WO2016190942A1 - Combustion de charbon propre - Google Patents

Combustion de charbon propre Download PDF

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Publication number
WO2016190942A1
WO2016190942A1 PCT/US2016/022107 US2016022107W WO2016190942A1 WO 2016190942 A1 WO2016190942 A1 WO 2016190942A1 US 2016022107 W US2016022107 W US 2016022107W WO 2016190942 A1 WO2016190942 A1 WO 2016190942A1
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WO
WIPO (PCT)
Prior art keywords
bed
flow
catalytic
stack
gas flow
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PCT/US2016/022107
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English (en)
Inventor
James Gary Davidson
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3 D Clean Coal Emissions Stack, Llc
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Publication date
Priority claimed from US14/722,244 external-priority patent/US9737849B2/en
Application filed by 3 D Clean Coal Emissions Stack, Llc filed Critical 3 D Clean Coal Emissions Stack, Llc
Priority claimed from US15/067,569 external-priority patent/US9919269B2/en
Publication of WO2016190942A1 publication Critical patent/WO2016190942A1/fr

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    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
    • B01D53/34—Chemical or biological purification of waste gases
    • B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
    • B01D53/86—Catalytic processes
    • B01D53/869—Multiple step processes
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
    • B01D53/34—Chemical or biological purification of waste gases
    • B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
    • B01D53/86—Catalytic processes
    • B01D53/8603—Removing sulfur compounds
    • B01D53/8609—Sulfur oxides
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
    • B01D53/34—Chemical or biological purification of waste gases
    • B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
    • B01D53/86—Catalytic processes
    • B01D53/8621—Removing nitrogen compounds
    • B01D53/8625—Nitrogen oxides
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
    • B01D53/34—Chemical or biological purification of waste gases
    • B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
    • B01D53/86—Catalytic processes
    • B01D53/864—Removing carbon monoxide or hydrocarbons
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2255/00—Catalysts
    • B01D2255/50—Zeolites
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2257/00—Components to be removed
    • B01D2257/20—Halogens or halogen compounds
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2257/00—Components to be removed
    • B01D2257/30—Sulfur compounds
    • B01D2257/302—Sulfur oxides
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2257/00—Components to be removed
    • B01D2257/40—Nitrogen compounds
    • B01D2257/404—Nitrogen oxides other than dinitrogen oxide
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2257/00—Components to be removed
    • B01D2257/50—Carbon oxides
    • B01D2257/502—Carbon monoxide
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2257/00—Components to be removed
    • B01D2257/50—Carbon oxides
    • B01D2257/504—Carbon dioxide
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2257/00—Components to be removed
    • B01D2257/60—Heavy metals or heavy metal compounds
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2258/00—Sources of waste gases
    • B01D2258/02—Other waste gases
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
    • B01D53/34—Chemical or biological purification of waste gases
    • B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
    • B01D53/86—Catalytic processes
    • B01D53/8659—Removing halogens or halogen compounds
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
    • B01D53/34—Chemical or biological purification of waste gases
    • B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
    • B01D53/86—Catalytic processes
    • B01D53/8665—Removing heavy metals or compounds thereof, e.g. mercury

Definitions

  • This invention relates to cleaning of stack gases such as those from coal fired power plants, from natural or propane burning heating plants, or from cement kilns.
  • stack gases such as those from coal fired power plants, from natural or propane burning heating plants, or from cement kilns.
  • the stack gases exhausted from such facilities are controlled by environmental regulations.
  • Such regulations require abatement of carbon monoxide (CO), carbon dioxide (CO 2 ) , nitrogen oxide (NOx), sulfur oxide (SOx) as well as halogens (such as chloride and fluorides) and trace metals, particularly mercury, lead, and zinc.
  • coal-fired stack gas Various methods and apparatuses have been proposed for abating these pollutants in stack gases.
  • a variety of methods have been proposed for reducing pollutants released from coal-fired stack gas.
  • One method of cleaning coal-fired stack gas is the use of scrubbers that inject a liquid or slurry into a gas stream that washes various pollutants, such as with acidic compounds, from the stack gas stream.
  • Another type of cleaning is the use of an exhaust burner that combusts volatile materials and other combustible compounds reducing pollution in the stack gas.
  • the stack gases be mixed with ammonia or urea and then passed through a catalyst in which the ammonia reacts selectively with the nitrous oxides to form nitrogen gas in water vapor, or combustion of a sulfur-containing fossil fuel in the presence of a calcium carbonate or magnesium carbonate to form calcium sulfate or magnesium sulfate.
  • a catalyst in which the ammonia reacts selectively with the nitrous oxides to form nitrogen gas in water vapor, or combustion of a sulfur-containing fossil fuel in the presence of a calcium carbonate or magnesium carbonate to form calcium sulfate or magnesium sulfate.
  • Catalytically converting unburned hydrocarbons and carbon monoxide to carbon dioxide and reducing nitrogen oxides to nitrogen subsequent to the combustion of fossil fuels, while absorbing sulfur oxide has been proposed, where the catalytic material is physically combined onto a dry powder of an adsorbent matrix selected from calcium aluminate, calcium aluminate cement, barium titanate, and calcium titanate. See U.S. Patent No. 4,483,259. It has also been proposed to pass the stack gases through a catalyst bed of a combination of active metals on the surface that is capable of reducing or converting sulfur oxides, carbon monoxide and hydrocarbons to inert compounds such as carbon dioxide, water and nitrogen. See U.S. Patent No. 7,399,458.
