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WO2014138323A1 - Lutte contre les émissions de mercure - Google Patents

Lutte contre les émissions de mercure Download PDF

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Publication number
WO2014138323A1
WO2014138323A1 PCT/US2014/020969 US2014020969W WO2014138323A1 WO 2014138323 A1 WO2014138323 A1 WO 2014138323A1 US 2014020969 W US2014020969 W US 2014020969W WO 2014138323 A1 WO2014138323 A1 WO 2014138323A1
Authority
WO
WIPO (PCT)
Prior art keywords
mercury
phyllosilicate
flue gas
air heater
particulate
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Ceased
Application number
PCT/US2014/020969
Other languages
English (en)
Inventor
James Robert BUTZ
Michael A. Lucarelli
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Novinda Corp
Original Assignee
Novinda Corp
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Novinda Corp filed Critical Novinda Corp
Publication of WO2014138323A1 publication Critical patent/WO2014138323A1/fr
Anticipated expiration legal-status Critical
Ceased legal-status Critical Current

Links

Classifications

    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F23—COMBUSTION APPARATUS; COMBUSTION PROCESSES
    • F23J—REMOVAL OR TREATMENT OF COMBUSTION PRODUCTS OR COMBUSTION RESIDUES; FLUES 
    • F23J15/00—Arrangements of devices for treating smoke or fumes
    • F23J15/003—Arrangements of devices for treating smoke or fumes for supplying chemicals to fumes, e.g. using injection devices
    • 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
    • B01D53/02—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 by adsorption, e.g. preparative gas chromatography
    • 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
    • B01D53/46—Removing components of defined structure
    • B01D53/64—Heavy metals or compounds thereof, e.g. mercury
    • 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
    • B01D53/81—Solid phase processes
    • B01D53/83—Solid phase processes with moving reactants
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2251/00—Reactants
    • B01D2251/40—Alkaline earth metal or magnesium compounds
    • B01D2251/404—Alkaline earth metal or magnesium compounds of calcium
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2251/00—Reactants
    • B01D2251/60—Inorganic bases or salts
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2253/00—Adsorbents used in seperation treatment of gases and vapours
    • B01D2253/10—Inorganic adsorbents
    • B01D2253/106—Silica or silicates
    • 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
    • B01D2257/602—Mercury or mercury 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
    • B01D2258/0283—Flue gases
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2259/00—Type of treatment
    • B01D2259/12—Methods and means for introducing reactants
    • B01D2259/128—Solid reactants
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F23—COMBUSTION APPARATUS; COMBUSTION PROCESSES
    • F23J—REMOVAL OR TREATMENT OF COMBUSTION PRODUCTS OR COMBUSTION RESIDUES; FLUES 
    • F23J2215/00—Preventing emissions
    • F23J2215/60—Heavy metals; Compounds thereof

