Effect of Adding Chelating Ligands on the Catalytic Performance of Rh-Promoted MoS2 in the Hydrodesulfurization of Dibenzothiophene
Abstract
:1. Introduction
2. Results and Discussion
2.1. UV-Vis Spectroscopy
2.2. Band Gaps of RhMo Catalysts
2.3. Fourier Transform Infrared Spectroscopy (FT-IR)
2.4. Energy Dispersion Spectroscopy (EDX)
2.5. X-ray Diffraction (XRD)
2.6. XPS Analysis
2.7. Transmission Electron Microscopy (TEM)
2.8. Scanning Electron Microscopy (SEM)
2.9. Stability of Catalysts—TGA and DSC Thermal Analyses
2.10. Catalytic Activity
2.11. Proposed Mechanism
3. Experimental Section
3.1. Materials
3.2. Synthesis of RhMo Catalysts Prepared with Ethylenediaminetetraacetic Acid (EDTA), Citric Acid (CA) and Acetic Acid (AA)
3.3. Catalyst Characterization
3.4. Catalyst Sulfidation and Hydrodesulfurization Measurements
4. Conclusions
Supplementary Materials
Author Contributions
Funding
Data Availability Statement
Conflicts of Interest
References
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Catalyst | Eg Values | NMo-O-Mo |
---|---|---|
RhMo/γ-Al2O3 | 3.779 | 1.975 |
RhMo-AA/γ-Al2O3 | 4.341 | 0.5134 |
RhMo-EDTA/γ-Al2O3 | 4.394 | 0.3756 |
RhMo-CA/γ-Al2O3 | 4.478 | 0.1572 |
Catalysts | Atomic Percentage (wt. %) | S/Mo | C/Mo | |||||
---|---|---|---|---|---|---|---|---|
C K | O K | Al K | S K | Rh L | Mo L | |||
RhMo/ɣ-Al2O3 | 7.97 | 63.24 | 26.47 | 0.68 | 0.17 | 1.46 | 0.47 | 5.46 |
RhMo-EDTA/ɣ-Al2O3 | 10.20 | 57.52 | 30.03 | 1.48 | 0.44 | 0.32 | 4.63 | 31.88 |
RhMo-AA/ɣ-Al2O3 | 9.38 | 62.61 | 25.63 | 1.35 | 0.19 | 0.73 | 1.85 | 12.85 |
RhMo-CA/ɣ-Al2O3 | 12.07 | 57.56 | 26.88 | 1.60 | 0.94 | 0.90 | 1.78 | 13.41 |
Elements (eV) | RhMo/ɣ-Al2O3 | RhMo-EDTA/ɣ-Al2O3 |
---|---|---|
C 1s | 289.5 | 285.5 |
O 1s | 530.0 | 529.0 |
Mo 3d | 226.2; 230.0; 233.2 | 226.0; 230.0 |
Rh 3d | 306.5; 310.6 | 305.0; 310.1 |
S 2p | 160.1; 167.0 | 160.5; 166.1 |
Al 2p | 72.4 | 72.0 |
Al 2s | 117.0 | 117.0 |
Catalysts | Average Diameter ± SD (nm) |
---|---|
RhMo/ɣ-Al2O3 | 4.4 (±1.38) |
RhMo-EDTA/ɣ-Al2O3 | 4.1 (±1.220) |
RhMo-AA/ɣ-Al2O3 | 3.3 (±0.757) |
RhMo-CA/ɣ-Al2O3 | 1.6 (±0.860) |
Catalysts | Crystallite Sizes (nm) | Eg Values | HDS (%) | BP(%) | PhCh(%) | HYD/DDS Ratio | TOF (h−1) a |
---|---|---|---|---|---|---|---|
RhMo/ɣ-Al2O3 | 5.903 | 3.779 | 88 | 65 | 13 | 0.20 | 51 |
RhMo-EDTA/ɣ-Al2O3 | 5.770 | 4.394 | 68 | 16 | 1 | 0.06 | 60 |
RhMo-AA/ɣ-Al2O3 | 5.750 | 4.341 | 73 | 65 | 3 | 0.05 | 79 |
RhMo-CA/ɣ-Al2O3 | 5.809 | 4.478 | 72 | 36 | 2 | 0.06 | 223 |
Catalysts | Model Compound | Reaction Temperature (°C) | HDS (%) | Reaction Pressure (Bar) | Reference |
---|---|---|---|---|---|
RhMo/ɣ-Al2O3 | DBT | 300 | 88 | 40 | This work |
RhMo-EDTA/ɣ-Al2O3 | DBT | 300 | 68 | 40 | This work |
RhMo-AA/ɣ-Al2O3 | DBT | 300 | 73 | 40 | This work |
RhMo-CA/ɣ-Al2O3 | DBT | 300 | 72 | 40 | This work |
Ni2P | DBT | 340 | 35 | 40 | [79] |
Ni2P | TH-DBT | 340 | 50 | 40 | [79] |
NiMoP/γ-Al2O3 | DBT | <320 | 22–90 | <25 | [80] |
RuxMoNi | DBT | 320 | 24–92 | 54.5 | [81] |
NiMo | DBT | 320 | 62 | 54.5 | [81] |
NiMo/TiO2-6 | DBT | 300 | 90 | 20 | [82] |
NiMo/MCM-41-Na | DBT | 300 | >95 | 50 | [83] |
Fe-Zn/TiO2-Al2O3 | DBT | 380 | >98 | 40 | [84] |
RhMo/ɣ-Al2O3 | DBT | 310 | 84 | 50 | [28] |
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Majodina, S.; Tshentu, Z.R.; Ogunlaja, A.S. Effect of Adding Chelating Ligands on the Catalytic Performance of Rh-Promoted MoS2 in the Hydrodesulfurization of Dibenzothiophene. Catalysts 2021, 11, 1398. https://doi.org/10.3390/catal11111398
Majodina S, Tshentu ZR, Ogunlaja AS. Effect of Adding Chelating Ligands on the Catalytic Performance of Rh-Promoted MoS2 in the Hydrodesulfurization of Dibenzothiophene. Catalysts. 2021; 11(11):1398. https://doi.org/10.3390/catal11111398
Chicago/Turabian StyleMajodina, Siphumelele, Zenixole R. Tshentu, and Adeniyi S. Ogunlaja. 2021. "Effect of Adding Chelating Ligands on the Catalytic Performance of Rh-Promoted MoS2 in the Hydrodesulfurization of Dibenzothiophene" Catalysts 11, no. 11: 1398. https://doi.org/10.3390/catal11111398