Combined Effects of EDTA and Heteroatoms (Ti, Zr, and Al) on Catalytic Activity of SBA-15 Supported NiMo Catalyst for Hydrotreating of Heavy Gas Oil
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Bibliographic record
Abstract
M-SBA-15 (M = Ti, Al, and Zr) materials with a Si/M ratio of 20 were synthesized using a direct synthesis method. M-SBA-15 supported NiMo hydrotreating catalysts with and without EDTA was prepared by an incipient wetness impregnation method. A EDTA/Ni molar ratio of 2 was used for catalysts with EDTA. The hydrotreating activities of these catalysts were measured using Athabasca bitumen derived heavy gas oil, and comparison was done with the performance of NiMo/SBA-15 and NiMo/γ-Al 2 O 3 catalysts. All catalysts were thoroughly characterized by BET, TPR, TPD, CO-chemisorption, XRD, XANES, HRTEM, ICP-MS, and 13 C NMR. Incorporation of Ti, Al, and Zr in SBA-15 framework results in an increase in the surface acidity and metal support interactions in otherwise neutral SBA-15 material. This increases the dispersion, and HDS, HDN and HDA activity of a NiMo/SBA-15 catalyst increases by 12%, 70%, and 22%, respectively, as in the case of a NiMo/Ti-SBA-15 (Cat-Ti) catalyst. EDTA addition helps in better redispersion of molybdenum during sulfidation/activation as indicated by HRTEM and CO chemisorption studies. A XANES Mo LIII-edge study for the oxide state of catalysts reveals that EDTA helps in the formation of a greater number of molybdenum in octahedral structures which are easily reducible during sulfidation as compared to molybdenum in tetrahedral structures. A power law based kinetic study indicates that addition of EDTA lowers the activation energy, which could be due to formation of a more favorable Type II NiMoS active site. The activity studies show that using EDTA increases the HDS, HDN, and HDA activity of a NiMo/M-SBA-15 catalyst by 18%, 36%, and 22%, respectively, as in the case of a NiMo/Ti-SBA-15/2EDTA (Cat-TiE) catalyst. Based on the results from different characterization techniques, the schematic is presented related to the effect of EDTA-Mo-support interactions on dispersion of active metals in catalysts. The results from characterization techniques are in parallel with catalytic activity which follows the order Cat-TiE > Cat-AlE > Cat-ZrE > Cat- Ti. However, the catalytic activity of Cat-TiE is almost comparable to that of a NiMo/γ-Al 2 O 3 catalyst and has the potential for superior hydrotreating catalyst.
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Full frame distilled prediction
Teacher imitationNot calibrated prevalence, not ground truth. Human validation pending. Learned from the 10,348 direct Codex labels and 10,348 direct Gemma labels. Candidate is the union of thresholded teacher heads; consensus is their intersection. These outputs are machine_predicted_unvalidated and are not human labels or direct frontier model labels.
Codex and Gemma teacher scores by category
| Category | Codex | Gemma |
|---|---|---|
| Metaresearch | 0.001 | 0.001 |
| Meta-epidemiology (narrow) | 0.000 | 0.000 |
| Meta-epidemiology (broad) | 0.001 | 0.000 |
| Bibliometrics | 0.000 | 0.000 |
| Science and technology studies | 0.000 | 0.000 |
| Scholarly communication | 0.000 | 0.000 |
| Open science | 0.000 | 0.000 |
| Research integrity | 0.000 | 0.000 |
| Insufficient payload (model declined to judge) | 0.000 | 0.000 |
Machine scores (provisional)
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Baseline scores from an immature model (maturity gate not passed, 7 training rounds). Scores rank; they never assert a category.
score_only:v0-immature-baseline · verbatim from the scoring run: score_only means the number may rank works, and no category label ships from it