Definitions

  • This disclosure relates to the apparatus and procedure for capturing mercury using a particulate mercury sorbent injected above an air heater in a boiler installation.
  • Combustion gasses from incinerators, power plants, and coal-fired furnaces typically contain oxides of sulfur (SO x ), oxides of nitrogen (NO x ), and volatile heavy metals such as mercury. On combustion, the mercury is volatilized and carried in the combustion exhaust gasses into the atmosphere.
  • SO x sulfur
  • NO x oxides of nitrogen
  • mercury volatile heavy metals
  • Coal-burning electric power plants are the single biggest source of mercury emissions, accounting for 40 percent of the total mercury emitted from all man-made sources. Coal-fired burners account for another 10 percent.
  • Coal fired power stations burning high sulfur bituminous and sub-bituminous coal combustion gases typically discharge combustion gases containing 10-20 ⁇ g/Nm 3 total mercury and 1 to 3 ⁇ g/Nm 3 elemental mercury (Hg°) from their electrostatic precipitation (ESP) systems.
  • ESP electrostatic precipitation
  • SO x absorption media with approximately 5% of the inbound Hg x passing through the system.
  • Wet FGD absorption media are typically 25-30% w/w solids dispersions of calcium carbonate, magnesium carbonate, or a mixture thereof and their respective sulphites and sulphates.
  • Mercury poses a serious problem for human beings and the environment and as such protection from exposure to mercury pollution has been the subject of US legislation resulting in The Clean Air Mercury Rule of Mar. 15, 2005 and the EPA's Clean Air Interstate Rule (CAIR).
  • Mercury, atomic symbol Hg is a persistent, bioaccumulative toxic metal that is emitted in combustion gasses in three forms: Elemental mercury, Hg°, oxidized mercury, Hg 2+ compounds, and particle-bound mercury. After mercury has precipitated from the air and deposited into bodies of water or onto the land, methylmercury is formed by microbial action in the top layers of sediment and soils. Once formed, methylmercury is taken up by aquatic organisms and bioaccumulates up the aquatic food web. Methylmercury is a well-established human neurotoxicant. Methylmercury that is ingested by humans is readily absorbed from the gastrointestinal tract and can cause effects in several organ systems.
  • Efforts to control mercury emissions employ sorbents and/or reactants in attempts to separate the gaseous mercury from the flue gas.
  • adsorbents such as powdered activated carbon, silicates, zeolites, clays and ash as solid supports for binding mercury on the surfaces of the solid.
  • Other approaches utilize adsorbents such as powdered activated carbon, silicates, zeolites, clays and ash as solid supports for binding mercury on the surfaces of the solid.
  • Other approaches utilize
  • sulfide/polysulfide reagents to react with mercury or mercury ions and form mercury sulfides (e.g., cinnabars).
  • a first embodiment is a process that includes providing a boiler installation that includes a furnace having a gas outlet which conveys flue gas to an air heater and a particulate collection device; injecting a phyllosilicate mercury sorbent into the gas outlet between the furnace and the air heater; mixing the phyllosilicate mercury sorbent with the flue gas in the gas outlet and in the air heater; forming a mercury sorbed phyllosilicate by reacting the phyllosilicate mercury sorbent with mercury carried in the flue gas; removing the mercury sorbed phyllosilicate from the flue gas with the particulate collection device; and providing a stack emission that includes at least a portion of the flue gas.
  • Another embodiment is an apparatus that includes a boiler installation that includes a furnace having a gas outlet that conveys flue gases to an air heater, the air heater upstream of a particulate collection device, and the particulate collection device fluidly connected to a stack; and a first particulate injection device adapted to provide a phyllosilicate mercury sorbent to flue gas carried in the gas outlet, the first particulate injection device further positioned to provide the phyllosilicate mercury sorbent at a location wherein the phyllosilicate mercury sorbent has a residence time in the flue gas of less than 1 second prior to entering the air heater.
  • Figure 1 is an illustration of a prior art a coal-fired utility boiler installation of the type used by utilities in the generation of electric power;
  • Figure 2 is a plot of data comparing mercury sorbent injection locations and performance
  • Figure 3 is a comparison plot of background/baseline data to the injection of a mercury sorbent above an air heater, as described herein;
  • Figure 4 is the performance over time for the injection of a mercury sorbent above an air heater, as described herein.
  • a mercury sorbent is subjected to an environment wherein thermal degradation and deactivation of the sorbent is expected but wherein the mercury capture is enhanced.
