Method of removing hydrogen sulfide from gases utilizing a polyvalent metal chelate solution and regenerating the solution in a fuel cell

• US 4,436,711 A
• Filed: 09/30/1982
• Issued: 03/13/1984
• Est. Priority Date: 09/30/1982
• Status: Expired due to Term

• Current Assignee: Shell Oil Company (Shell Plc)
• Original Assignee: Shell Oil Company (Shell Plc)
• Inventors: Olson, Donald C.
• Primary Examiner(s): Thomas, Earl C.
• Application Number:
  US06/430,467
• Time in Patent Office: 530 Days
• Field of Search: 423/224, 423/226, 423/573 G, 423/573 R, 204/129-131, 429/17, 429/27
• US Class Current: 423/576.6
• CPC Class Codes: B01D 53/1425 Regeneration of liquid absorbents
• CPC Class Codes: B01D 53/1468 Removing hydrogen sulfide
• CPC Class Codes: B01D 53/1493 Selection of liquid materials for use as absorbents
• CPC Class Codes: C01B 17/05 by wet processes

Abstract

A process for the removal of H₂ S from sour gas streams is described, the process being characterized by the utilization of washing solutions containing oxidizing polyvalent metal chelates of specified amino-carboxylic acids, and by the regeneration of the spent solutions in a fuel cell mode.

Claims

1. A process for the removal of H₂ S from a sour gaseous stream comprising

(a) contacting the sour gaseous stream in a contacting zone with an aqueous reaction solution at a temperature below the melting point of sulfur, the solution containing an effective amount of an oxidizing reactant comprising a oxidizing polyvalent metal chelate of an acid having the formula ##STR3## wherein from two to four of the groups Y are selected from acetic and propionic acid groups;

from zero to two of the groups Y are selected from 2-hydroxyethyl, 2-hydroxy propyl, and ##STR4## wherein X is selected from acetic acid and propionic acid groups; and

R is ethylene, propylene or isopropylene or alternatively cyclohexane or benzene where the two hydrogen atoms replaced by nitrogen atoms are in the 1,2 position, and mixtures thereof; and

producing a sweet gas stream and an aqueous reaction solution containing crystalline sulfur, hydrogen ions and the reduced polyvalent metal chelate or chelates of said acid, said contacting zone comprising an anode section of an electrochemical cell, said electrochemical cell also comprising a separate cathode section containing a cathode connected through an external load to the anode, the anode section and cathode section being separated by a hydrogen ion permeable barrier;

(b) oxidizing reduced polyvalent metal chelate or chelates of said acid in the aqueous reaction solution, while concomitantly supplying oxygen to the cathode section and allowing hydrogen ions to migrate to the cathode section and producing direct current through the load, and water at the cathode;

(c) removing sulfur from the aqueous reaction solution, and water from cathode section.

4. The process of claim 1 wherein the aqueous reaction solution comprises a liquid absorbent selective for CO₂.

2. A process for the removal of H₂ S from a sour gaseous stream comprising

(a) contacting the sour gaseous stream in a contacting zone with an aqueous reaction solution at a temperature below the melting point of sulfur, the solution containing an effective amount of an oxidizing reactant comprising a oxidized polyvalent metal chelate of an acid having the formula ##STR5## wherein from two to four of the groups Y are selected from acetic and propionic acid groups;

from zero to two of the groups Y are selected from 2-hydroxyethyl, 2-hydroxy propyl, and ##STR6## wherein X is selected from acetic acid and propionic acid groups; and

R is ethylene, propylene or isopropylene or alternatively cyclohexane or benzene where the two hydrogen atoms replaced by nitrogen atoms are in the 1,2 position, and mixtures thereof; and

producing a sweet gas stream and an aqueous admixture containing crystalline sulfur, hydrogen ions and the reduced polyvalent metal chelate or chelates of said acid;

(b) removing sulfur from the aqueous admixture;

(c) regenerating aqueous admixture from step (b) by passing aqueous admixture from step (b) through the anode section of an electrochemical cell, said electrochemical cell also comprising a separate cathode section containing a cathode connected through an external load to the anode, the anode section and cathode section being separated by a hydrogen ion permeable barrier, and oxidizing reduced polyvalent metal chelate or chelates in the admixture at the anode to produce a regenerated aqueous admixture containing regenerated oxidizing polyvalent metal chelate or chelates while concomitantly supplying oxygen to the cathode section and allowing hydrogen ions to migrate to the cathode section, and producing direct current through said load and water at the cathode.

(d) removing regenerated aqueous admixture from said anode section, and water from said cathode section; and

(e) returning regenerated aqueous admixture to the contacting zone.

3. The process of claim 2 wherein the oxidizing reactant is the ferric chelate of N-(2-hydroxyethyl)ethylene diamine triacetic acid.

5. The process of claim 2 wherein the aqueous reaction solution comprises a liquid absorbent selective for CO₂.

6. The process of claim 3 wherein the aqueous reaction solution comprises a liquid absorbent selective for CO₂.