Process for the removal of hydrogen sulfide from a gas stream

• US 5,730,784 A
• Filed: 06/05/1995
• Issued: 03/24/1998
• Est. Priority Date: 12/06/1989
• Status: Expired due to Term

• Current Assignee: Eco-Tec Ltd.
• Original Assignee: Apollo Environmental Systems Corp., University of Toronto Innovations Foundation
• Inventors: Smith, James W., Harbinson, John N., Ellenor, David Todd R.
• Primary Examiner(s): Reifsnyder, David A.
• Application Number:
  US08/462,692
• Time in Patent Office: 1,023 Days
• Field of Search: 426/220, 426/224, 426/226, 426/576.4, 426/576.6, 422/168, 210/221.1, 210/221.2, 210/242.2, 210/703, 210/704, 210/758, 210/787, 261/84, 423/224, 423/242.1, 423/242.2, 95/181, 95/261
• US Class Current: 95/181
• CPC Class Codes: B01D 21/0042 Baffles or guide plates
• CPC Class Codes: B01D 21/2427 The feed or discharge opening located at a distant position from the side walls
• CPC Class Codes: B01D 21/2438 provided with scrapers on the liquid surface for removing floating particles
• CPC Class Codes: B01D 21/2494 provided with means for the removal of gas, e.g. noxious gas, air
• CPC Class Codes: B01D 21/26 Separation of sediment aided by centrifugal force or centripetal forcecentrifuges B04B; cyclones B04C
• CPC Class Codes: B01D 2221/04 Separation devices for treating liquids from earth drilling, mining separation of well effluents E21B43/34, flotation in general B03D1/00
• CPC Class Codes: B01D 2251/90 Chelants
• CPC Class Codes: B01D 2251/902 EDTA
• CPC Class Codes: B01D 53/18 Absorbing units; Liquid distributors therefor B01D3/16, B01D3/26, B01D3/30 take precedence; packing elements B01J19/30, B01J19/32
• CPC Class Codes: B01D 53/52 Hydrogen sulfide
• CPC Class Codes: B01D 53/74 General processes for purification of waste gases; Apparatus or devices specially adapted therefor B01D53/92 takes precedence
• CPC Class Codes: B01D 53/78 with gas-liquid contact
• CPC Class Codes: B01F 23/2331 characterised by the introduction of the gas along the axis of the stirrer or along the stirrer elements
• CPC Class Codes: B01F 23/23341 with tubes surrounding the stirrer
• CPC Class Codes: B01F 23/23342 the stirrer being of the centrifugal type, e.g. with a surrounding stator
• CPC Class Codes: B01F 23/2368 Mixing receptacles, e.g. tanks, vessels or reactors, being completely closed, e.g. hermetically closed
• CPC Class Codes: B01F 27/1125 with vanes or blades extending parallel or oblique to the stirrer axis
• CPC Class Codes: B03D 1/02 Froth-flotation processes
• CPC Class Codes: B03D 1/04 by varying ambient atmospheric pressure
• CPC Class Codes: B03D 1/1462 Discharge mechanisms for the froth
• CPC Class Codes: B03D 1/1493 : with means for establishing a specified flow pattern
• CPC Class Codes: B03D 1/16 : with impellers; Subaeration machines mixing gases or vapours with liquids B01F23/20
• CPC Class Codes: C01B 17/0232 : Purification, e.g. degassing
• CPC Class Codes: C01B 17/05 : by wet processes
• CPC Class Codes: C01F 11/181 : Preparation of calcium carbonate by carbonation of aqueous solutions and characterised by control of the carbonation conditions
• CPC Class Codes: C02F 1/20 : by degassing, i.e. liberation of dissolved gases degasification of liquids in general B01D19/00; arrangement of degassing apparatus in boiler feed supply F22D
• CPC Class Codes: C02F 1/72 : by oxidation C02F1/4672 takes precedence
• CPC Class Codes: C02F 1/725 : by catalytic oxidation
• CPC Class Codes: C02F 1/76 : with halogens or compounds of halogens C02F1/4674 takes precedence
• CPC Class Codes: C02F 1/78 : with ozone C02F1/4672 takes precedence
• CPC Class Codes: C02F 3/205 : Moving, e.g. rotary, diffusers; Stationary diffusers with moving, e.g. rotary, distributors
• CPC Class Codes: Y02W 10/10 : Biological treatment of water, waste water, or sewage

