Process for removal of hydrogen sulfide from a gas stream

• US 5,733,516 A
• Filed: 09/09/1996
• Issued: 03/31/1998
• Est. Priority Date: 09/09/1996
• Status: Expired due to Term

• Current Assignee: URS Corporation (Aecom Incorporated)
• Original Assignee: Gas Research Institute (GTI Energy)
• Inventors: DeBerry, David W.
• Primary Examiner(s): Straub, Gary P.
• Assistant Examiner(s): Vanoy, Timothy C.
• Application Number:
  US08/711,122
• Time in Patent Office: 568 Days
• Field of Search: 423/226, 423/228, 423/220, 423/562, 423/573.1, 423/578.1, 423/575, 423/571
• US Class Current: 423/220
• CPC Class Codes: B01D 53/1468 Removing hydrogen sulfide
• CPC Class Codes: B01D 53/52 Hydrogen sulfide
• CPC Class Codes: B01D 53/73 After-treatment of removed components
• CPC Class Codes: C01B 17/05 by wet processes

Abstract

A process and system for removing hydrogen sulfide from a gaseous stream such as one of natural gas. A sour gas stream containing H₂ S is contacted with a nonaqueous, water-insoluble sorbing liquor which comprises an organic solvent for elemental sulfur, dissolved elemental sulfur, an organic base to promote the reactions, and an organic solubilizing agent an agent suitable for maintaining the solubility of polysulfide intermediates which may otherwise separate when they are formed during operation of the process. Hydrogen sulfide (H₂ S) gas is sorbed into this liquor and then reacts with the dissolved sulfur in the presence of the base to form polysulfide molecules. The solution is then sent to a reactor where sufficient residence time is provided to allow the polysulfide forming reactions to reach the desired degree of completion. From the reactor, the solution flows to a regenerator where the solution is oxidized (e.g., by contact with air), forming dissolved elemental sulfur and water. The temperature of the solution is then lowered, forming sulfur crystals, which are easily removed by gravity settling, filtration, centrifuge, or other separation method. Enough sulfur remains dissolved in the solution following removal of the sulfur crystals that when this solution is reheated and returned to the absorber a sufficient amount of sulfur is present to react with the inlet H₂ S gas.

Claims

1. A process for removing H₂ S from a gaseous stream, comprising the steps of:

(a) contacting the H₂ S-containing gaseous stream with a sorbing liquor comprising a nonaqueous solvent containing dissolved sulfur, and a base consisting essentially of a tertiary amine having sufficient strength and concentration to drive the reaction converting H₂ S sorbed by said liquor and reacting with said dissolved sulfur, to form nonvolatile polysulfide which is soluble in the sorbing liquor;

(b) converting the dissolved nonvolatile polysulfide in said sorbing liquor to sulfur which remains dissolved in said liquor by contacting said liquor from step (a) with an oxidizing gas;

(c) converting at least part of said dissolved sulfur in the liquor from step (b) to solid particulate sulfur; and

(d) separating said solid sulfur from step (c) from the liquor.

2. A process in accordance with claim 1, wherein said nonaqueous solvent is water-insoluble.

3. A process in accordance with claim 2, wherein said sorbing liquor includes a solubilizing agent for maintaining the solubility of polysulfide intermediates which may otherwise separate during the process.

4. A process in accordance with claim 3, further including recycling the sorbing liquor separated from the sulfur for further contact with the H₂ S-containing gaseous stream.

5. A process in accordance with claim 3, wherein said nonaqueous solvent has a solubility for sulfur in the range of about 0.05 to 3.0 g-moles of sulfur per liter of solution.

6. A process in accordance with claim 3, wherein said base is selected from the group consisting of 2-(dibutylamino)ethanol, N-methyldicyclohexylamine, N-methyldiethanolamine, tributylamine, dodecyldimethylamine, tetradecyldimethylamine, hexadecyldimethylamine and mixtures thereof.

7. A process in accordance with claim 3, wherein said solubilizing agent is selected from the group consisting of benzyl alcohol, benzhydrol, 3-phenyl-1-propanol, tri(ethylene glycol), alkylaryl polyether alcohols and mixtures thereof.

8. A process in accordance with claim 3, wherein said nonaqueous solvent is selected from the group consisting of 1,2,3,4 tetrahydronaphthalene, N,N dimethylaniline, diphenyl ether, dibenzyl ether, partially hydrogenated terphenyls, partially hydrogenated diphenyl ethanes, and mixtures thereof.

9. A process in accordance with claim 3 wherein said precipitated sulfur is purified by washing with a solvent for removal of residual traces of said nonaqueous solvent.

10. A process in accordance with claim 3, wherein byproduct sulfur salts are removed from the nonaqueous solvent, when said solvent is water insoluble, by water or aqueous alkalai washing said solvent.

11. A process in accordance with claim 4, wherein at least part of said dissolved sulfur is converted to a solid by cooling the sorbing liquor, following said oxidation of said polysulfide, to a temperature at which said solid particulate sulfur precipitates.

12. A process in accordance with claim 11, wherein said sorbing liquor is at a temperature in the range of about 15°

C. to 70°

C. before being cooled.

13. A process in accordance with claim 12, wherein said sorbing liquor is cooled 5°

C. to 20°

C. to effect said sulfur precipitation.

14. A process in accordance with claim 11, wherein enough dissolved sulfur remains in said sorbing liquor following separation of the precipitated sulfur that when said solution is returned to the absorber for recycling in the process, a sufficient amount of sulfur is present to react with the inlet H₂ S gas.