This invention utilizes a novel method and set of operating conditions to efficiently and economically process a potentially very fouling hydrocarbon feedstock. A multi-stage catalytic process for the upgrading of coal pyrolysis oils is developed. Coal Pyrolysis Oils are highly aromatic, olefinic, u
This invention utilizes a novel method and set of operating conditions to efficiently and economically process a potentially very fouling hydrocarbon feedstock. A multi-stage catalytic process for the upgrading of coal pyrolysis oils is developed. Coal Pyrolysis Oils are highly aromatic, olefinic, unstable, contain objectionable sulfur, nitrogen, and oxygen contaminants, and may contain coal solids which will plug fixed-bed reactors. The pyrolysis oil is fed with hydrogen to a multi-stage ebullated-bed hydrotreater and hydrocracker containing a hydrogenation or hydrocracking catalyst to first stabilize the feed at low temperature and is then fed to downstream reactor(s) at higher temperatures to further treat and hydrocrack the pyrolysis oils to a more valuable syncrude or to finished distillate products. The relatively high heat of reaction is used to provide the energy necessary to increase the temperature of the subsequent stage thus eliminating the need for additional external heat input. A refined heavy oil product stream is recycled to the fresh feed to minimize feedstock fouling of heat exchangers and feed heaters.
대표청구항▼
1. A process of processing coal pyrolysis oils containing at least 15% wt of compounds boiling below 360° C. and less than 40% wt boiling at least at 520° C. said coal pyrolysis oil also containing less than 20% wt of particles of coal having a size of less than 1 mm, and at least 1% wt of oxygenate
1. A process of processing coal pyrolysis oils containing at least 15% wt of compounds boiling below 360° C. and less than 40% wt boiling at least at 520° C. said coal pyrolysis oil also containing less than 20% wt of particles of coal having a size of less than 1 mm, and at least 1% wt of oxygenated compounds (calculated as oxygen), said process comprising: a) combining a hydrogen stream with coal pyrolysis oil feedstock;b) feeding the combined stream from step a) to a first ebullated-bed reactor to remove compounds including olefins, diolefins, and nitrogen, sulfur, and oxygen contaminates and create a stabilized stream; andc) feeding said stabilized stream to a second ebullated-bed reactor to remove some additional heteroatoms and convert the stream to lower boiling hydrocarbons; andwherein said first ebullated-bed reactor from step b) is always operated at a temperature of at least 15°C. less than said second ebullated-bed reactor of step c) and wherein steps a-c result in the conversion of the 343° C.+ material in said coal pyrolysis oil feedstock in the range of between 10 wt % and 99 wt %. 2. The process of claim one wherein steps a-c result in the conversion of the 343° C.+ material in said coal pyrolysis oil feedstock of greater than 30 wt %. 3. The process of claim one wherein steps a-c result in the conversion of the 343° C.+ material in said coal pyrolysis oil feedstock of greater than 50 wt %. 4. The process of claim one wherein steps a-c result in the conversion of the 343° C.+ material in said coal pyrolysis oil feedstock of greater than 75 wt %. 5. The process of claim one wherein steps a-c result in the conversion of the 343° C.+ material in said coal pyrolysis oil feedstock of greater than 90 wt %. 6. The process of claim one wherein steps a-c result in the conversion of the 343° C.+ material in said coal pyrolysis oil feedstock of greater than 95 wt %. 7. The process of claim one wherein steps a-c result In the reduction of sulfur, nitrogen, and oxygen contaminants In said coal pyrolysis oil feedstock of greater than 70%. 8. The process of claim one wherein steps a-c result in the reduction of sulfur, nitrogen, and oxygen contaminants in said coal pyrolysis oil feedstock of greater than 90%. 9. The process of claim one wherein steps a-c result in the reduction of sulfur, nitrogen, and oxygen contaminants in said coal pyrolysis oil feedstock of greater than 95%. 10. The process of claim one wherein the first ebullaled-bed reactor from step b) is operated at 360° C-420° C., and 69-275 bars hydrogen partial pressure and at a feed rate of 0.5-2.0 volume of feed/hr/settled volume of catalyst in the reactor. 11. The process of claim one wherein the second ebullated-bed reactor from step c) is operated at a temperature of 400-440° C., 69-275 bars hydrogen partial pressure, and a feed rate of 0.2-2.0 volume of feed/hr/settled volume of catalyst in the reactor. 12. The process of claim one wherein a separate heavy oil product stream nominally boiling above 343° C.