IP Library Granted Patent US 9,669,355
Granted Patent B2
US 9,669,355 · App. 14/195,360 · Granted Jun 6, 2017

Activated carbon sorbent including nitrogen and methods of using the same

Inventors: Edwin S. Olson (Grand Forks, ND); John Henry Pavlish (East Grand Forks, MN)
Assignee: Energy & Environmental Research Center Foundation
B01D53/64B01D53/02B01J20/20B01J20/28004B01J20/324B01J20/3204B01J20/3208B01J20/3236B01J20/3293C01B31/083C01B31/10B01D53/025B01D53/04B01D53/10B01D53/8665B01D2253/102B01D2253/25B01D2253/304B01D2257/602B01D2258/0283
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Quick Facts
Patent No.
US 9,669,355
App. No.
14/195,360
Granted
Jun 6, 2017
Kind
B2
Abstract

The present invention relates to activated carbon sorbents including nitrogen. In various embodiments, the present invention provides an activated carbon sorbent including a halogen- or halide-promoted activated carbon, the activated carbon sorbent particles including nitrogen in a surface layer of the sorbent particles. In various embodiments, the present invention provides a method of reducing the pollutant content in a pollutant-containing gas using the activated carbon sorbent. In various embodiments, the activated carbon sorbent can remove mercury from a mercury-containing gas that includes sulfur(VI) such as SO 3 more efficiently than other sorbents.

Claims (31)

1. A method of reducing the mercury content in a pollutant-containing gas, the method comprising:

heating a carbon precursor comprising indole, quinoxaline, isoquinoline, piperazine, quinolone, diazabicyclo[2.2.2]octane (DABCO), polyvinylpyrrolidone, vinylpyrrolidone-vinyl acetate copolymer, vinylpyrrolidone-acrylic acid copolymer, vinylpyrrolidone-maleic acid copolymer, or a combination thereof, to about 200° C. to about 10,000° C., to provide an activated carbon sorbent comprising activated carbon sorbent particles comprising nitrogen in a surface layer of the sorbent particles;

contacting a mercury-containing gas with the activated carbon sorbent, to form a mercury-sorbent composition; and

separating at least some of the mercury-sorbent composition from the mercury-containing gas, to give a separated gas.

2. The method of claim 1 , wherein the mercury-containing gas further comprises a concentration of sulfur(VI) and the concentration of sulfur(VI) in the mercury-containing gas is greater than about 3 ppm by mole and the activated carbon sorbent forms a mercury-sorbent composition at a higher absorption rate relative to a corresponding activated carbon sorbent comprising at least one of a) less or substantially no nitrogen in a corresponding particle surface layer, b) less or substantially no halide- or halogen-promotion, wherein the activated carbon sorbent comprising the activated carbon sorbent particles is halide- or halogen-promoted, and c) less or substantially no inorganic matrix support, wherein the activated carbon sorbent comprising the activated carbon sorbent particles is inorganic matrix-supported.

3. The method of claim 1 , wherein the concentration of nitrogen in the surface layer of the sorbent particles is higher than the concentration of nitrogen in a core of the sorbent particles.

4. The method of claim 1 , wherein the mercury-containing gas further comprises a concentration of sulfur(VI) and the concentration of sulfur(VI) in the mercury-containing gas is about 3 ppm-2000 ppm.

5. The method of claim 1 , wherein the nitrogen in the surface layer at least one of decreases neutralization of carbocations in the activated carbon by at least one of SO 3 2 and HSO 3 1− , and at least partially blocks carbocations in the activated carbon from at least one of SO 3 2 and HSO 3 1− , as compared to a corresponding activated carbon sorbent comprising less or substantially no nitrogen in a corresponding particle surface layer.

6. The method of claim 1 , further comprising:

obtaining or providing an unpromoted carbon sorbent;

obtaining or providing a promoter; and

promoting at least a portion of the unpromoted sorbent by contacting the portion of the unpromoted sorbent with the promoter to form the activated carbon sorbent.

7. The method of claim 6 , wherein the promoter comprises a halogen or halide promoter.

8. The method of claim 1 , wherein the core of the activated carbon sorbent particles comprise about 0 wt %-about 99 wt % nitrogen.

