Process and device for treating a gas containing hydrogen sulfide, with recycling of the reduced catalytic solution

• US 6,589,498 B1
• Filed: 06/09/2000
• Issued: 07/08/2003
• Est. Priority Date: 06/10/1999
• Status: Expired due to Term

• Current Assignee: Institut Francais Du Petrole (IFP Energies Nouvelles)
• Original Assignee: Institut Francais Du Petrole (IFP Energies Nouvelles)
• Inventors: Huard, Thierry, Streicher, Christian, Barrere-Tricca, Cécile
• Primary Examiner(s): Silverman, Stanley S.
• Assistant Examiner(s): Vanoy, Timothy C.
• Application Number:
  US09/589,744
• Time in Patent Office: 1,124 Days
• Field of Search: 423/573.1, 423/576.2, 423/576.4, 423/576.5, 423/576.6, 481/277, 481/983
• US Class Current: 423/573.1
• CPC Class Codes: B01D 53/1468 Removing hydrogen sulfide

Abstract

A process intended for desulfurization of a gaseous feed containing hydrogen sulfide, includes at least the following stages: a) contacting the gaseous feed with a catalytic solution containing at least one polyvalent metal chelated by at least one chelating agent, under suitable conditions for oxidation of the hydrogen sulfide to elemental sulfur and concomitant reduction of the polyvalent metal from a higher oxidation level to a lower oxidation level, b) recovering on the one hand a gaseous effluent substantially freed from hydrogen sulfide and, on the other hand, the catalytic solution at least reduced and containing elemental sulfur, and c) recycling at least a fraction F₁ of the catalytic solution at least reduced and containing solid elemental sulfur to absorption stage a) so as to reduce the number of sulfur grains of very small size.

Claims

1. A process for desulfurization of a gaseous feed containing hydrogen sulfide, comprising at least the following stages:

a) contacting the gaseous feed with a catalytic solution containing at least one polyvalent metal chelated by at least one chelating agent to oxidize the hydrogen sulfide to elemental sulfur and concomitantly reduce the polyvalent metal from a higher oxidation level to a lower oxidation level in an absorption stage,

b) recovering a gaseous effluent substantially freed from hydrogen sulfide and said catalytic solution at least reduced and containing elemental sulfur, wherein at least a fraction F₁ of said catalytic solution at least reduced and containing solid elemental sulfur is recycled to the absorption stage a), and wherein the grain size of the sulfur grains suspended in the catalytic solution at least reduced after stage a) is determined and the quantity of recycled fraction F₁ of said solution is adjusted so as to maintain a desired grain size distribution of the particles.

2. A process as claimed in claim 1, wherein, in a stage c), the solid elemental sulfur is separated from a non-recycled fraction F₂ of the catalytic solution.

3. A process as claimed in claim 2, wherein at least a fraction of said non-recycled fraction F₂ from which said solid elemental sulfur has been separated in stage c) is at least partly regenerated, and at least part of the regenerated catalytic solution is recycled to a stage of contacting the regenerated solution with a gaseous feed consisting at least of hydrogen sulfide.

4. A process as claimed in claim 2, wherein the sulfur produced during separation stage c) is washed with water in order to recover the catalytic solution imbibing it and the catalytic solution is processed by reverse osmosis in order to control the water content of said catalytic solution.

5. A process as claimed in claim 2, wherein the sulfur produced during separation stage c) is washed with water in order to recover the catalytic solution imbibing it and the catalytic solution is processed by nanofiltration in order to control the proportion of at least water in the catalytic solution.

6. A process as claimed in claim 2, wherein separation stage c) is carried out by filtration and the grain size distribution range of the sulfur grains is selected according to the filtering means.

7. A process as claimed in claim 2, wherein at least part of the reduced catalytic solution freed from most of the elemental sulfur, obtained in stage c), is expanded.

8. A process as claimed in claim 2, wherein said reduced catalytic solution depleted in elementary sulfur from stage c) is fractionated into a fraction F₄ and a fraction F₃, fraction F₃ is expanded and non-expanded fraction F₄ is recycled to (absorption stage a).

9. A process as claimed in claim 8, further comprising measuring a potential of said reduced catalytic solution freed from most of the elemental sulfur obtained in stage c) prior to the fractionation stage, and controlling the quantity of said fractions F₃ and F₄ in order to maintain the ratio of the ferric ions to the ferrous ions between 0.1 and 100.

10. A process as claimed in claim 8, further comprising measuring a potential of said reduced catalytic solution freed from most of the elemental sulfur obtained in stage c) prior to the fractionation stage, and controlling the quantity of said fractions F₃ and F₄ in order to maintain the ratio of the ferric ions to the ferrous ions between 0.5 and 20.

11. A process as claimed in claim 1, wherein said gaseous feed containing hydrogen sulfide is natural gas.