  • Levels of mercury in stack gases from coal combustion have also been reduced by introducing a sorbent composition into the gas stream in a zone where temperature is greater than 500 °C, where the sorbent composition comprises an effective amount of nitrate salt and/or a nitrite salt. See U.S. Patent Nos. 7,468,170 and 7,731,781.
  • an apparatus for drying and cleaning stack gases comprising: (a) a first catalytic flow-through bed of natural calcium zeolite with a porosity of a total surface area of not greater than 1200 m 2 /g adapted to reduce carbon oxides present in an exhaust stack; (b) a second catalytic flow-through bed of a blend of natural sodium zeolite and natural calcium zeolite of a porosity with a total surface area of not greater than 1200 m 2 /g adapted to reduce sulfur oxides present in the exhaust stack downstream of the first bed; (c) a third catalytic flow-through bed of natural calcium zeolite with a porosity of a total surface area not greater than 1200 m 2 /g adapted to reduce nitrogen oxides present in the exhaust stack downstream of the second bed; (d) a pair of electrodes adapted to be positioned inline in the gas flow upstream of the first catalytic flow-through bed and insulated from containment of the gas flow, such
  • an exhaust stack adapted to provide a gas flow, selected from the group consisting of volatiles from combustion of coal or from combustion of natural gas or from a cement kiln, sequentially past the pair of electrodes and through the first catalytic flow-through bed, the second catalytic flow-through bed, and the third catalytic flow-through bed, each catalytic bed collecting residuals, and providing stack gases exiting the third catalytic flow-through bed with at least 70% reduction in sulfur oxides, nitrogen oxides, and carbon oxides; and (e) the first catalytic flow-through bed, the second catalytic flow-through bed, and the third catalytic flow-through bed each adapted to be periodically purged with nitrogen to remove solids and/or liquids collected in the first catalytic flow-through bed, the second catalytic flow-through bed, and/or the third catalytic flow-through bed so
  • the electrodes may be positioned in the gas flow downstream of a baghouse.
  • the D.C. voltage applied between the electrodes may be less than 34 volts which may be effective to ionize the water vapor as previously described, but be sufficiently low to avoid the presence of hydrogen gas in substantial quantities downstream of the catalytic beds in the stack gas stream, as described.
  • the electrodes in the gas flow upstream of the first catalytic flow-through bed insulated from containment of the gas flow may apply such voltage to ionize water vapor in the gas flow and reduce moisture content of the gas flow in the first catalytic flow-through bed to be below 8% or 5% or a lower or different moisture content as desired.
  • the exhaust stack may be adapted to exit gases from the third catalytic flow- through bed with at least 80% or 90% reduction in carbon oxides, sulfur oxides, and nitrogen oxides compared to the stack gases after reaching the electrodes.
  • the apparatus in addition may have a venturi positioned in the gas flow downstream of the third catalytic flow- through bed to stabilize gas flow through the beds.
  • the apparatus may also include stabilizing veins to improve laminar flow of the stack gases through the beds. Stabilizing veins may improve efficiency of separation of pollutants from the stack gases. Stabilizing veins may be positioned upstream or downstream of the electrodes in the gas stream, but may be more advantageously positioned downstream of the electrodes.
  • the blend of natural sodium zeolite and natural calcium zeolite in the second catalytic flow-through bed may be between 25% and 75%.
  • the first catalytic flow-through bed, the second catalytic flow-through bed, and the third catalytic flow-through bed may also each have a porosity of total surface area not greater than 800 m 2 /g.
  • a fourth catalytic flow-through bed of calcium zeolite may also be provided in the gas flow after passing the pair of electrodes and before the first catalytic flow-through bed with a porosity of total surface area not greater than 1200 m 2 /g, or not greater than 800 m 2 /g, adapted to collect bauxite compounds before passage through the first catalytic flow-through bed.
  • the fourth catalytic flow-through bed also may be adapted to be periodically purged with nitrogen.
  • exhaust stack gases may exit from the third catalytic flow-through bed with at least 70% or 90% reduction in bauxite compounds, carbon oxides, sulfur oxides, nitrogen oxides, and mercury oxides compared to the stack gases delivered through the pair of electrodes.
  • the apparatus may comprise at least two series of sequential gas flows both through a pair of electrodes, a first catalytic flow-through bed, a second catalytic flow- through bed, and a third catalytic flow-through bed, provided in parallel, so stack gases can be cleaned through one of the series of beds while other series of beds can be purged.
  • Also disclosed is a method of drying and cleaning stack gases comprising the steps of:
  • the voltage between the electrodes may be below 34 volts, and the gas flow sequentially circulated past the pair of electrodes and through the first catalytic flow-through bed, the second catalytic flow-through bed, and the third catalytic flow-through bed also may remove from the gas flow at least 50% or 70% of mercury in all forms.
  • the pair of electrodes in step (a) may also be positioned in the gas flow downstream of a baghouse.
  • the method of drying and cleaning stack gas may also have the pair of electrodes in the gas flow upstream of the first catalytic flow-through bed insulated from containment of the gas flow with D.C.
