System and method for sequestration and separation of mercury in combustion exhaust gas aqueous scrubber systems

• US 7,722,843 B1
• Filed: 11/26/2007
• Issued: 05/25/2010
• Est. Priority Date: 11/24/2006
• Status: Active Grant

• Current Assignee: Srivats Srinivasachar
• Original Assignee: Srivats Srinivasachar
• Inventors: Srinivasachar, Srivats
• Primary Examiner(s): Vanoy; Timothy C
• Application Number:
  US11/944,705
• Time in Patent Office: 911 Days
• Field of Search: 423/210, 423/243.01, 423/243.08, 422/168, 252/62.51 R, 252/62.56, 252/182.11, 252/182.32, 252/182.33, 502/400, 502/416, 502/417, 502/423, 951/34, 951/37
• US Class Current: 423/210
• CPC Class Codes: B01D 2251/404 of calcium
• CPC Class Codes: B01D 2253/102 Carbon
• CPC Class Codes: B01D 2255/20738 Iron
• CPC Class Codes: B01D 2257/302 Sulfur oxides
• CPC Class Codes: B01D 2257/602 Mercury or mercury compounds
• CPC Class Codes: B01D 2259/80 Employing electric, magnetic, electromagnetic or wave energy, or particle radiation
• CPC Class Codes: B01D 53/502 characterised by a specific solution or suspension
• CPC Class Codes: B01D 53/64 Heavy metals or compounds thereof, e.g. mercury
• CPC Class Codes: B01D 53/77 Liquid phase processes
• CPC Class Codes: B01J 20/02 comprising inorganic material
• CPC Class Codes: B01J 20/0229 Compounds of Fe
• CPC Class Codes: B01J 20/027 Compounds of F, Cl, Br, I
• CPC Class Codes: B01J 20/0281 Sulfates of compounds other than those provided for in B01J20/045
• CPC Class Codes: B01J 20/0288 Halides of compounds other than those provided for in B01J20/046
• CPC Class Codes: B01J 20/0296 Nitrates of compounds other than those provided for in B01J20/04
• CPC Class Codes: B01J 20/06 comprising oxides or hydroxides of metals not provided for in group B01J20/04
• CPC Class Codes: B01J 20/10 comprising silica or silicate
• CPC Class Codes: B01J 20/12 Naturally occurring clays or bleaching earth
• CPC Class Codes: B01J 20/16 Alumino-silicates B01J20/12 takes precedence
• CPC Class Codes: B01J 20/18 Synthetic zeolitic molecular sieves
• CPC Class Codes: B01J 20/20 : comprising free carbon; comprising carbon obtained by carbonising processes
• CPC Class Codes: B01J 20/223 : containing metals, e.g. organo-metallic compounds, coordination complexes
• CPC Class Codes: B01J 20/28009 : Magnetic properties
• CPC Class Codes: B01J 20/3204 : Inorganic carriers, supports or substrates
• CPC Class Codes: B01J 20/3236 : containing metal, other than zeolites, e.g. oxides, hydroxides, sulphides or salts

Abstract

A process, system and sorbent for removal of mercury from a combustion exhaust gas stream in a combustion exhaust gas purification scheme that includes a combustion exhaust scrubber system that uses an aqueous liquid to remove acid gases from the combustion exhaust gas. A powdered mercury sorbent is used. The sorbent is introduced into the aqueous scrubber liquid in the scrubber system. After introduction of the mercury sorbent into the scrubber liquid, at least some of the mercury sorbent is separated from the scrubber liquid.

Claims

1. A process for removal of mercury from a combustion exhaust gas stream in a combustion exhaust gas purification scheme that includes a combustion exhaust scrubber system that uses an aqueous liquid to remove acid gases from the combustion exhaust gas, the process comprising:

providing a powdered mercury sorbent comprising activated carbon that has been modified with a sulfur species;

introducing the powdered mercury sorbent into the aqueous liquid in the scrubber system; and

after introduction of the mercury sorbent into the aqueous liquid, separating at least some of the mercury sorbent and at least some of the aqueous liquid.

2. The process of claim 1 in which the aqueous liquid comprises a calcium-containing alkaline material selected from the group consisting of limestone, lime, magnesium-enhanced lime and dolomite.

3. The process of claim 1 in which the aqueous liquid comprises an alkaline substance that reacts with the acid gases to create a reaction product, and the combustion exhaust gas purification scheme further comprises separation of at least some of the reaction product from the aqueous liquid, and in which the reaction product is at least partially removed from the aqueous liquid based at least in part on its particle size and density.

4. The process of claim 3 in which the reaction product comprises gypsum, and at least most of the mercury sorbent has a particle size that is smaller than that of at least some of the gypsum, and at least most of the mercury sorbent is less dense than at least some of the gypsum.

5. The process of claim 4 in which the at least partial removal is accomplished at least in part with an inertial separation device.

6. The process of claim 5 further comprising removing mercury sorbent from the reaction product that was removed from the aqueous liquid by the inertial separation device.