9. The method of claim 1 , wherein the surface layer of the activated carbon sorbent particles comprises about 0.001 wt %-about 99 wt % nitrogen.

10. The method of claim 1 , wherein the surface layer of the activated carbon sorbent comprises a layer at the surface of the particle having a thickness of about 0.001% to about 99% of the radius of the particles.

11. The method of claim 1 , wherein the activated carbon sorbent particles have an average diameter of about 0.1 μm to about 1000 μm.

12. The method of claim 1 , wherein obtaining or providing the activated carbon sorbent comprises:

obtaining or providing a carbon precursor comprising nitrogen; and

processing the carbon precursor with at least one of heating, microwaving, and irradiating, to provide the activated carbon sorbent.

13. The method of claim 12 , wherein the carbon precursor comprises a carbonaceous material comprising carbon and a nitrogenous material comprising nitrogen.

14. The method of claim 12 , further comprising:

obtaining or providing a substrate material;

contacting the carbon precursor and the substrate material, to provide a sorbent starting material; and

processing the sorbent starting material with at least one of heating, microwaving, and irradiating, to provide the activated carbon sorbent.

15. The method of claim 14 , wherein the substrate comprises at least one of diatomaceous earth, a clay, a zeolite, or a mineral.

16. The method of claim 14 wherein the activated carbon sorbent comprises a carbon nanocomposite sorbent.

17. The method of claim 1 , wherein at least one of the contacting and the separating occurs in an aqueous scrubber.

18. A method of making an activated carbon sorbent, comprising:

contacting a carbonaceous material comprising brown sugar, barley sugar, caramel, cane sugar, corn syrup, starch, molasses, molasses raffinate, glucans, galactans, xylans, a sugar waste product, activated carbon, granular activated carbon, carbon black, carbon fiber, carbon honeycomb or plate structure, aerogel carbon film, or a combination thereof, and a nitrogenous material that is indole, quinoxaline, isoquinoline, piperazine, quinolone, diazabicyclo[2.2.2]octane (DABCO), polyacrylonitrile, polyvinylpyrrolidone, vinylpyrrolidone-vinyl acetate copolymer, vinylpyrrolidone-acrylic acid copolymer, vinylpyrrolidone-maleic acid copolymer, or a combination thereof, to provide a carbon precursor comprising nitrogen; and

heating the carbon precursor to about 200° C. to about 10,000° C. to form an activated carbon sorbent comprising activated carbon sorbent particles comprising nitrogen in a surface layer of the sorbent particles, wherein the concentration of nitrogen in the sorbent particles is higher than the concentration of nitrogen in the carbonaceous material.

Assignments (6)
CHANGE OF NAME Recorded Nov 7, 2024
From: MIDWEST ENERGY EMISSIONS CORP.
To: BIRCHTECH CORP.
Reel/Frame 069187/0413 →
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Jun 8, 2017
From: ENERGY AND ENVIRONMENTAL RESEARCH CENTER FOUNDATION
To: MIDWEST ENERGY EMISSIONS CORP.
Reel/Frame 042647/0351 →
CORRECTIVE ASSIGNMENT TO CORRECT THE RECEIVING PARTY'S ADDRESS PREVIOUSLY RECORDED ON REEL 033643 FRAME 0436. ASSIGNOR(S) HEREBY CONFIRMS THE ASSIGNMENT. Recorded Sep 9, 2014
From: OLSON, EDWIN S.
To: ENERGY AND ENVIRONMENTAL RESEARCH CENTER FOUNDATION
Reel/Frame 033698/0612 →
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Aug 29, 2014
From: PAVLISH, JOHN H.
To: ENERGY AND ENVIRONMENTAL RESEARCH CENTER FOUNDATION
Reel/Frame 033643/0339 →
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Aug 29, 2014
From: OLSON, EDWIN S.
To: ENERGY AND ENVIRONMENTAL RESEARCH CENTER FOUNDATION
Reel/Frame 033643/0436 →
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Jul 23, 2014
From: OLSON, EDWIN S.; PAVLISH, JOHN HENRY
To: ENERGY & ENVIRONMENTAL RESEARCH CENTER FOUNDATION
Reel/Frame 033377/0775 →
Continuity (2)
Provisional Application 61773549 · Mar 6, 2013
Related Publication 20140255279A1 · Sep 11, 2014