Competitive effects of hetero-atom containing compounds in the hydrodemetallisation of vanadyl-tetraphenyl-porphyrin
Heavy oil residua contain large amounts of hetero-atoms, such as sulfur, nitrogen, oxygen and metals. The metals, mainly vanadium and nickel, are removed by catalytic hydrotreatment. Sulfur, nitrogen and oxygen containing compounds present in heavy oil residua can influence the rate at which the met...
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Published in | Fuel (Guildford) Vol. 77; no. 12; pp. 1367 - 1375 |
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Main Authors | , , , , , |
Format | Journal Article |
Language | English |
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Oxford
Elsevier Ltd
01.10.1998
Elsevier |
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Abstract | Heavy oil residua contain large amounts of hetero-atoms, such as sulfur, nitrogen, oxygen and metals. The metals, mainly vanadium and nickel, are removed by catalytic hydrotreatment. Sulfur, nitrogen and oxygen containing compounds present in heavy oil residua can influence the rate at which the metals are removed, since they can adsorb competitively on the active site of the catalyst. Hence, the rate of the hydrogenation and ring cleavage steps in the hydrodemetallisation of the organo-metallic compounds may be slowed down. In the present work the competitive effect of hetero-atom containing compounds which are analogues of those occurring in heavy oil residua, i.e. quinoline, ammonia, benzofuran, water, dibenzothiophene and anthracene, has been investigated on the hydrodemetallisation of vanadyl-tetraphenyl-porphyrin. The spiked amount of hetero-atoms has been chosen near to those occurring in oil residua. The added hetero-atom containing compounds appeared to decrease the rate of metal removal. An increasing effect on the hydrogenation steps was found in the following sequence: dibenzothiophene < quinoline < anthracene ≈ benzofuran < ammonia ≈ water. For the lumped ring cleavage step the effect increased in the following sequence: dibenzothiophene < anthracene ≈ quinoline ≈ benzofuran < ammonia < water. The effect of quinoline, benzofuran, dibenzothiophene and anthracene is caused by competitive adsorption on the active sites of the catalyst. Water and ammonia, which have the most pronounced effect, are suggested to be co-ordinated to the vanadyl group in the porphyrin and, therefore, decrease the rate of metal removal. It is concluded that competitive adsorption of the reaction products from the ring cleavage of VO-TPP is negligible and that the presence of hetero-atom containing compounds in realistic feedstocks can decrease the rate of metal removal significantly. |
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AbstractList | Heavy oil residua contain large amounts of hetero-atoms, such as sulfur, nitrogen, oxygen and metals. The metals, mainly vanadium and nickel, are removed by catalytic hydrotreatment. Sulfur, nitrogen and oxygen containing compounds present in heavy oil residua can influence the rate at which the metals are removed, since they can adsorb competitively on the active site of the catalyst. Hence, the rate of the hydrogenation and ring cleavage steps in the hydrodemetallisation of the organo-metallic compounds may be slowed down. In the present work the competitive effect of hetero-atom containing compounds which are analogues of those occurring in heavy oil residua, i.e. quinoline, ammonia, benzofuran, water, dibenzothiophene and anthracene, has been investigated on the hydrodemetallisation of vanadyl-tetraphenyl-porphyrin. The spiked amount of hetero-atoms has been chosen near to those occurring in oil residua. The added hetero-atom containing compounds appeared to decrease the rate of metal removal. An increasing effect on the hydrogenation steps was found in the following sequence: dibenzothiophene < quinoline < anthracene ≈ benzofuran < ammonia ≈ water. For the lumped ring cleavage step the effect increased in the following sequence: dibenzothiophene < anthracene ≈ quinoline ≈ benzofuran < ammonia < water. The effect of quinoline, benzofuran, dibenzothiophene and anthracene is caused by competitive adsorption on the active sites of the catalyst. Water and ammonia, which have the most pronounced effect, are suggested to be co-ordinated to the vanadyl group in the porphyrin and, therefore, decrease the rate of metal removal. It is concluded that competitive adsorption of the reaction products from the ring cleavage of VO-TPP is negligible and that the presence of hetero-atom containing compounds in realistic feedstocks can decrease the rate of metal removal significantly. |
Author | Xu, Youming Moulijn, Jacob A. Janssens, Jean-Paul Tiong Sie, S. Witte, Gerald van Langeveld, A.Dick |
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CitedBy_id | crossref_primary_10_1021_acs_energyfuels_1c01228 crossref_primary_10_1016_S1389_1723_01_80032_3 crossref_primary_10_1081_CR_200057492 crossref_primary_10_1016_j_ces_2006_08_048 |
Cites_doi | 10.1016/0021-9517(83)90172-0 10.1016/0021-9517(85)90156-3 10.1021/i200024a004 10.1021/i200031a017 10.1016/S0167-2991(97)80166-8 10.1016/S0167-2991(08)62758-5 10.1016/0021-9517(94)90032-9 10.1016/0021-9673(92)87065-G 10.1016/S0065-2377(08)60101-5 10.1016/0021-9517(83)90155-0 10.1002/recl.19961151104 10.1021/ie00023a013 10.1021/ie00038a017 10.1006/jcat.1993.1077 10.1021/i260058a011 10.1016/0021-9517(86)90036-9 10.1016/0021-9517(78)90303-2 10.1016/S0021-9673(01)94589-3 10.1016/0021-9517(88)90328-4 10.1016/0021-9517(86)90277-0 10.1021/i200014a026 10.1016/0021-9517(84)90194-5 |
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Keywords | vanadyl-tetraphenyl-porphyrin hydrodemetallisation competition Vanadyl Porphyrin Refining Hydrodemetalation Heavy oil |
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SubjectTerms | Applied sciences competition Crude oil, natural gas and petroleum products Energy Exact sciences and technology Fuels hydrodemetallisation Processing of crude oil and oils from shales and tar sands. Processes. Equipment. Refinery and treatment units vanadyl-tetraphenyl-porphyrin |
Title | Competitive effects of hetero-atom containing compounds in the hydrodemetallisation of vanadyl-tetraphenyl-porphyrin |
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