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United States Patent (19) 11 Patent Number: 4,457,693 Mckay (45) Date of Patent: Jul

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United States Patent (19) 11 Patent Number: 4,457,693 Mckay (45) Date of Patent: Jul United States Patent (19) 11 Patent Number: 4,457,693 McKay (45) Date of Patent: Jul. 3, 1984 (54) COMBUSTION PROCESS (56) References Cited (75) Inventor: Dwight L. McKay, Bartlesville, Okla. U.S. PATENT DOCUMENTS 73) Assignee: Phillips Petroleum Company, 4,033,861 7/1977 Holloway et al. .................. 208/211 Bartlesville, Okla. 4,036,740 7/1977 Readal et al. ...... ... 208/120 4,133,644 1/1979 Holloway et al. ... 422/138 (21) Appl. No.: 371,369 4,146,463 3/1979 Radford et al. ..................... 208/120 22 Filed: Apr. 23, 1982 4,280,898 7/1981 Tatterson et al. .............. 208/120 X Primary Examiner-Samuel Scott Related U.S. Application Data Assistant Examiner-Randall L. Green 63) Continuation-in-part of Ser. No. 117,927, Feb. 4, 1980, 57 ABSTRACT Pat. No. 4,335,021. A combustion catalyst containing both manganese and (51) Int. Cl. .......................... F23Q3/00; B01J 29/06 antimony in a temperature range of above about 1260 (52) U.S. C. ........................................ 431/2; 431/268; F. has been found to result in unexpectedly high 208/120; 502/.65; 502/241; 502/.324 CO2/CO ratios in the regenerator off-gas when CO is 58 Field of Search ..................... 431/2, 5, 7, 10, 268, combusted. 431/326; 252/471, 417; 423/239, 247, 244 R; 208/120; 252/455 R, 416, 455 Z, 456 14 Claims, 6 Drawing Figures (CATALYST B WITH Mn 8 Sb) CO COMBUSION 8OO 90O 1OOO 11 OO 2OO 3OO 14OO TEMPERATURE F U.S. Patent Jul. 3, 1984 Sheet 1 of 2 4,457,693 A/G / 9 (CATALYST OUNTREATED ) A/G 2 9 (CATALYST A WITH MnSb) A/G 3 (CATALYST B, WITH MnSb) c O - O 2 O CD n S. d 12 A/G 4 9 (CATALYST C. WITH Mn.) A/G 5 (CATALYST D WH Sb) 8OO 900 OOO 11 OO 12OO 3OO 14OO TEMPERATURE OF U.S. Patent Jul. 3, 1984 Sheet 2 of 2 4,457,693 (CATALYST B WITH Mn & So) CO COMBUSTION 8OO 9OO 1OOO 1 OO 12OO 3OO 14OO TEMPERATURE F 4,457,693 1. 2 the combustion is carried out in a very limited tempera COMBUSTION PROCESS ture range of 1260-1280 F. In addition, it has been discovered in accordance This application is a continuation-in-part of applica with this invention that a catalyst containing both anti tion Ser. No. 117,927, filed Feb. 4, 1980, now U.S. Pat. mony and manganese catalyzes a combustion process in No. 4,335,021. which carbonaceous fuel and free oxygen are passed in This invention relates to a combustion process. In contact with such a catalyst under combustion condi another aspect, this invention relates to the regeneration tions to produce an off-gas with high CO2/CO ratio. of catalyst that are useful for cracking hydrocarbons. In Thus, in accordance with one embodiment of this another aspect, this invention relates to a hydrocarbon 10 invention a process for combustion of carbonaceous cracking process. material is provided for. In accordance with another embodiment of this in BACKGROUND vention a cracking process is provided for in which a It is well known in the art that cracking of hydrocar hydrocarbon feedstock is cracked in a cracking zone bons with silica or silica/alumina base catalysts pro 15 with a cracking catalyst containing manganese and duces coke on such catalysts which can be burned off. antimony; the cracking catalyst containing manganese One of the problems arising in the cracking step consists and antimony is then subjected to a regeneration by in the detrimental effects brought about by such metals contacting it with a free oxygen containing gas at a as nickel, vanadium, and iron contained in many hydro temperature of 1260-1280. F.; thereafter the regener carbon feedstocks. These metals cause production of 20 ated cracking catalyst is again utilized for the cracking hydrogen and coke. A problem arising in the catalyst step. regeneration step resides in the fact that the ratio of It has surprisingly been found that manganese and carbon dioxide to carbon monoxide normally decreases antimony together result in a synergistic improvement with increasing temperature. Therefore, although high and increase of CO2/CO ratio of the regenerator off-gas 25 when these metals are present on a catalyst in a crack temperatures are a desirable process parameter, it is not ing/regeneration cycle. Manganese and antimony are feasible to increase the temperature since this would passivating agents for the contaminating metals such as lead to a further decrease in an already low carbon nickel, vanadium and iron causing a reduction of hydro dioxide to carbon monoxide ratio in the off gases. gen and coke produced during the cracking process and It has been claimed in the art that antimony, bismuth 