  • the sulfide based mercury sorbents employed herein are known to deactivate (e.g., by sulfide oxidation) at elevated temperatures whereas, the mercury capture by these materials under the herein described process and apparatus provides exceptional mercury capture.
  • the injection of the mercury sorbent downstream of a SCR unit and upstream of the air heater is in excess of 200 °C, 300 °C, or 400 °C.
  • the temperature of the flue gases at the injection point is less than the temperature in the furnace or at a steam generation unit, for example less than 500 °C.
  • Figure 1 illustrates a typical boiler installation 10 that includes a furnace 12, air heater 18, particulate collection device 26, wet scrubber 30 and stack 32.
  • the boiler installation 10 includes a furnace 12 having a gas outlet 14 which conveys flue gases, generally designated 16, to an air heater 18 used to preheat incoming air 20 for combustion.
  • Pulverizers 22 grind a fossil fuel 24 (e.g., coal) to a desired fineness and the pulverized coal 24 is conveyed via burners 25 into the furnace 12 where it is burned to release heat used to generate steam for use by a steam turbine-electric generator (not shown).
  • a fossil fuel 24 e.g., coal
  • Flue gases 16 produced by the combustion process are conveyed through the gas outlet 14 to the air heater 18 and then to various types of downstream flue gas cleanup equipment.
  • the flue gas cleanup equipment may comprise a particulate collection device (e.g., fabric filter or, as shown, an electrostatic precipitator (ESP)) 26 which removes particulates from the flue gas 16.
  • a flue gas conduit 28 downstream of the particulate collection device 26 conveys the flue gas 16 to a wet scrubber absorber module 30 which is used to remove sulfur dioxide and other contaminants from the flue gas 16.
  • Flue gas 16 exiting from the wet scrubber absorber module or, simply, the wet scrubber 30, is conveyed to a stack 32 and exhausted to atmosphere.
  • Forced draft fans 34 and induced draft fans 36 are used to propel the air 20, fuel 24, and flue gases 16 through the installation 10.
  • an apparatus that includes a boiler installation 10.
  • the boiler installation 10 includes a furnace 12 having a gas outlet 14 that conveys flue gases 16 to an air heater 18, the air heater 18 upstream of a particulate collection device 26, and the particulate collection device 26 fluidly connected to a stack 32.
  • the apparatus further including a first particulate injection device adapted to provide a phyllosilicate mercury sorbent to flue gas 16 carried in the gas outlet 14.
  • the first particulate injection device further positioned to provide the phyllosilicate mercury sorbent at a location wherein the phyllosilicate mercury sorbent has a residence time in the flue gas of less than two seconds, preferably less than one second, prior to entering the air heater 18.
  • the first particulate injection device includes a first particulate duct injection lance and a means of supplying the phyllosilicate mercury sorbent to the duct injection lance.
  • the phyllosilicate mercury sorbent is a powdered material and is supplied to the duct injection lance by the flow of a pressurized gas.
  • the first particulate injection device can further include a means of supplying the pressurized gas (e.g., an air compressor or a pressurized gas tank).
  • the first particulate injection device can include one or more pressurized gas lines in addition to a phyllosilicate mercury sorbent supply line.
  • the apparatus can further include a second particulate injection device.
  • the second particulate injection device can be adapted to provide lime to flue gas 16 carried in the gas outlet 14.
  • the second particulate injection device further positioned to provide the lime at a location wherein the lime has a residence time in the flue gas of less than one second prior to entering the air heater 18.
  • lime can include calcium oxides and/or calcium hydroxides (e.g., quicklime, slaked lime, or hydrated lime).
  • the air heater 18 is typically a heat exchanger.
  • the air heater 18 can be a shell and tube type heat exchanger, a stationary plate heat exchanger, (rotating) regenerative heat exchanger.
  • the air heater 18 can be adapted to induce turbulent flow on the flue gas.
  • the air heater 18 can be adapted to provide lamellar flow on the flue gas.
  • the arrangement of the first and second particulate injection devices can be adjusted to provide for longer residence times prior to the injected particulates entering the air heater 18.
  • the second particulate injection device is positioned upstream of the first particulate injection device.
  • the air heater 18 includes a flue gas inlet and a flue gas outlet.
  • the flue gas conduit carrying the flue gas from the flue gas outlet of the air heater 18 includes at least one 90° turn.