Abstract

Hydrogen Sulfide is substantially completely removed from a gas stream in a two-stage operation. Hydrogen Sulfide is first partially oxidized to sulfur dioxide and the sulfur dioxide reacted with part of the remaining hydrogen sulfide while the hydrogen sulfide not so reacted is subsequently oxidized, thereby removing all of the hydrogen sulfide from the gas stream.

Claims

1. A process for the removal of hydrogen sulfide from a gas stream containing hydrogen sulfide, which comprises:

oxidizing a portion of the hydrogen sulfide therein to form sulfur dioxide therefrom and to produce an oxidized gas stream containing sulfur dioxide and a stoichiometric excess of hydrogen sulfide,

reacting substantially all said sulfur dioxide in said oxidized gas stream with hydrogen sulfide remaining in said oxidized gas stream in a first liquid phase to form sulfurous material therefrom contained in the first liquid phase and to produce a further gas stream having a decreased and residual hydrogen sulfide content,

oxidizing substantially all hydrogen sulfide remaining in said further gas stream in a second liquid phase to form a sulfurous material therefrom contained in the second liquid phase and to produce a gas stream substantially free from gaseous sulfur compounds, and

venting said gas stream substantially free from gaseous sulfur compounds.

2. A process for the removal of hydrogen sulfide from a gas stream containing hydrogen sulfide, which comprises:

(A) oxidizing a portion of the hydrogen sulfide therein to form sulfur dioxide therefrom and to produce an oxidized gas stream containing sulfur dioxide and a stoichiometric excess of hydrogen sulfide;

(B) reacting substantially all said sulfur dioxide in said oxidized gas stream in a first liquid phase in a first reaction vessel to form a sulfurous material therefrom contained in the liquid phase and to produce a further gas stream having a decreased hydrogen sulfide content by the steps of;

(a) feeding said oxidized gas stream to said first reaction vessel in which is located the first liquid phase,

(b) rotating a first impeller comprising a plurality of blades about a generally vertical axis at a submerged location in said first liquid phase so as to induce flow of said oxidized gas stream along a generally vertical flow path from external to said first reaction vessel to said submerged location,

(c) surrounding said first impeller with a first shroud through which are formed a first plurality of openings while said first impeller is rotated at a speed corresponding to a first blade tip velocity of at least about 350 in/sec so as to generate sufficient shear forces between said first impeller blades and said first plurality of openings in first said shroud to distribute said oxidized gas stream as gas bubbles in said first liquid phase to interior of said first shroud, and to effect intimate contact of said oxidized gas stream and first liquid medium at said submerged location so as to form a first gas-liquid mixture of gas bubbles in said first liquid phase contained within the shroud while effecting shearing of said first gas-liquid phase within said first shroud and to react substantially all of the sulfur dioxide with hydrogen sulfide in the oxidized gas stream, and

(d) flowing said first gas-liquid mixture from the first shroud through and in contact with the first plurality of openings therein into the body of the first liquid phase external to the first shroud at a first gas velocity index at approximately atmospheric pressure of at least about 18 per second per opening in the first shroud, so as to effect further shearing of the first gas-liquid mixture and further intimate contact of said oxidized gas stream and liquid phase whereby any oxidation of sulfur dioxide not effected in the interior of the first shroud is completed in the region of the first liquid phase adjacent to the exterior of the first shroud,

said first gas velocity index (GVI) being determined by the expression;