  • a method of drying and cleaning stack gases comprising the steps of:
  • a first catalytic flow-through bed comprised of calcium zeolite of natural zeolite particles of a majority between 44 ⁇ and 64 ⁇ in size at a temperature above the dew point between 125 °F and 500 °F and a pressure between 3 psi and 200 psi adapted to reduce carbon oxides in the stack gases;
  • the voltages between the electrodes may be less than 34 volts, and the stack gas may have the flow sequentially circulated past the same or a different pair of electrodes and through the series of a first catalytic flow-through bed, a second catalytic flow-through bed, and a third catalytic flow-through bed.
  • the method also may remove from the gas flow at least 50% of mercury or at least 70% of mercury in all forms.
  • the electrodes in step (a) of the alternative method of cleaning and drying may be positioned in the gas flow downstream of a baghouse.
  • the alternative method of drying and cleaning stack gas may also have the additional step of passing the gas flow through a venturi positioned downstream of the third catalytic flow-through bed to stabilize the gas flow through the beds.
  • the alternative method of drying and cleaning stack gas may also comprise a fourth catalytic flow-through bed of calcium zeolite comprising natural zeolite particles between 44 ⁇ and 64 ⁇ in size positioned in the stack gas flow after the pair of electrodes and before the first catalytic bed with an electrical charge on said fourth catalytic flow- through bed to separately collect bauxite compounds from the stack gas flow before passing through the first catalytic bed.
  • the stack gas exiting a stack from the third catalytic bed may have at least 70% or 90% reduction in bauxite compounds, carbon oxides, sulfur oxides, nitrogen oxides, and mercury oxide compared to the stack gas flow delivered through the stack.
  • the alternative method of drying and cleaning stack gas may have the pair of electrodes positioned in the gas flow upstream of the first catalytic flow-through bed insulated from containment of the gas flow with applied direct voltage to ionize water vapor without creating substantial amounts of hydrogen gas in the gas flow and reduce moisture content of the gas flow through the catalytic flow-through beds to below, for example, 8% or 5% or a lower or different moisture content as desired.
  • the alternative method of drying and cleaning stack gas may comprise the additional step of passing the gas flow through a venturi positioned downstream of the third catalytic flow-through bed to stabilize the gas flow through the beds.
  • the alternative method of drying and cleaning stack gas may have at least two series of stack gas flows are provided in parallel to provide for the gas flow to passed a pair of electrodes inline and through a first catalytic bed, a second catalytic bed, and a third catalytic bed to enable at least one bed in series of beds can be purged while the stack gas flow continues to be dried and cleaned through a series of beds and optionally another pair of electrodes.
  • a second alternative method of drying and cleaning stack gases comprising the steps of:
  • the electrodes in step (a) may be positioned in the gas flow downstream of a baghouse and the voltage between the electrodes may be less than 34 volts.
  • the second alternative method of drying and cleaning stack gas may have the pair of electrodes in the gas flow upstream of the first catalytic flow-through bed insulated from containment of the gas flow with an applied voltage to the electrodes to ionize water vapor in the gas flow and reduce moisture content of the gas flow in the first catalytic flow-through bed.
  • the second alternative method of drying and cleaning stack gas may have the stack gas flow sequentially circulated past the pair of electrodes and through the first catalytic flow-through bed, the second catalytic flow-through bed, and the third catalytic flow-through bed also removes from the gas flow at least 50% or at least 70% of mercury in all forms.
  • the second alternative method of drying and cleaning stack gas may comprise the additional step of passing the gas flow through a venturi positioned downstream of the third catalytic flow-through bed to stabilize the gas flow through the beds.
  • the second alternative method of drying and cleaning stack gas may comprise in addition a fourth catalytic flow-through bed of calcium zeolite comprising natural zeolite particles between 44 ⁇ and 64 ⁇ in size positioned in the stack gas flow after the pair of electrodes and before the first catalytic bed with an electrical charge on said fourth catalytic flow-through bed to separately collect bauxite compounds from the stack gas flow before passing through the first catalytic bed.
  • this alternative method of drying and cleaning stack gas may have the stack gas exiting a stack from the third catalytic bed may have at least 70% or at least 90% reduction in bauxite compounds, carbon oxides, sulfur oxides, nitrogen oxides, and mercury oxide compared to the stack gas flow delivered through the stack.
  • the second alternative method of drying and cleaning stack gas may have at least two series of stack gas flows provided in parallel to pass the same or a different pair of electrodes inline to dry the stack gas by applying a voltage between the electrodes to ionize the water vapor without creating substantial amounts of hydrogen gas and through a series of a first catalytic bed, a second catalytic bed, and a third catalytic bed so that one stack gas flow can be dried and cleaned by the method described, while an alternative series of a first catalytic bed, a second catalytic bed, and a third catalytic bed may be purged for reuse.
  • a third alternative method of drying and cleaning stack gases comprising the steps of:
  • the electrodes in step (a) of this third alternative method may be positioned in the gas flow downstream of a baghouse.
  • This third alternative method of drying and cleaning stack gas may also provide the pair of electrodes in the gas flow upstream of the first catalytic flow-through bed and insulated from containment of the gas flow, and may apply D.C. voltage less than 34 volts to ionize water vapor in the gas flow and reduce moisture content of the gas flow in the first catalytic flow-through bed, preferably to below 8% or 5% or a lower or different moisture content as desired.
  • the first catalytic flow-through bed, the second catalytic flow-through bed, and the third catalytic flow-through bed may include other sizes of particles of zeolite as explained in more detail below.