+ is recycled and blended with the hydrogen stream and coal pyrolysis oil feedstock of step a). 13. The process of claim one wherein the spent catalyst from the ebullated-bed in step b) is cascaded to and used In the ebullated-bed reactor of step c). 14. The process of claim one wherein a separate phenolics stream is combined and processed with the hydrogen stream and coal pyrolysis oil feedstock of step a). 15. The process of claim 14 in which said phenolics stream is combined and processed with the hydrogen stream and coal pyrolysis oil feedstock of step a) at a concentration of 5 wt % to 50 wt % of the coal pyrolysis oil feedstock. 16. The process of claim 15 wherein additional hydrogen is fed to the ebullated-bed reactor of step c). 17. The process of claim 1 wherein crude naphtha is combined and processed with the hydrogen stream and coal pyrolysis oil feedstock of step a) at a concentration of 3 wt % to 30 wt % of the coal pyrolysis oil feedstock. 18. The process of claim one wherein a separate stream, selected from a group consisting of: FCC slurry oil, FCC light cycle oil, decant oil, anthracene oil, coke oven oils, petroleum derived pyrolysis oils, and steam cracker tars, is combined and processed with the hydrogen stream and coal pyrolysis oil in step a). 19. The process of claim 1 wherein a separate heavy wax stream from Fischer-Tropsch processing of synthesis gases, which may contain solids such as catalyst fines, is combined and processed with the hydrogen stream and coal pyrolysis oil feedstock of step a). 20. The process of claim 19 wherein said heavy wax stream from Fischer-Tropsch processing of synthesis gases, which may contain solids such as catalyst fines, is combined and processed with the hydrogen stream and coal pyrolysis oil feedstock of step a) at a concentration of 3 wt % to 30 wt % of the coal pyrolysis oil feedstock. 21. The process of claim 1 wherein the solids content of the coal pyrolysis oils is less than 10 wt. %. 22. The process of claim 1 wherein the solids content of the coal pyrolysis oils is less than 1 wt. %. 23. A process of processing coal pyrolysis oils containing at least 15% wt of compounds boiling below 360° C. and less than 40% wt boiling at least at 520° C. said coal pyrolysis oil also containing less than 20% wt of particles of coal having a size of less than 1 mm, and at least 1% wt of oxygenated compounds (calculated as oxygen), said coal pyrolysis oil being obtained from a process for treating coat, said process comprising: a. combining a hydrogen stream with a coal pyrolysis oil feedstock;b. feeding the combined stream from step a) to a first ebullated-bed reactor to remove compounds as olefins, diolefins, and nitrogen, sulfur, and oxygen contaminates and create a stabilized stream; andc. feeding said stabilized stream to a second ebullated-bed reactor to remove some heteroatoms and convert the 343° C+ materials in the stream;d. feeding said converted stream to one or more additional ebullated-bed reactors for further heteroatom removal and for conversion of the 343° C.+ materials; andwherein said first ebullated-bed reactor from step b) is always operated at a temperature of at least 15° C. less than said second ebullated-bed reactor of step c) and wherein steps a-d result in the conversion of the 343° C.+ material in said coal pyrolysis oil feedstock in the range of between 10 wt % and 99 wt %.
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이 특허에 인용된 특허 (10)
Colyar James J. ; MacArthur James B. ; Peer Eric D., Catalytic hydrogenation process utilizing multi-stage ebullated bed reactors.
MacArthur James B. (Denville NJ) McLean Joseph B. (So. Somerville NJ) Comolli Alfred G. (Yardley PA), Catalytic two-stage coal hydrogenation and hydroconversion process.
MacArthur James B. (Denville NJ) Comolli Alfred G. (Yardley PA) McLean Joseph B. (Somerville NJ), Catalytic two-stage coal hydrogenation process using extinction recycle of heavy liquid fraction.
McLean Joseph B. (S. Somerville NJ) Comolli Alfred G. (Yardley PA) MacArthur James B. (Denville NJ), Catalytic two-stage liquefaction of coal utilizing cascading of used ebullated-bed catalyst.
Hippo Edwin J. (Makanda IL) Comolli Alfred G. (Yardley PA) O\Brien Robert (Jackson NJ), Hydrogenation of coal and subsequent liquefaction of hydrogenated undissolved coal.
Trachte Kenneth L. (Baton Rouge LA) Lasko Willian (Flanders NJ) Effron Edward (Springfield NJ) Stuntz Gordon F. (Baton Rouge LA) Chomyn Karl D. (Denville NJ), Three-stage process for producing ultra-clean distillate products.
Jung Henry ; Gupta Ramesh ; Ellis Edward S. ; Lewis William E., Two stage hydroprocessing with vapor-liquid interstage contacting for vapor heteroatom removal.
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