##EQU11## wherein Q is the volumetric flow rate of said oxidized gas stream (m³ /n), n is the number of openings in the first shroud, A is the area of an individual opening (m²) and P is the length of the perimeter of an individual opening, wherein said reaction of substantially all of said sulfur dioxide in said first reaction vessel is carried out at an Effective Shear Index (ESI) value of about 1 to about 2500, as determined by the ##EQU12## relationship;

where GVI is the first Gas Velocity Index (/s), V_i is the first blade tip velocity (m/s) for the blades of the first impeller, D_s is the inside diameter (m) of the first shroud, D_i is the outside diameter (m) of the first impeller, and at a Shear Effectiveness Index (SEI) value of about 1 to about 10, as determined by the relationship;

##EQU13## where Q is the gas flow rate of the oxidized gas stream to the first impeller (m³ /s), h is the height (m) of the first impeller blades, D_i is the outside diameter (m) of the first impeller and V_i is the first impeller blade tip velocity (m/s);

(C) venting said further gas stream having a decreased hydrogen sulfide content from a gas atmosphere above the liquid level in said first reaction vessel;

(D) oxidizing substantially all hydrogen sulfide remaining in said further gas stream in a second liquid phase in a second reaction vessel to form a sulfurous material therefrom by the steps of;

(e) feeding said further gas stream to said second reaction vessel in which is located said second liquid phase,

(f) rotating a second impeller comprising a plurality of blades about a generally vertical axis at a submerged location in said second liquid phase so as to induce flow of said further gas stream along a generally vertical flow path from external to said second reaction vessel to said submerged location,

(g) providing an oxygen-containing gas stream at said submerged location,

(h) surrounding said second impeller with a second shroud through which are formed a second plurality of openings while said second impeller is rotated at a speed corresponding to a second blade tip velocity of at least 350 in/sec. so as to generate sufficient shear forces between said second impeller blades and said second plurality of openings in said second shroud to distribute said further gas stream and said oxygen-containing gas as gas bubbles in said second liquid phase to the interior of said second shroud, and to effect intimate contact of said further gas stream, said oxygen-containing gas stream and second liquid phase at said submerged location so as to form a second gas-liquid mixture of gas bubbles in said second liquid phase contained within the shroud while effecting shearing of said second gas-liquid mixture within said second shroud and to effect oxidation of substantially all the hydrogen sulfide in said further gas stream, and

(i) flowing said second gas-liquid mixture from the second shroud through and in contact with the second plurality of openings therein into the body of the second liquid phase external to the second shroud at a second gas velocity index at approximately atmospheric pressure of at least 18 per second per opening in said second shroud, so as to effect further shearing of the second gas-liquid mixture and further intimate contact of said further gas stream, oxygen-containing gas stream and second liquid phase whereby any removal of hydrogen-sulfide from the gas stream not effected in the interior of the second shroud is completed in the region of the second liquid phase adjacent to the exterior of the second shroud,

said second gas velocity index (GVI) being determined by the expression;

##EQU14## where Q is the volumetric flow rate of said further gas stream (m³ /s), n is the number of openings in the second shroud, A is the area of the opening (m²) and P is the length of the perimeter of the opening (m),

wherein said reaction of substantially all said hydrogen sulfide in said further gas stream is carried out at an Effective Shear index (ESI) value of 1 to 2500, as determined by the relationship;

##EQU15## in which GVI is the second Gas Velocity Index (/s), V_i is the second blade tip velocity (m/s) for the blades of the second impeller, D_s is the inside diameter (m) of the second shroud and D_i is the outside diameter (m) of the second impeller, and at a Shear Effectiveness Index (SEI) value of 1 to 10, in which the Shear Effectiveness Index is determined by the relationship;

##EQU16## in which Q is the gas flow rate of the further gas stream to the second impeller (m³ /s), h is the height (m) of the second impeller blades, D_i is the outside diameter (m) of the second impeller, and V_i is the second impeller blade tip velocity (m/s); and

(E) venting a gas stream substantially free from gaseous sulfur compounds from said second reaction vessel.

3. The process of claim 2 wherein said liquid medium comprises liquid sulfur, tricresyl phosphate or an aqueous medium.

4. The process of claim 3 wherein said aqueous medium contains phosphoric acid.