  • an additional fourth catalytic flow-through bed of calcium zeolite comprising natural zeolite particles with a porosity of a total surface area not greater than 1200 m 2 /g may be positioned in the stack gas flow after the pair of electrodes and before the first catalytic bed with an electrical charge to separately collect bauxite compounds from the stack gas flow before passing through the first catalytic bed.
  • This method of drying and cleaning stack gas may have the stack gas exiting a stack from the third catalytic bed with at least 70% or at least 90% reduction in bauxite compounds, carbon oxides, sulfur oxides, nitrogen oxides, and mercury oxide compared to the stack gas flow delivered to the stack.
  • This third alternative method of drying and cleaning stack may have at least two series of stack gas flows provided in parallel to pass the same or a different pair of electrodes positioned inline to ionize the water vapor in the stack gas without creating substantial amounts of hydrogen gas and through a first catalytic bed, a second catalytic bed, and a third catalytic bed so that one bed of stack gas flow can be dried and cleaned by the method described while another series of stack gas flow-through flow is purged.
  • This third alternative method of drying and cleaning stack gas may also comprise a fourth catalytic flow-through bed comprised of calcium zeolite of natural zeolite particles between 44 ⁇ and 64 ⁇ in size positioned in the stack gas flow after the pair of electrodes and before the first catalytic bed, with an electrical charge on said fourth catalytic flow-through bed, to separately collect bauxite compounds from the stack gas flow before passing through the first catalytic bed.
  • the stack gas exiting a stack from the third catalytic bed may have at least 70% or at least 90% reduction in bauxite compounds, sulfur oxides, nitrogen oxides, mercury oxide, and carbon oxides compared to the stack gas flow delivered through the stack.
  • the method and alternative methods of drying and cleaning stack gas may comprise the additional step of passing the gas flow through a venturi positioned downstream of the third catalytic flow-through bed to stabilize the gas flow through the catalytic flow- through beds.
  • the method and alternative methods of drying and cleaning stack gas may have the stack gas flow sequentially circulated past the pair of electrodes and through the first catalytic flow-through bed, the second catalytic flow-through bed, and the third catalytic flow-through bed to also remove at least 50% or at least 70% of mercury in all forms from the gas flow.
  • fertilizer product produced by the steps of:
  • fertilizer product produced by the steps of:
  • Also disclosed is a method of reducing moisture content in a gas flow comprising the steps of:
  • carbon monoxide (CO), carbon dioxide (CO 2 ), nitrogen oxide ( ⁇ ), sulfur dioxide (SO 2 ) and nitrogen dioxide (N0 2 ) in the gas stack flow may be reduced.
  • the solid waste may also include nitrate salt formed by reaction of nitrogen and nitrogen compounds retained in the zeolite beds with available oxygen. Exit from the third catalytic bed may typically include excess oxygen from the reduction according in the first, second and third catalytic flow- through beds as described above.
  • the apparatus may also include a product purged with liquid nitrogen.
  • the exiting stack gas with increased oxygen levels may be returned from the gas cleaning system to the burner where it is combusted with the coal or natural gas.
  • the system may also include a solid waste draw for collecting the materials and drawing the waste material away from the gas cleaning section.
  • FIG. 1 is a schematic illustrating a coal-fired boiler for electric power generation using stack gases that are cleaned and solid/liquid products recovered in accordance with the present invention
  • FIGS. 2 A, 2B, and 2C fragment parts of the piping for the stack gas cleaning and recovery system shown in FIG. 1 upstream of the portion shown in FIG. 3 A or FIG. 3B;
  • FIG. 3A is an enlarged portion of part of the stack gas cleaning and recovery system shown in FIG. 1 in which three catalytic flow beds are utilized;
  • FIG. 3B is an enlarged portion of part of the stack gas cleaning and recovery shown in FIG. 1 in which four catalytic beds are utilized;
  • FIG. 4 is a cross-section taken along line 3-3 of FIG. 3A or FIG. 3B;
  • FIG. 5 is a schematic illustrating a test facility designed to test the cleaning of stack gases and recovery of solids and liquids in accordance with the invention
  • FIG. 6 is an enlarged portion of the test facility shown in FIG. 5;
  • FIG. 7 is an illustration corresponding to FIG. 6 in top view showing the movement of catalytic flow through three catalytic beds of FIG. 6;
  • FIG. 8 is an alternative to a test facility corresponding to FIG. 5 where four catalytic flow beds are provided;
  • FIG. 8A is a graph illustrating CO 2 levels before and after cleaning
  • FIG. 8B is a graph illustrating SO 2 levels before and after cleaning.
  • FIG. 8C is a graph illustrating NO levels before and after cleaning.
  • FIG. 1 is a schematic illustrating a coal-fired boiler for electric power generation producing stack gases that are cleaned and solid/liquid products recovered.
  • a coal fired boiler 10 is shown utilizing the stack gas cleaning and recovery apparatus and method of the present invention.
  • Fresh air intake 12 flows through preheater 14 to supply preheated fresh air to the boiler 10 that is coal fired.
  • the stack gases 16 from boiler 10 pass through preheater 14 whereby heat is transferred to the fresh air intake 12.
  • the stack gases 16, now processed by preheater 14, are conveyed to an emission control unit where the stack gases 16 are circulated to emission control system 18 through inlet 20 and allowed to rise through the emission control system 18 and up through gas cleaning apparatus 22.
