DFT insights into the adsorption behavior of 4,6-dimethyldibenzothiophene on the Ni-Mo-S corner sites: Effect of the promoter magnetism
Source abstract
Abstract
Abstract The computational method based on the first principle of numerical atomic functions of density functional theory (DFT) was established to investigate the effects of ferromagnetism for Ni species on the Ni-Mo-S monolayer nanocluster as well as the adsorption behavior of 4,6-DMDBT for the first time. The spin charge density analysis, the Hirshfield analysis, the frontier orbital analysis and the deformation charge analysis were performed. The results show that the ferromagnetism of Ni species significantly affected the spin charge density of the Ni-Mo-S corner active site, while it has little effect on the spin charge density of Ni-Mo-S edge sites due to the loss of magnetism caused by the frustrating interactions of the ferromagnetic Ni atom in the hexagonal honeycomb MoS2 structure. The 4,6-DMDBT adsorption behavior investigation results show that the ferromagnetism of the Ni species has greatly influenced the adsorption of 4,6-DMDBT over the magnetic corner active sites: type-2 adsorption configuration with adsorption energy of about 108.2 kJ·mol−1 is the predominant adsorption configuration without considering the magnetic features of Ni-Mo-S corner active site; while type-10 adsorption configuration with that of about 110.1 kJ·mol−1 becomes the predominant one after considering the magnetic features of Ni-Mo-S corner active site. The adsorption behavior of 4,6-DMDBT on the Ni-Mo-S edge active site has barely affected by the ferromagnetism of Ni Species. Besides, 4,6-DMDBT molecule is more inclined to adsorb on the corner active site via σ adsorption by formation of σ bond between the corner Ni atom and the S atom from 4,6-DMDBT.
Source: openaire · Quality: candidate unverified · Source record ↗
Research context
OpenAlex topics: Catalysis and Hydrodesulfurization Studies · Electrocatalysts for Energy Conversion · 2D Materials and Applications
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
References (73)
Show source-provided references
1. An overview of new approaches to deep desulfurization for ultra-clean gasoline, diesel fuel and jet fuel10.1016/S0920-5861(03)00412-7 ↗
2. Science and technology of novel processes for deep desulfurization of oil refinery streams: a review10.1016/S0016-2361(02)00324-1 ↗
3. Synthesis, characterization, and catalytic performance of NiMo catalysts supported on different crystal alumina materials in the hydrodesulfurization of diesel10.1016/j.fuproc.2016.10.007 ↗
4. Site-dependent reactivity of MoS2 nanoparticles in hydrodesulfurization of thiophene10.1038/s41467-020-18183-4 ↗
5. Mechanistic investigations on the adsorption of thiophene over Zn3NiO4 bimetallic oxide cluster10.1016/j.apsusc.2012.06.096 ↗
6. Crucial technologies supporting future development of petroleum refining industry10.1016/S1872-2067(11)60508-1 ↗
7. Adsorptive removal of aromatic organosulfur compounds over the modified Na-Y zeolites10.1016/j.apcatb.2008.01.006 ↗
8. Hydrodesulfurization of 4, 6-dimethyldibenzothiophene over CoMo catalysts supported on γ-alumina with different morphology10.1021/ie5007504 ↗
9. Extraordinarily High Activity in the Hydrodesulfurization of 4,6-Dimethyldibenzothiophene over Pd Supported on Mesoporous Zeolite Y10.1021/ja2072719 ↗
10. Sustainable synthesis of ammonium nickel molybdate for hydrodesulfurization of dibenzothiophene10.1016/S1872-2067(16)62453-1 ↗
11. Hydrodesulfurization of diesel in a slurry reactor10.1016/j.ces.2009.05.046 ↗
12. Effects of gallium addition to mesoporous alumina by impregnation on dibenzothiophene hydrodesulfurization performances of the corresponding NiMo supported catalysts10.1016/j.fuel.2018.04.084 ↗
13. The development and application of catalysts for ultra-deep hydrodesulfurization of diesel10.1016/S1872-2067(11)60506-8 ↗
14. The effect of Co-promotion on MoS2 catalysts for hydrodesulfurization of thiophene: A density functional study10.1016/j.jcat.2009.09.016 ↗