  • the flue gas conduit can include a turn sufficient to carry the flue gas in a direction perpendicular to the flow of the flue gas through the air heater 18.
  • the flue gas conduit makes at least two, even more preferably three, 90° turns prior to depositing the flue gas at a flue gas inlet of the particle collection device.
  • the apparatus of the present embodiment can further include a conveyor adapted to carry the phyllosilicate mercury sorbent from a phyllosilicate mercury sorbent reservoir to the first particulate injector.
  • the reservoir can include a silo, preferably with a chute adapted to provide the phyllosilicate mercury sorbent from the silo to a conveying line.
  • the conveying line adapted to provide the phyllosilicate mercury sorbent to duct injection lances.
  • the apparatus further includes a blower package adapted to provide a pressurized gas flow through the conveying line and carry the phyllosilicate mercury sorbent to the duct injection lances.
  • the above described apparatus can be used to capture and remove mercury from the flue gases produced by the combustion of fossil fuels.
  • the process includes providing a boiler installation 10 that includes a furnace 12 having a gas outlet 14 which conveys flue gas 16 to an air heater 18 and a particulate collection device 26; injecting a phyllosilicate mercury sorbent into the gas outlet between the furnace and the air heater 18; mixing the phyllosilicate mercury sorbent with the flue gas in the gas outlet and in the air heater 18; forming a mercury sorbed phyllosilicate by reacting the phyllosilicate mercury sorbent with mercury carried in the flue gas 16; removing the mercury sorbed phyllosilicate from the flue gas 16 with the particulate collection device 26; and providing a stack emission that includes at least a portion of the flue gas 16.
  • the process can additionally include providing less than a two second or less than a one second residence time for the phyllosilicate mercury sorbent in the flue gas prior to the phyllosilicate entering the air heater 18.
  • the phyllosilicate mercury sorbent can be injected into the gas outlet at a location where the flue gas has a temperature in a range of about 200 °C to about 425 °C, about 260 °C to about 370 °C, about 260 °C to about 290 °C, or about 315 °C to about 370 °C.
  • the process can include injecting lime into the gas outlet 14 between the furnace 12 and the air heater 18; and mixing the lime with the flue gas 16 in the gas outlet 14 and in the air heater 18.
  • lime refers to calcium oxide and/or calcium hydroxide.
  • the lime can be injected into the gas outlet at a location where the flue gas has a temperature in a range of about 200 °C to about 425 °C, about 260 °C to about 370 °C, about 260 °C to about 290 °C, or about 315 °C to about 370 °C.
  • the process results in reducing a mercury concentration in the flue gas by at least 50%, at least 60%, at least 70%, at least 80% across the particulate collection device. That is, the mercury concentration in the flue gas after the particulate collection device is at least 50% less than the mercury concentration in the flue gas after the air heater 18. Still further, the process includes capturing a majority of the mercury in the flue gas at the particulate collection device. The mercury can be sorbed by the particulate mercury sorbent, the fly ash, and/or other particulates in the flue gas or added to the flue gas.
  • the process can further include an additional reduction in the mercury concentration in the flue gas before stack emission.
  • the mercury concentration is further reduced by about 5% to about 25%, about 5% to about 20%, about 5 to about 15% before the stack emission.
  • This further reduction in mercury concentration can be provided by or achieved using a wet scrubber.
  • Comparative testing was performed on an apparatus as described above, where the particulate collection device was an ESP (electrostatic precipitator). Flue gas mercury concentrations were determined before the ESP, after the ESP and before the wet scrubber, and after the wet scrubber (corresponding to stack emissions). Injections of the particulate mercury sorbent (e.g., the mercury sorbent provided in the Assignee's US Patents Nos.
  • ESP electrostatic precipitator
  • 6,719,828; 7,048,781 ; and 7,288,499) were performed up-stream of the air heater (as described herein), down-stream of the air heater and up-stream of the particulate collection device, and up-stream of the wet scrubber.
  • Figure 2 provides results for the capture of mercury dependent on the location of particulate mercury sorbent injection.
  • Figures 3 and 4 provide the results of a 100 hour continuous injection test, where a copper sulfide based phyllosilicate (AMENDED SILICATES available from NOVINDA) is injected up-stream of the air heater at a rate of about 400 Ibs/hr and where hydrated lime is injected up-stream of the air heater at a rate of about 500 Ibs/hr.
  • AMENDED SILICATES available from NOVINDA