  • the stack gases 16 at this point typically include carbon monoxide, carbon dioxide, sulfur oxides and nitrogen oxides.
  • the stack gases 16 also include water vapor and particulates such as aluminum oxides, mercury compounds and other particulate matters such as uranium and rare earth metals as well as halogens such as fluoride and chloride.
  • FIGS 2A, 2B and 2C is shown a part of the piping 21 for the stack gas cleaning apparatus 22 shown in FIG. 1 upstream of the portion shown in FIG. 3 A or FIG. 3B as described further below.
  • a pair of electrodes 23 A and 23B are placed in line piping 21 in the stack gas 16 and are of dimensions that extend into piping 22 A sufficient to efficiently ionize the stack gas 16 flowing past the electrodes 23 A and 23B.
  • Electrodes 23 A and 23B are insulated at 21A from piping 21 to efficiently provide for ionization of stack gas 16.
  • Electrodes 23A and 23B are applied between the electrodes 23A and 23B sufficient to form the various ions of 3 ⁇ 40 such as HO+, 3 ⁇ 40+, H+, 0+ and O2+, while avoiding formation of substantial amounts of 3 ⁇ 4 + which is produced at higher voltages (e.g., about 34 volts). See “The Ionization of Water Vapor by Electron Impact” Physical Review Vol 43, 116 et seq. (January 1933) The voltage may vary with varying sizes of piping 21 and varying flow rates of stack gas 16. For increases in efficiency of ionization, electrodes 23 A and 23B can be increased in size to provide for greater surface area and more than one pair of electrodes in the stack gas flow can be employed.
  • the desire is to provide sufficient ionization to reduce the moisture content of the stack gas 16 flowing through the catalytic flow-through beds 24, 26 and 28, or the catalytic flow-through beds 30, 24, 26 and 28, to below, for example, 8%, or 5% or 3%, as desired to provide for efficient operation of the catalytic flow-through beds in cleaning the stack gas 16 as described below.
  • gas cleaning apparatus 22 further comprises first catalytic flow-through bed 24, second catalytic bed 26 and third catalytic flow-through bed 28 as shown in FIG. 3A, or through fourth catalytic flow-through bed 30, first catalytic flow-through bed 24, second catalytic flow-through bed 26, and third catalytic flow-through bed 28 as shown in FIG. 3B.
  • the rising stack gases 16 in cleaning apparatus 22 first flow through the first catalytic flow-through bed 24, followed by the adjacent second catalytic flow-through bed 26, and then followed by the third catalytic flow-through bed 28.
  • fourth catalytic flow-through bed 30 is utilized as shown in FIG. 3B, fourth catalytic flow-through bed 30 in stack 32 in gas stack 16 may be positioned after the pair of electrodes 23A and 23B and before the first catalytic flow-through bed 24.
  • First catalytic flow through bed 24 is comprised of calcium zeolite of natural zeolite particles with a majority between 44 ⁇ and 64 ⁇ in size.
  • "Majority" in the particle size range means here, as well as throughout this application, that it necessarily is 50% or more of the particle sizes in the particle size increment of zeolite to efficiently achieve reduction of carbon oxides in the stack gas.
  • the calcium zeolite is a calcium-sodium- potassium aluminosilicate that is relative high calcium oxide that is available from a natural source.
  • Typical chemical analyses of such calcium zeolite are (i) 2.85% calcium oxide (CaO), 2.85% potassium oxide (K 2 0), 0.98% manganese oxide (MgO), 0.06% manganese oxide (MnO), 0.19% titanium dioxide (Ti0 2 ), 0.05% potassium oxide (P 2 0 5 ), 0.03% sodium oxide (Na 2 0), 11.43% aluminum oxide (A1 2 0 3 ), 1.26% ferric oxide (Fe 2 0 3 ) 66.35% silicon dioxide (S1O 2 ) and 13.28% LOI; and (ii) 3.4% calcium oxide (CaO), 3.0% potassium oxide (K 2 O), 1.5% manganese oxide (MgO), 0.05% potassium oxide (P 2 O 5 ), 0.3% sodium oxide (Na 2 0), 12.1% aluminum oxide (A1 2 0 3 ), 1.6% ferric oxide (Fe 2 0 3 ), 70.0% silicon dioxide (Si0 2 ).
  • a source for calcium zeolite is St. Cloud Mining Company mines at Winston and Truth or Consequences, New Mexico 87901, or a similar mine available in other parts of the world. "Natural zeolite” means here, and elsewhere in this description, zeolite that is mined as opposed to artificially created.
  • First catalytic flow- through bed 24 is provided as a flow-through bed held in position by lower screen 34 and upper screen 36 each of between 150 and 250 mesh designed to hold the bed of calcium zeolite in position while allowing flow through of the stack gases 16.
  • first catalytic flow-through bed 24 The primary function of first catalytic flow-through bed 24 is splitting carbon monoxide and carbon dioxide, and retaining carbon in various forms and compounds in the zeolite bed. First catalytic flow-through bed 24 also captures ash and other particular matter not previously captured, as well as bauxite compound if the fourth catalytic flow-through bed 30 is not provided as shown in FIG. 3A.
  • Second catalytic flow-through bed 26 is comprised of a blend between 25% and 75% of sodium zeolite and calcium zeolite with a majority being natural sodium and calcium zeolite particles between 65 ⁇ and 125 ⁇ in size available from a natural source.