30 also have the additional function of strongly increasing and manganese added to a cracking catalyst increased the CO2/CO ratio as described. Antimony or a com the carbon dioxide to carbon monoxide ratio. The art pound thereof and manganese or a compound thereof gives examples utilizing antimony and bismuth. There is together in addition to their metals passivation effect a continuing interest in increasing the CO2/CO volume cause an increase in the carbon combustion from cata ratio in a catalyst regeneration step. 35 lyst during the regeneration thus releasing more heat in STATEMENT OF THE INVENTION the regenerator. At the same time, the quantity of car bon monoxide released is reduced. The latter is of par It is thus one object of this invention to provide a ticular significance where a portion or all of the regen process for combusting carbonaceous materials on cata erator off-gases are released to the atmosphere. lyst particles with a high carbon dioxide to carbon mon 40 A second embodiment of this invention resides in a oxide ratio. combustion process. This combustion process in accor Another object of this invention is to provide a crack dance with this invention is characterized by subjecting ing process including a catalyst regeneration step in carbonaceous fuel and free oxygen in contact with cata which process both the detrimental effects of metals lyst containing both manganese and antimony to com such as nickel, vanadium, and iron are mitigated and the 45 bustion conditions. The carbonaceous fuel is separate CO2/CO ratio of the regeneration off gases is maxi from and not adhering to the catalyst. The fuel and mized. oxygen forming a combustible mixture are passed in A yet further object of this invention is to provide a fluid contact with the catalyst under combustion condi combustion process in which a carbonaceous fuel and tions to yield the off-gas with the high CO2/CO ratio. free oxygen are subjected to combustion conditions and 50 a off-gas having a high CO2/CO ratio is produced. Fuels These and other objects, advantages, details, and The fuels useful for the combustion process of this features of this invention will become apparent to those invention are gaseous, normally liquid or normally solid skilled in the art from the following detailed description carbonaceous materials. The gaseous carbonaceous thereof and the appended claims. 55 materials include such gases as carbon monoxide, meth ane, propane or mixtures thereof. The preferred gaseous BRIEF DESCRIPTION OF THE DRAWINGS fuel is carbon monoxide in view of the discovery that FIGS. 1-5 show a graphic representation of regener carbon monoxide and free oxygen in contact with the ation data with the carbon dioxide to carbon monoxide catalyst defined above is converted to a gas having a volume ratio plotted versus the temperature in F., and 60 high CO2/CO ratio. Liquid carbonaceous fuels useful in FIG. 6 shows a graphic representation of a combus accordance with this invention include paraffinic, ole tion process with the carbon dioxide to carbon monox finic or aromatic liquid fuels and oils such as kerosene, ide volume plotted versus the temperature in F. gasoline, fuel oils, etc. Among the solid carbonaceous In accordance with this invention it has now been material useful as fuel in accordance with this invention found that carbonaceous material accumulated on 65 graphite, tar sand, coal, char, oil shale, wood, soot, cracking catalyst can be burned off with a very high combustion byproducts, etc. should be mentioned. CO2/CO volume ratio in the produced gases if the When solid carbonaceous materials are used in the pro catalyst contains both antimony and manganese and if cess of this invention these fuels are utilized in finely 4,457,693 3 4. divided form and the catalyst is used in particulate form The concentration of manganese and antimony on the also. In a variation of this process it is within the scope cracking catalyst can be related to the total effective of this invention to first combust the fuel and free oxy metals content of the feedstock as shown in the follow gen to form an off-gas and subject this off-gas which ing table. still contains CO and free oxygen to a further combus tion step in contact with the manganese and antimony Total Effective Metals Min -- Sb Concentration containing catalyst to yield a secondary off-gas which in Feedstock (ppm)' in Catalyst, Wt. 2% has the high CO2/CO ratio. In this variation of the 1-40 0.01-0.6 process, which is particularly applicable to solid fuels, 40-100 0.05-0.8 ashes can be separated between the two combustion 10 100-200 0.1-1 steps thus minimizing the quantity of ash materials and 200-300 0.15-1.5 solid particles actually contacting the catalyst.
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