15. H. Topsøe, B.S. Clausen, F.E. Massoth, Hydrotreating catalysis, Springer, Berlin, Heidelberg, In: Anderson J.R, 1996.10.1007/978-3-642-61040-0_1 ↗
16. Hydrodeoxygenation pathways catalyzed by MoS2 and NiMoS active phases: A DFT study10.1016/j.jcat.2011.01.025 ↗
17. Surface Engineering of CoMoS Nanosulfide for Hydrodeoxygenation of Lignin-Derived Phenols to Arenes10.1021/acscatal.8b03402 ↗
18. A molecular MoS2 edge site mimic for catalytic hydrogen generation10.1126/science.1215868 ↗
19. Solvent-assisted oxygen incorporation of vertically aligned MoS2 ultrathin nanosheets decorated on reduced graphene oxide for improved electrocatalytic hydrogen evolution10.1021/acsami.6b06031 ↗
20. Activation of MoS2 monolayers by substitutional copper and silver atoms embedded in sulfur vacancies: A theoretical study10.1016/j.apsusc.2019.03.107 ↗
21. The hydrogenation and direct desulfurization reaction pathway in thiophene hydrodesulfurization over MoS2 catalysts at realistic conditions: A density functional study10.1016/j.jcat.2007.02.028 ↗
22. Hydrodesulfurization reaction pathways on MoS2 nanoclusters revealed by scanning tunneling microscopy10.1016/j.jcat.2004.02.009 ↗
23. Atomic-scale structure of Co–Mo–S nanoclusters in hydrotreating catalysts10.1006/jcat.2000.3088 ↗
24. Atomic-scale structure of single-layer MoS 2 nanoclusters10.1103/PhysRevLett.84.951 ↗
25. Catalytic characteristics of active corner sites in CoMoS nanostructure hydrodesulfurization–A mechanism study based on DFT calculations10.1016/j.jcat.2016.11.011 ↗
26. Location and coordination of promoter atoms in Co-and Ni-promoted MoS2-based hydrotreating catalysts10.1016/j.jcat.2007.04.013 ↗
27. DFT Insights into the Competitive Adsorption of Sulfur- and Nitrogen-Containing Compounds and Hydrocarbons on Co-Promoted Molybdenum Sulfide Catalysts10.1021/acscatal.6b00058 ↗
28. DFT insights into the direct desulfurization pathways of DBT and 4,6-DMDBT catalyzed by Co-promoted and Ni-promoted MoS2 corner sites10.1016/j.ces.2019.05.032 ↗
29. The combined DFT and microkinetics methods to investigate the favorite sulfur vacancies of Co(Ni)MoS2 catalysts for maximizing HDS/HYDO selectivity10.1016/j.apcatb.2020.119242 ↗
30. Modeling the adsorption of sulfur containing molecules and their hydrodesulfurization intermediates on the Co-promoted MoS2 catalyst by DFT10.1016/j.jcat.2017.12.001 ↗
31. Understanding the trends in the hydrodesulfurization activity of the transition metal sulfides10.1007/BF00770941 ↗
32. Promotion of the Inactive Iron Sulfide to an Efficient Hydrodesulfurization Catalyst10.1021/acscatal.6b03495 ↗
33. The role of Co–Mo–S type structures in hydrotreating catalysts10.1016/j.apcata.2007.01.002 ↗
34. Effect of promoters on the HDS activity of alumina-supported Co–Mo sulfide catalysts10.1039/C5RA17414G ↗
35. Synthesis of mesoporous materials SBA-16 with different morphologies and their application in dibenzothiophene hydrodesulfurization10.1016/j.ces.2016.08.001 ↗
36. Synthesis of NiMo catalysts supported on mesoporous Al2O3 with different crystal forms and superior catalytic performance for the hydrodesulfurization of dibenzothiophene and 4,6-dimethyldibenzothiophene10.1016/j.jcat.2016.10.016 ↗
37. Overview of support effects in hydrotreating catalysts10.1016/S0920-5861(03)00400-0 ↗
38. Reactivities in deep catalytic hydrodesulfurization: challenges, opportunities, and the importance of 4-methyldibenzothiophene and 4, 6-dimethyldibenzothiophene10.1016/S0277-5387(97)00074-0 ↗
39. Hydrodesulfurization of dibenzothiophene catalyzed by sulfided CoO-MoO3γ-Al2O3: The reaction network10.1002/aic.690240611 ↗
40. Hydrodesulyfurization of dibenzaothiophene and related compounds catalyzed by sulfided CoO-MoO3/Gamma-Al2O3.Effects of reactant structure of reactivity
41. A density functional theory study of the hydrodesulfurization reaction of dibenzothiophene to biphenyl on a single-layer NiMoS cluster10.1016/j.cattod.2007.06.078 ↗
42. Influence of sulfur vacancy on thiophene hydrodesulfurization mechanism at different MoS2 edges: A DFT study10.1016/j.ces.2017.02.037 ↗