  • the source of the calcium zeolite can be the same as that used to provide first catalytic flow-through bed 24, but comprised of a majority of a particle size between 65 ⁇ and 125 ⁇ .
  • the sodium zeolite may be natural sodium-potassium clinoptilolite that is relatively high in sodium oxide content.
  • Typical chemical analyses of such sodium zeolite are (i) 3.5% sodium oxide (Na 2 0), 3.8% potassium oxide (K 2 O), 11.9% aluminum oxide (AI 2 O 3 ), 0.7% ferric oxide (Fe 2 0 3 ), 0.8% calcium oxide (CaO), 0.4% manganese oxide (MgO), 0.02% manganese oxide (MnO), 0.1% titanium oxide (T1O 2 ) and 69.1% silicon dioxide (S1O 2 ); and (ii) 3.03% sodium oxide (Na 2 0), 3.59% potassium oxide (K 2 0), 10.27% aluminum oxide (A1 2 0 3 ), 0.86% ferric oxide (Fe 2 0 3 ), 1.77% calcium oxide (CaO), 0.00% potassium oxide (K 2 O), 0.4% manganese oxide (MgO), 0.02% manganese oxide (MnO), 0.11% titanium oxide (Ti0 2 ), 69.1% silicon dioxide (S1O 2 ), and 13.09% LOI.
  • a source of the sodium zeolite, amongst others, is the St. Cloud mines in Ash Meadows, Nevada, or a similar zeolite mine in another part of the world. Again, the size and depth of the second set of the flow-through bed is determined by the physical dimensions of the stack 32 and the flow rate and pressure drop through the stack 32 at the gas cleaning apparatus 22.
  • the primary purpose of the second catalytic flow-through bed 26 is to capture and split sulfur oxides (SOx) in the stack gas 16.
  • the second catalytic flow-through bed 26 is also effective in reducing metal compounds such as mercury, lead, uranium and other trace materials.
  • a lower screen 38 and an upper screen 40 may be provided with mesh sizes between 150 and 250 mesh to maintain the second catalytic flow-through bed 28 while allowing appropriate flow through of stack gas 16.
  • the stack gases 16 flow downstream through third catalytic flow-through bed 28.
  • the third catalytic flow-through bed is comprised of calcium zeolite similar in chemical analysis to the first catalytic flow- through bed 24 but with a majority of natural zeolite in the particle size for this bed between 78 ⁇ and 204 ⁇ .
  • the third catalytic flow-through bed 28 is provided primarily to split nitrogen oxides present in the stack gas 16.
  • the third catalytic flow-through bed may also reduce other pollutant compounds and ash in the stack gas 16.
  • the composition of natural calcium zeolite in third catalytic flow-through bed 28 may be comprised of the same composition as the first catalytic flow through bed 24, but with different zeolite particle sizes, as described herein, for efficient reduction of nitrogen oxides.
  • a lower screen 42 and an upper screen 44 with mesh size between 150 and 250 mesh is provided to maintain the third catalytic flow through bed 28.
  • FIG. 3A is a method of cleaning stack gases after the stack gas flow passes the pair of electrodes 23A and 23B comprising the steps of:
  • a second catalytic flow-through bed 26 comprised of a blend between 25 and 75% of natural sodium zeolite and natural calcium zeolite of zeolite particles with a majority zeolite between 65 ⁇ and 125 ⁇ in size, at a temperature above the dew point between 125 °F and 500 °F and a pressure between 3 psi and 200 psi, adapted to reduce sulfur oxides from the stack gases;
  • stack gases selected from the group consisting of volatiles from combustion of coal or from combustion of natural gas or from a cement kiln, sequentially past the electrodes and through the first flow-through catalytic bed 24, the second flow-through catalytic bed 26, and the third flow-through catalytic bed 28, each flow-through catalytic bed collecting residuals in the catalytic beds and providing gas exiting the third catalytic bed with at least 70% reduction in carbon oxides, sulfur oxides, and nitrogen oxides.
  • the method may also sequentially circulate the stack gas flow past the same or a different pair of electrodes and through the first flow-through catalytic bed 24, the second flow-through catalytic bed 26, and the third flow-through catalytic bed 28 to remove from the stack gas at least 50% or 70% of mercury in all forms, namely, elemental and oxidized forms.
  • FIG. 3A Alternatively disclosed in FIG. 3A is a method of drying and cleaning stack gases comprising the steps of:
  • a second catalytic flow-through bed 26 comprised of a blend between 25 and 75% of sodium zeolite and calcium zeolite of natural zeolite particles at a temperature above the dew point between 125 °F and 500 °F and a pressure between 3 psi and 200 psi adapted to reduce sulfur oxides from the stack gas and increase oxygen levels in the stack gases;
  • the nitrogen from the stack gas is in large part retained in the zeolite beds, and is available for reaction with available oxygen present particularly during purging as described below.
  • a fourth catalytic flow through bed 30 is provided as shown in FIG. 3B
  • the fourth catalytic flow-through bed is provided in the stack gas 16 after passing the pair of electrodes and before the first catalytic flow-through bed 24.
  • the gas stream 16 may flow through the fourth catalytic-flow-through bed 30 before flowing into the first catalytic flow- through bed 24.
  • the composition of the fourth catalytic flow-through bed 30 is comprised of the same composition as the first catalytic flow-through bed, namely, comprised of calcium zeolite, but with a majority of the natural zeolite being particles between 44 ⁇ and 64 ⁇ in size.
