Separation of carbon dioxide (CO 2 ) from gas mixtures by calcium based reaction separation (CaRS-CO 2 ) process

• US 8,501,105 B2
• Filed: 07/20/2012
• Issued: 08/06/2013
• Est. Priority Date: 02/06/2003
• Status: Active Grant

• Current Assignee: Ohio State University
• Original Assignee: Ohio State University
• Inventors: Fan, Liang-Shih, Gupta, Himanshu, Iyer, Mahesh V.
• Primary Examiner(s): JOHNSON, EDWARD M
• Application Number:
  US13/555,054
• Publication Number:
  US 20130078159A1
• Time in Patent Office: 382 Days
• Field of Search: 422/177, 422/168
• US Class Current: 422/177
• CPC Class Codes: B01D 2251/404 of calcium
• CPC Class Codes: B01D 2253/10 Inorganic adsorbents
• CPC Class Codes: B01D 2257/504 Carbon dioxide
• CPC Class Codes: B01D 53/1475 Removing carbon dioxide
• CPC Class Codes: B01D 53/1493 Selection of liquid materials for use as absorbents
• CPC Class Codes: B01D 53/508 by treating the gases with solids
• CPC Class Codes: B01D 53/62 Carbon oxides
• CPC Class Codes: B01J 20/041 Oxides or hydroxides
• CPC Class Codes: B01J 20/06 comprising oxides or hydroxides of metals not provided for in group B01J20/04
• CPC Class Codes: B01J 20/28057 Surface area, e.g. B.E.T specific surface area
• CPC Class Codes: B01J 20/28071 being less than 0.5 ml/g
• CPC Class Codes: B01J 20/3085 Chemical treatments not covered by groups B01J20/3007 - B01J20/3078
• CPC Class Codes: B01J 20/3433 of sorbents or filter aids other than those covered by B01J20/3408 - B01J20/3425
• CPC Class Codes: B01J 20/3466 with steam
• CPC Class Codes: B01J 20/3483 by thermal treatment not covered by groups B01J20/3441 - B01J20/3475, e.g. by heating or cooling
• CPC Class Codes: B01J 8/06 in tube reactors; the solid particles being arranged in tubes
• CPC Class Codes: B82Y 30/00 Nanotechnology for materials or surface science, e.g. nanocomposites
• CPC Class Codes: C01F 11/06 of carbonates
• CPC Class Codes: C01P 2002/32 spinel-type (AB2O4)
• CPC Class Codes: C01P 2002/72 by d-values or two theta-values, e.g. as X-ray diagram
• CPC Class Codes: C01P 2006/12 : Surface area
• CPC Class Codes: C01P 2006/14 : Pore volume
• CPC Class Codes: C01P 2006/17 : Pore diameter distribution
• CPC Class Codes: C10J 2300/0996 : Calcium-containing inorganic materials, e.g. lime
• CPC Class Codes: C10J 2300/1807 : Recycle loops, e.g. gas, solids, heating medium, water
• CPC Class Codes: C10J 3/482 : Gasifiers with stationary fluidised bed
• CPC Class Codes: C10K 1/024 : by filtration
• CPC Class Codes: C10K 3/04 : reducing the carbon monoxide content , e.g. water-gas shift [WGS]
• CPC Class Codes: H01M 2008/1293 : Fuel cells with solid oxide electrolytes
• CPC Class Codes: H01M 8/0668 : Removal of carbon monoxide or carbon dioxide
• CPC Class Codes: Y02C 20/40 : of CO2
• CPC Class Codes: Y02E 60/50 : Fuel cells
• CPC Class Codes: Y02P 20/151 : Reduction of greenhouse gas [GHG] emissions, e.g. CO2

Abstract

A reaction-based process developed for the selective removal of CO2 from a multicomponent gas mixture to provide a gaseous stream depleted in CO2 compared to the inlet CO2 concentration. The proposed process effects the separation of CO2 from a mixture of gases by its reaction with metal oxides. The Calcium based Reaction Separation for CO2 (CaRS-CO2) process consists of contacting CO2 laden gas with CaO in a reactor such that CaO captures CO2 by the formation of CaCO3. CaCO3 is regenerated by calcination leading to the formation of fresh CaO sorbent and the evolution of a concentrated stream of CO2. The “regenerated” CaO is then recycled for the further capture of CO2. This carbonation-calcination cycle forms the basis of the CaRS-CO2 process. This process also may use a mesoporous CaCO3 structure that attains >90% conversion over multiple carbonation and calcination cycles.

Claims

1. A facility separating carbon dioxide and sulfur dioxide from a flow of gas comprising carbon dioxide and sulfur dioxide, comprising:

a gas-solid contact reactor receiving said flow of gas;

a sorbent within said gas-solid reactor, comprising a metal oxide, said sorbent reacting with said carbon dioxide and said sulfur dioxide so as to convert at least a portion of said sorbent to a metal carbonate and at least a portion of said sorbent to a metal sulfate; and

a calcinator, said calcinator receiving said at least a portion of said metal carbonate, said calcinatory calcining said metal carbonate to form said metal oxide and carbon dioxide,

wherein said sorbent is replenished in said gas-solid reactor with said metal oxide formed in said calcinatory.

2. The facility of claim 1, further comprising a cyclone, said cyclone separating said metal carbonate from said flow of gas.

3. The facility of claim 1, wherein said gas-solid reactor is operated at between about 600°

to about 650°

Celsius to facilitate the reaction between said carbon dioxide and said sulfur dioxide with said sorbent.

4. The facility of claim 1, further comprising an apparatus to sequester said carbon dioxide formed is said calcinatory.

5. The facility of claim 1, wherein said metal oxide is calcium oxide that has a surface area of less than 22 m²/g, a pore volume of at least 0.005 cm³/g, and a mesoporous pore size distribution.

6. The facility of claim 1, wherein said calcinator is under at least a partial vacuum when said metal carbonate is calcined.

7. The facility of claim 1, wherein steam is used to calcine said metal carbonate in said calcinator.

8. The facility of claim 1, wherein metal oxide is selected from the group consisting of:

ZnO, MgO, MnO₂, NiO, CuO, PbO, and CaO.

9. The facility of claim 1, wherein said sorbent has a sorption capacity of at least about 70 grams of carbon dioxide per kilogram of sorbent.

10. The facility of claim 1, wherein said sorbent has a sorption capacity of at least about 300 grams of carbon dioxide per kilogram of sorbent.

11. The facility of claim 1, wherein said sorbent has substantially the same sorption capacity after calcining as said sorbent had prior to absorbing said carbon dioxide.

12. The facility of claim 1, wherein said calcinator is operated at temperatures in the range of from about 800°

to about 850°

Celsius to calcine said metal carbonate.