A combined computational and experimental study of the adsorption of sulfur containing molecules on molybdenum disulfide nanoparticles

Combining density functional theory calculations and temperature programmed desorption (TPD) experiments, the adsorption behavior of various sulfur containing compounds, including C2H5SH, CH3SCH3, tetrahydrothiophene, thiophene, benzothiophene, dibenzothiophene, and their derivatives on the coordina...

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Published inJournal of materials research Vol. 33; no. 21; pp. 3589 - 3603
Main Authors Yang, Tao, Feng, Junpeng, Liu, Xingchen, Wang, Yandan, Ge, Hui, Cao, Dongbo, Li, Hao, Peng, Qing, Ramos, Manuel, Wen, Xiao-Dong, Shen, Baojian
Format Journal Article
LanguageEnglish
Published New York, USA Cambridge University Press 14.11.2018
Springer International Publishing
Springer Nature B.V
Subjects
Adsorption
Applied and Technical Physics
Aromaticity
Benzothiophene
Biomaterials
Bonding strength
Catalysis
Density functional theory
Dibenzothiophene
Hydrogen
Hydrogenation
Inorganic Chemistry
Materials Engineering
Materials research
Materials Science
Mathematical analysis
Molybdenum
Molybdenum disulfide
Nanoparticles
Nanotechnology
Steric effects
Sulfur
Theory
hydrogenation
adsorption
catalytic
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Summary:Combining density functional theory calculations and temperature programmed desorption (TPD) experiments, the adsorption behavior of various sulfur containing compounds, including C2H5SH, CH3SCH3, tetrahydrothiophene, thiophene, benzothiophene, dibenzothiophene, and their derivatives on the coordinately unsaturated sites of Mo27Sx model nanoparticles, are studied systematically. Sulfur molecules with aromaticity prefer flat adsorption than perpendicular adsorption. The adsorption of nonaromatic molecules is stronger than the perpendicular adsorption of aromatic molecules, but weaker than the flat adsorption of them. With gradual hydrogenation (HYD), the binding affinity in the perpendicular adsorption modes increases, while in flat adsorption modes it increases first, then decreases. Significant steric effects on the adsorption of dimethyldibenzothiophene were revealed in perpendicular adsorption modes. The steric effect, besides weakening adsorption, could also activate the S–C bonds through a compensation effect. Finally, by comparing the theoretical adsorption energies with the TPD results, we suggest that HYD and direct-desulfurization path may happen simultaneously, but on different active sites.
ISSN:0884-2914
2044-5326
DOI:10.1557/jmr.2018.309