  • the fourth catalytic flow-through bed is maintained in position by lower screen 46 and upper screen 48 with a mesh size between 150 and 250 mesh while allowing flow of stack gas 16 though the bed.
  • An electrical charge is also provided on the lower screen 46 to provide that the fourth catalytic flow-through bed 30 attracts and retains bauxite particles from stack gas 16.
  • the fourth catalytic flow- through bed 30 comprised of calcium zeolite of natural zeolite particles between 44 ⁇ and 64 ⁇ in size positioned in the stack before the first catalytic bed 24 with an electrical charge beneath said fourth catalytic flow- through bed 30 to efficiently collect bauxite compounds from the stack gases before passing through the first catalytic bed.
  • the fourth catalytic flow-through catalytic bed 30 is provided as shown in FIG. 3B, aluminum oxide may be largely separately collected and separately processed to be recovered, as explained further herein.
  • the stack gas 16 flowing through gas cleaning apparatus 22 is separately cleaned of bauxite compounds as well as cleaned as described above of carbon dioxide, carbon monoxide, nitrogen oxides, sulfur oxides as well as mercury oxides, water vapor and other trace metals in the stack gas 16.
  • the cleaning of the stack gases 16 flowing through first catalytic flow-through bed 24, second catalytic flow-through bed 26, third catalytic flow-through bed 28, and if present also fourth catalytic flow-through bed 30, provides at least 90%, 95%, or even 99% reduction in bauxite compounds, carbon oxides, sulfur oxides, nitrogen oxides, and mercury oxides from the stack gases 16.
  • a method of drying and cleaning stack gases may involve putting all of the zeolite beds in to all three or four of the catalytic flow-through beds. Therefore the method may comprising the steps of:
  • a catalytic flow- through bed comprised of a mixture of calcium zeolite of natural zeolite particles of a majority between 44 ⁇ and 64 ⁇ in size, a blend between 25 and 75% of sodium zeolite and calcium zeolite of natural sodium and calcium zeolite particles of a majority between 65 ⁇ and 125 ⁇ in size, and calcium zeolite of natural zeolite particles of a majority between 78 ⁇ and 204 ⁇ at a temperature above the dew point between 125 °F and 500 °F and a pressure between 3 psi and 200 psi adapted to reduce carbon oxides in the stack gas flow, the mixture having a porosity of a total surface area not greater than 1200 m 2 /g; and
  • the size of the pair of electrodes may be varied to provide the surface area to the desired moisture content in the stack gas flow, depending on the desired moisture content desired in the stack gas, for processing to reduce the levels of carbon oxides, sulfur oxides and nitrogen oxides, and the flow through volume of stack gas to be processed.
  • Figures 8A-8C represent data taken from a combustion gas emissions test where charcoal and 3g of organic sulfur were combusted in a combustion oven.
  • data was collected from the lower flue stack before the stack gas 16 passed through the stack gas cleaning apparatus 22.
  • data was collected from the upper flue stack after the stack gas 16 passed through the gas cleaning apparatus. Data was collected every 5 seconds using a Testo 350XL portable combustion multi-gas analyzer. Data for the first test run (lower flue stack) was compared to and plotted with data for the second test run (upper flue stack) to provide an analysis of the results of the gas cleaning apparatus 22.
  • FIG. 8A illustrates measured levels of carbon dioxide (CO 2 ) (ppm) before
  • FIG. 8B illustrates measured levels of sulfur dioxide (SO 2 ) (ppm) before (solid line) and after (dashed line) the stack gas 16 is cleaned by the cleaning apparatus 22.
  • FIG. 8C illustrates measured levels of nitrous oxide (NO) (ppm) before (solid line) and after (dashed line) the stack gas 16 is cleaned by the cleaning apparatus 22.
  • NO nitrous oxide
  • the cleaning apparatus While the cleaning apparatus is in operation 22, residuals including carbon, sulfur, nitrogen, and other products are collected by the catalytic through-flow beds.
  • the first catalytic through-flow bed 24, second catalytic through-flow bed 26, third catalytic through-flow bed 28 and fourth catalytic through-flow bed 30 may be switched between parallel systems as shown in FIGS. 3 and 4.
  • the stack gases 16 may thus continue to flow through stack 32 and be cleaned in stack cleaning apparatus 22 while the parallel first catalytic through-flow bed 24, second catalytic through-flow bed 26, third catalytic through-flow bed 28 and fourth catalytic through-flow bed 30 (where present) are taken off-line and purged with nitrogen to remove material from the catalytic beds.
  • This purging of the beds may be done with cryogenic nitrogen or nitrogen gas, generally available as a purge fluid.
  • purge fluid including nitrogen is released from a reservoir 54 and the purge fluid passes through one or more beds of the first catalytic through-flow bed 24, second catalytic through-flow bed 26, third catalytic through-flow bed 28 and/or fourth catalytic through-flow bed 30 (where present).
  • the purge fluid may be pressurized or may fall by gravity through one or more of the catalytic through- flow beds, releasing material from the catalytic through-flow beds.
  • This purging produces residual waste largely of fertilizer composition that is discharged through outlet 50 into a container 52.
  • the fertilizer compounds can be formed by reaction of the nitrogen and nitrogen compounds with the residuals retained by the zeolite beds with the oxygen present during purging.