43. Competitive hydrodesulfurization of 4, 6-dimethyldibenzothiophene, hydrodenitrogenation of 2-methylpyridine, and hydrogenation of naphthalene over sulfided NiMo/γ-Al2O310.1016/j.jcat.2004.03.005 ↗
44. A new multi–metallic bulk catalyst with high hydrodesulfurization activity of 4,6–DMDBT prepared using layered hydroxide salts as structural templates10.1016/j.apcata.2013.09.002 ↗
45. Active Sites on Nickel-Promoted Transition-Metal Sulfides That Catalyze Hydrogenation of Aromatic Compounds10.1002/anie.201808428 ↗
46. Hydrodesulfurization of 4,6-dimethyldibenzothiophene over NiMo sulfide catalysts supported on meso-microporous Y zeolite with different mesopore sizes10.1016/j.apcatb.2018.07.042 ↗
47. Single-atom Pt promotion of industrial Co-Mo-S catalysts for ultra-deep hydrodesulfurization10.1016/j.jcat.2021.03.008 ↗
48. Modeling the active sites of Co-promoted MoS 2 particles by DFT10.1039/C6CP06881B ↗
49. DFT insights into the hydrodenitrogenation mechanism of quinoline catalyzed by different Ni-promoted MoS2 edge sites: Effect of the active phase morphology10.1016/j.jhazmat.2021.125127 ↗
50. Substituent effects of 4, 6-DMDBT on direct hydrodesulfurization routes catalyzed by Ni-Mo-S active nanocluster—A theoretical study10.1016/j.cattod.2017.10.040 ↗
51. Insight into the effect of non-stoechiometric sulfur over NiMoS hydrodesulfurization catalyst
52. First-principles study of the origin of magnetism induced by intrinsic defects in monolayer MoS210.1016/j.apsusc.2015.11.134 ↗
53. Location of Co and Ni promoter atoms in multi-layer MoS2 nanocrystals for hydrotreating catalysis10.1016/j.cattod.2015.08.053 ↗
54. Recent STM, DFT and HAADF-STEM studies of sulfide-based hydrotreating catalysts: Insight into mechanistic, structural and particle size effects10.1016/j.cattod.2007.08.009 ↗
55. Substitution of sulfur atoms on Ni-Mo-S by ammonia-A DFT study10.1016/j.cattod.2019.12.030 ↗
56. Direct magnetic reinforcement of electrocatalytic ORR/OER with electromagnetic induction of magnetic catalysts10.1002/adma.202007525 ↗
57. Recent Advances in Magnetic Field-Enhanced Electrocatalysis10.1021/acsaem.0c02104 ↗
58. Ab initio energy-adjusted pseudopotentials for elements of groups 13–1710.1080/00268979300103121 ↗
59. Mechanistic study of methanol synthesis from CO2 hydrogenation on Rh-doped Cu(111) surfaces
60. Mechanistic Study of Pd–Cu Bimetallic Catalysts for Methanol Synthesis from CO2 Hydrogenation10.1021/acs.jpcc.7b06166 ↗
61. A DFT Study on the Adsorption Behavior of Sulfur and Nitrogen Compounds on the NiMoS Phase
62. Catalysis performance of nonpromoted and co-promoted MoS2 catalysts on a hydrodesulfurization reaction: A DFT study
63. Unveiling the decomposition mechanism of formic acid on Pd/WC (0001) surface by using density function theory10.1016/S1872-2067(19)63463-7 ↗
64. Zirconia-modified copper catalyst for CO2 conversion to methanol from DFT study10.1016/j.apsusc.2020.146900 ↗
65. Theoretical study of methanol synthesis from CO2 hydrogenation on PdCu3 (111) surface10.1016/j.apsusc.2018.04.128 ↗
66. An efficient and stable Cu/SiO2 catalyst for the syntheses of ethylene glycol and methanol via chemoselective hydrogenation of ethylene carbonate10.1016/S1872-2067(18)63032-3 ↗
67. Semiempirical GGA-type density functional constructed with a long-range dispersion correction10.1002/jcc.20495 ↗
68. Niobium modification effects on hydrodesulfurization of 4, 6-DMDBT catalyzed on Ni-Mo-S active sites: A combination of experiments and theoretical study10.1016/j.fuel.2018.10.002 ↗
69. Ni structural doping induced spin polarization effects on the optical and electric properties of nano-SiC film10.1016/j.apsusc.2019.03.351 ↗
70. Order induced by dipolar interactions in a geometrically frustrated antiferromagnet10.1103/PhysRevB.62.488 ↗
71. Spin liquids in frustrated magnets10.1038/nature08917 ↗
72. Calculation of magnetic exchange couplings in the S= 3/2 honeycomb system (Bi3Mn4O12) NO3 from first principles10.1103/PhysRevB.83.140412 ↗
73. Atomic scale analysis of sterical effects in the adsorption of 4, 6-dimethyldibenzothiophene on a CoMoS hydrotreating catalyst10.1016/j.jcat.2016.09.004 ↗