7. The process of claim 1 in which the scrubber system comprises an aqueous liquid recirculation loop, and the mercury sorbent is introduced into the aqueous liquid recirculation loop.

8. A process for removal of mercury from a combustion exhaust gas stream in a combustion exhaust gas purification scheme that includes a combustion exhaust scrubber system that uses an aqueous liquid to remove acid gases from the combustion exhaust gas, the process comprising:

providing a powdered mercury sorbent in which at least some of the mercury sorbent is magnetic;

introducing the powdered mercury sorbent into the aqueous liquid in the scrubber system; and

after introduction of the mercury sorbent into the aqueous liquid, separating at least some of the mercury sorbent and at least some of the aqueous liquid.

9. The process of claim 8 in which the magnetic mercury sorbent comprises a magnetic component.

10. The process of claim 9 in which the magnetic component comprises an iron species.

11. The process of claim 10 in which the powdered mercury sorbent comprises activated carbon that has been modified with a sulfur species.

12. The process of claim 8 in which mercury sorbent is at least partially removed from the aqueous liquid by magnetic separation.

13. The process of claim 12 in which magnetic separation is accomplished with a high intensity magnetic separator or a permanent magnetic flocculator.

14. The process of claim 12 in which the aqueous liquid comprises an alkaline substance that reacts with the acid gases to create a reaction product, and the combustion exhaust gas purification scheme further comprises separation of at least some of the reaction product from the aqueous liquid, and the magnetic separation of the mercury sorbent from the aqueous liquid takes place before the separation of at least some of the reaction product from the aqueous liquid.

15. The process of claim 14 in which at least most of the mercury sorbent has a particle size that is smaller than that of at least some of the reaction product, and the reaction product is at least partially removed from the aqueous liquid based at least in part on particle size.

16. The process of claim 13 in which the activated carbon has been modified with halogen or a halogen-containing substance.

17. The process of claim 16 in which the activated carbon is treated with a material selected from the group of materials consisting of chlorine, bromine, iodine, fluorine, metal halides and ammonium halides, and then the treated activated carbon is heated to fix the halogen on the carbon.

18. The process of claim 15 in which at least most of the mercury sorbent is less dense than at least some of the reaction product, and the reaction product is at least partially removed from the aqueous liquid also based at least in part on density.

19. The process of claim 18 in which the at least partial removal is accomplished at least in part with an inertial separation device.

20. The process of claim 19 in which the reaction product comprises gypsum.

21. A process for removal of mercury from a combustion exhaust gas stream in a combustion exhaust gas purification scheme that includes a combustion exhaust scrubber system that uses an aqueous liquid to remove acid gases from the combustion exhaust gas, the process comprising:

providing a powdered mercury sorbent in which the mercury sorbent is mixed with a powder dispersing agent

introducing the powdered mercury sorbent into the aqueous liquid in the scrubber system; and

after introduction of the mercury sorbent into the aqueous liquid, separating at least some of the mercury sorbent and at least some of the aqueous liquid.

22. The process of claim 21 in which the powdered mercury sorbent comprises activated carbon that has been modified with a sulfur species.

23. The process of claim 21 in which the mercury sorbent comprises activated carbon that has been modified with halogen or a halogen-containing substance.

24. The process of claim 21 in which at least some of the mercury sorbent is magnetic.

25. A system for removal of mercury from a flue gas stream, comprising:

a wet flue gas desulfurization (FGD) scrubber system that uses an aqueous scrubbing liquor containing an alkaline substance that is sprayed into an absorber vessel to remove sulfur oxides from the flue gas through reaction between the alkaline substance and the sulfur oxides, the scrubber system comprising a scrubbing liquor recirculation loop that returns scrubbing liquor from the bottom portion of the absorber vessel to be sprayed in the vessel;

powdered, magnetic mercury sorbent;

a mercury sorbent storage system;

a feeder for introducing the mercury sorbent into the scrubbing liquor recirculation loop;

equipment for withdrawing a portion of the scrubbing liquor from the recirculation loop as a spent sorbent and reaction product stream;

a magnetic separator that receives the spent stream and removes at least some of the mercury sorbent from the spent stream; and

an inertial separation device downstream of the magnetic separator for removing at least some of the reaction product from the spent stream.

26. A mercury sorbent that can be used to remove solubilized mercury from an aqueous combustion exhaust gas stream scrubber liquor, comprising:

a powdered solid sorbent with a particle size such that about 90% of the particles are smaller than about 25 microns, in which the powdered solid sorbent comprises activated carbon that has been modified with at least a sulfur species; and

a magnetic substance coupled to the solid sorbent.

27. The mercury sorbent of claim 26 in which the activated carbon has a particle size such that about 90% of the particles are smaller than about 15 microns.

28. The mercury sorbent of claim 26 in which the activated carbon is treated with a material selected from the group of materials consisting of chlorine, bromine, iodine, fluorine, metal halides and ammonium halides, and then the treated activated carbon is heated to fix the halogen on the carbon.

29. The mercury sorbent of claim 26 in which the activated carbon has been modified with a sulfur species, and with halogen or a halogen-containing substance.