Patent EA-003072-B1 (EA)
Title: Desulfurization process
IPC: B01D53/52
Filed: 1999-09-16
Abstract: 1. A process for removing sulfur from sulfur-containing carbonaceous materials, comprising: A. providing a carbonaceous material containing sulfur; B. contacting said carbonaceous material with a source of active oxygen in the presence of a base, using amounts of said active oxygen and said base effective to reduce the sulfur content of said carbonaceous material; and C. exposing said carbonaceous material to a source of energy of a type and under conditions effective to further reduce the sulfur content of said carbonaceous material. 2. The process of claim 1, wherein said carbonaceous material is a fossil fuel. 3. The process of claim 1, wherein said carbonaceous material is a petroleum product. 4. The process of claim 1, wherein said carbonaceous material is coal. 5. The process of claim l, wherein said source of active oxygen is a peroxide. 6. The process of claim l, wherein said source of active oxygen is aqueous hydrogen peroxide solution. 7. The process of claim 1, wherein said source of active oxygen is an ozone generator. 8. The process of claim 1, wherein said base is added to said source of active oxygen. 9. The process of claim 1, wherein said contacting step is carried out by adding a base to said source of active oxygen to form a source of basic active oxygen, then combining said source of basic active oxygen with said carbonaceous material. 10. The process of claim 9, where said contacting step is carried out by combining said carbonaceous material, said source of basic active oxygen, and a mutual solvent for said carbonaceous material and said source of basic active oxygen. 11. The process of claim 1, where said contacting step is earned out in the presence of a fluid having one of the following structures:   wherein X and Z are independently selected from C=O and -O-; Y is independently selected from X, -OR2O- or a direct linkage between R1 and R2; R1 is selected from hydrogen or an independently selected R2 as defined below; R2 is selected from straight or branched chain alkyl, alkenyl, or alkynyl having from 1 to 16 carbon atoms, aralkyl having a single ring or multiple ring aryl having from 6 to 24 carbon atoms attached to a straight or branched chain alkyl, alkenyl, or alkynyl as previously defined. 12. The process of claim 11, wherein X and Z are either linkages. 13. The process of claim 1, where said contacting step is carried out in the presence of a fluid selected from the group consisting of: diethyl ether, isopropyl ether, butyl ether, ethyl methyl ether, ethyl n-butyl ether, tetrahydrofuran, dioxane, furan, α-pyran, γ-pyran, δ-trioxane, ethylene oxide, propylene oxide, acetone, methyl isobutyl ketone, formaldehyde. acetaldehyde, methanol ethanol, and combinations thereof. 14. The process of claim 1, where said contacting step is carried out in the presence of diethyl ether. 15. The process of claim 1, wherein said base is a hydroxide. 16. The process of claim 1, wherein said base is sodium hydroxide. 17. The process of claim 1, wherein said energy is selected from the group consisting of alpha radiation, beta radiation, gamma radiation, x-radiation, ultraviolet radiation, visible light radiation, infrared radiation, microwave radiation, radiation resulting from radioactive decay, ultrasonic energy, and combinations thereof. 18. The process of claim 1, wherein said energy comprises x-radiation. 19. The process of claim 1, wherein said energy comprises ultrasonic energy. 20. The process of claim 1, wherein said source of active oxygen is watersoluble, further comprising the step of separating said carbonaceous material from said source of active oxygen after said contacting step. 21. The process of claim 1, wherein said contacting step generates a sulfurcontaining gas, further comprising the step of separating said sulfur-containing gas from said carbonaceous material. 22. The process of claim 21, further comprising the step of extracting elemental sulfur from said sulfur-containing gas. 23. The process of claim 21, further comprising the step of oxidizing said sulfur-containing gas, forming sulfur oxides. 24. The process of claim 23, further comprising the step of reacting said sulfur oxides with lime, forming calcium sulfate. 25. The process of claim 1, wherein said carbonaceous material as provided is classified as a high-sulfur fuel, and said carbonaceous material after said contacting step is classifies as a low-sulfur fuel. 26. The process of claim 1, wherein said carbonaceous material as provided contains at least about 2% by weight elemental sulfur, and said carbonaceous material after said contacting step contains less than about 1% by weight sulfur. 27. The process of claim 1, wherein said carbonaceous material as provided contains at least about 2% by weight elemental sulfur, and said carbonaceous material after said contacting step contains less than about 0.5% by weight sulfur. 28. The process of claim 1, wherein said carbonaceous material as provided contains at least about 1% by weight elemental sulfur, and said carbonaceous material after said contacting step contains less than about 0.5% by weight sulfur. 29. The process of claim 1, wherein said contacting step is carried out at a temperature between about 0 degree C and about 121 degree C. 30. The process of claim 1, wherein said contacting step is carried out at a pressure of from about 0.1 atmosphere to about 2 atmospheres. 31. A process for removing sulfur from sulfur-containing carbonaceous materials, comprising: A. providing a carbonaceous material containing sulfur; and  B. contacting said carbonaceous material with a source of active oxygen, a base, and a solvent under conditions effective to reduce the sulfur content of said carbonaceous material; said solvent having one of the following structures:   wherein X and Z are each -O-; Y is independently selected from -O-, OR2O-, or a direct linkage between R1 and R2; R1 is selected from hydrogen or an independently selected R2 as defined below; R2 is selected from straight or branched chain alkyl, alkenyl, or alkynyl having from 1 to 16 carbon atoms, aralkyl having a single ring or multiple ring aryl having from 6 to 24 carbon, atoms attached to a straight or branched chain alkyl, alkenyl, or alkynyl as previously defined. 32. The process of claim 31, wherein said solvent is an aliphatic ether. 33. The process of claim 31, wherein said solvent is diethyl ether. 34. A reduced-sulfur carbonaceous material made by the process of claim 1. 35. A reduced-sulfur carbonaceous material made by the process of claim 31. 36. Treated California heavy crude oil having a sulfur content of less than shout 1% by weight. 37. Treated California heavy crude oil having a sulfur content of less than about 0.5% by weight. 38. The process of claim 1, wherein said energy comprises ultraviolet radiation. 39. The process of claim 1, wherein said energy comprises visible light radiation. 40. The process of claim 1, wherein said energy comprises microwave radiation. 41. The process of claim 1, wherein said energy comprises radiation resulting from radioactive decay.