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  • Engineering & Computer Science (AREA)
  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • General Chemical & Material Sciences (AREA)
  • Analytical Chemistry (AREA)
  • Oil, Petroleum & Natural Gas (AREA)
  • Environmental & Geological Engineering (AREA)
  • Health & Medical Sciences (AREA)
  • Biomedical Technology (AREA)
  • Mechanical Engineering (AREA)
  • General Engineering & Computer Science (AREA)
  • Treating Waste Gases (AREA)

Abstract

La présente invention concerne un procédé dans le cadre duquel un sorbant du mercure est soumis à un environnement dans lequel le sorbant va faire l'objet d'une dégradation thermique et d'une désactivation s'accompagnant d'une capture renforcée du mercure. Selon un mode de réalisation, un procédé comprend les étapes consistant à injecter un sorbant du mercure à base de phyllosilicate dans l'orifice de sortie de gaz entre le four et le dispositif de chauffage de l'air; à obtenir un phyllosilicate dans lequel le mercure est retenu suite à la réaction du sorbant du mercure à base de phyllosilicate avec le mercure présent dans le gaz de combustion; et à éliminer le phyllosilicate dans lequel est retenu le mercure du gaz de combustion au moyen d'un dispositif de recueil de particules. Selon un autre mode de réalisation, un appareil comporte un dispositif d'injection de particules conçu pour alimenter en sorbant du mercure à base de phyllosilicate le gaz de combustion s'échappant par l'orifice de sortie de gaz, ledit dispositif d'injection de particules étant positionné de façon à pouvoir introduire le sorbant du mercure à base de phyllosilicate au niveau d'un site tel que la durée de séjour du sorbant du mercure à base de phyllosilicate dans le gaz de combustion se révèle inférieure à 1 seconde avant son entrée dans le dispositif de chauffage de l'air.
PCT/US2014/020969 2013-03-06 2014-03-06 Lutte contre les émissions de mercure Ceased WO2014138323A1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
US201361773459P 2013-03-06 2013-03-06
US61/773,459 2013-03-06

Publications (1)

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WO2014138323A1 true WO2014138323A1 (fr) 2014-09-12

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Citations (7)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US6528030B2 (en) * 1998-12-07 2003-03-04 Mcdermott Technology, Inc. Alkaline sorbent injection for mercury control
US6558454B1 (en) * 1997-08-19 2003-05-06 Electric Power Research Institute, Inc. Method for removal of vapor phase contaminants from a gas stream by in-situ activation of carbon-based sorbents
US20070092418A1 (en) * 2005-10-17 2007-04-26 Chemical Products Corporation Sorbents for Removal of Mercury from Flue Gas
US7288499B1 (en) * 2001-04-30 2007-10-30 Ada Technologies, Inc Regenerable high capacity sorbent for removal of mercury from flue gas
US20090056538A1 (en) * 2003-06-03 2009-03-05 Srivats Srinivasachar Control of mercury emissions from solid fuel combustion
US7776141B2 (en) * 2007-09-25 2010-08-17 Hitachi Power Systems America, Ltd. Methods and apparatus for performing flue gas pollution control and/or energy recovery
US20110230334A1 (en) * 2007-08-02 2011-09-22 David Goldberg Composition, Production And Use Of Sorbent Particles For Flue Gas Desulfurization

Patent Citations (7)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US6558454B1 (en) * 1997-08-19 2003-05-06 Electric Power Research Institute, Inc. Method for removal of vapor phase contaminants from a gas stream by in-situ activation of carbon-based sorbents
US6528030B2 (en) * 1998-12-07 2003-03-04 Mcdermott Technology, Inc. Alkaline sorbent injection for mercury control
US7288499B1 (en) * 2001-04-30 2007-10-30 Ada Technologies, Inc Regenerable high capacity sorbent for removal of mercury from flue gas
US20090056538A1 (en) * 2003-06-03 2009-03-05 Srivats Srinivasachar Control of mercury emissions from solid fuel combustion
US20070092418A1 (en) * 2005-10-17 2007-04-26 Chemical Products Corporation Sorbents for Removal of Mercury from Flue Gas
US20110230334A1 (en) * 2007-08-02 2011-09-22 David Goldberg Composition, Production And Use Of Sorbent Particles For Flue Gas Desulfurization
US7776141B2 (en) * 2007-09-25 2010-08-17 Hitachi Power Systems America, Ltd. Methods and apparatus for performing flue gas pollution control and/or energy recovery

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