  • the mechanism of formation of these fertilizer materials may involve catalytic splitting of the carbon oxide, sulfur oxide and nitrogen oxide compounds present in the stack gas stream and retained by the zeolite beds, which are then available to react with free oxygen atoms and/or oxygen ions in purging with nitrogen. Because large amounts of nitrogen are present in the stack gas stream, relatively large amounts of nitrate compounds may be present in the fertilizers produced. In any case, these fertilizer compositions provide a valuable byproduct of the present process.
  • a fourth catalytic through-flow bed 30 may be separately purged through a separate outlet into a separate container (not shown) to allow for recovery of bauxite compounds as a separate product.
  • the bauxite compounds are collected in the catalytic through-flow beds and provided as a part of a fertilizer composition.
  • the metals such as mercury, zinc, lead and other trace metals are also collected known to be beneficial to compositions for soil collected as part of the fertilizer product that is recovered.
  • the purging may also produce gases, such as oxygen (O 2 ) and nitrogen (N 2 ) that may be extracted by a first gas outlet 58 that transports a portion of the gases (e.g. N 2 ) to a recycler and a second gas outlet 60 that transports a portion of the gases (e.g. O 2 ) to the burner for combusting the fuel, providing steam to drive the turbines in the power plant.
  • gases such as oxygen (O 2 ) and nitrogen (N 2 ) that may be extracted by a first gas outlet 58 that transports a portion of the gases (e.g. N 2 ) to a recycler and a second gas outlet 60 that transports a portion of the gases (e.g. O 2 ) to the burner for combusting the fuel, providing steam to drive the turbines in the power plant.
  • FIGS. 5-6 A test apparatus is illustrated in FIGS. 5-6.
  • the testing apparatus includes a stack 32 for transporting stack gas 16 to the gas cleaning apparatus 22 described above.
  • the gas cleaning apparatus 22 is shown in further detail in FIG. 6 and includes first 24, second 26 and third 28 catalytic flow-through- beds each comprising a zeolite composition as described above.
  • Each of the catalytic flow-through beds may be connected to a central drive shaft 58 that is adapted to rotate or otherwise move each of the catalytic flow-through beds, individually, from a first position where stack gas 16 passes through the bed to a second position where the catalytic flow-through bed is purged by the purge fluid.
  • a handle 60 is provided that may be translated vertically to select one of the catalytic flow-through beds and rotated or otherwise move the selected flow-through bed from the first position to the second position.
  • FIG. 7 is a top view of the cleaning apparatus 22 according to the testing apparatus shown in FIGS. 5-6. In this view, the compositions and particle size of catalytic through- flow beds are adjusted with the composition of the coal stack 32.
  • the tests with the test facility shown in FIGS. 5-7 included Kentucky co-fired by propane, Ohio coal fired and two tests with charcoal mixed with organic sulfur.
  • the samples were fired by a propane burner at 62 shown in FIG. 5 or in a combustion oven (not shown) positioned upstream of stack 32. These illustrate the operation of the method and equipment.
  • the data from these tests is set forth in table and graphic form in the Appendix to this application.

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  • Engineering & Computer Science (AREA)
  • Environmental & Geological Engineering (AREA)
  • Chemical & Material Sciences (AREA)
  • Health & Medical Sciences (AREA)
  • Biomedical Technology (AREA)
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Abstract

La présente invention concerne un procédé et un appareil de nettoyage et de recyclage de gaz de combustion provenant de centrales électriques alimentées au charbon, d'installations de chauffage au gaz naturel ou au propane, ou de fours à ciment, au moyen de catalyseurs de zéolite renouvelables permettant de séparer des matières polluantes en matériaux recyclables et réutilisables. Le procédé permet une réduction, dans le gaz de combustion, du monoxyde de carbone (CO), du dioxyde de carbone (CO2), de l'oxyde d'azote (NOx), de l'oxyde de soufre (SOx), de même que des halogènes tels que du chlorure et des fluorures, et des métaux à l'état de traces, particulièrement de mercure, de plomb et de zinc.
PCT/US2016/022107 2015-05-27 2016-03-11 Combustion de charbon propre WO2016190942A1 (fr)

Applications Claiming Priority (4)

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US14/722,244 US9737849B2 (en) 2013-03-15 2015-05-27 Cleaning stack gas
US14/722,244 2015-05-27
US15/067,569 US9919269B2 (en) 2013-03-15 2016-03-11 Clean coal stack
US15/067,569 2016-03-11

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CN109847571A (zh) * 2019-04-02 2019-06-07 江苏优拿大环保科技有限公司 一种新的半干法脱硫工艺
CN111569626A (zh) * 2020-05-22 2020-08-25 四川君和环保股份有限公司 一种烧结烟气处理工艺及系统

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EP2862619A1 (fr) * 2013-10-21 2015-04-22 IMIS Spolka z ograniczona Procédé de dissociation des gaz d'échappement, en particulier de gaz contenant du dioxyde de carbone (CO2) et une chambre de réacteur

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* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN109847571A (zh) * 2019-04-02 2019-06-07 江苏优拿大环保科技有限公司 一种新的半干法脱硫工艺
CN109847571B (zh) * 2019-04-02 2022-03-04 江苏优拿大环保科技有限公司 一种新的半干法脱硫工艺
CN111569626A (zh) * 2020-05-22 2020-08-25 四川君和环保股份有限公司 一种烧结烟气处理工艺及系统

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