
English
Source (journal)
Applied surface science. - Amsterdam
Publication
Amsterdam : 2018
ISSN
0169-4332
Volume/pages
439 (2018) , p. 934-945
ISI
000427457100112
Full text (Publisher's DOI)
UAntwerpen
Faculty/Department
Research group
Project info
Computational design of improved catalysts for plasma catalytic dry reforming of methane.
Publication type
Subject
Affiliation
Publications with a UAntwerp address
External links
Web of Science
Record
Identification
Creation 04.05.2018
Last edited 19.10.2021
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