US20130330257A1 - Sorbents for removal of mercury - Google Patents

Sorbents for removal of mercury Download PDF

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Publication number
US20130330257A1
US20130330257A1 US13/841,315 US201313841315A US2013330257A1 US 20130330257 A1 US20130330257 A1 US 20130330257A1 US 201313841315 A US201313841315 A US 201313841315A US 2013330257 A1 US2013330257 A1 US 2013330257A1
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United States
Prior art keywords
calcium
adsorptive material
mercury
bromide
chloride
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US13/841,315
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English (en)
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Walter G. Tramposch
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Calgon Carbon Corp
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Calgon Carbon Corp
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Priority to US13/841,315 priority Critical patent/US20130330257A1/en
Assigned to CALGON CARBON CORPORATION reassignment CALGON CARBON CORPORATION ASSIGNMENT OF ASSIGNORS INTEREST (SEE DOCUMENT FOR DETAILS). Assignors: TRAMPOSCH, WALTER G.
Priority to PCT/US2013/045061 priority patent/WO2013188327A1/en
Priority to CA2876269A priority patent/CA2876269C/en
Priority to JP2015516277A priority patent/JP6545616B2/ja
Priority to PL13804633T priority patent/PL2858747T3/pl
Priority to IN69MUN2015 priority patent/IN2015MN00069A/en
Priority to MX2014014943A priority patent/MX371091B/es
Priority to AU2013274508A priority patent/AU2013274508A1/en
Priority to CN201710707005.1A priority patent/CN107349902B/zh
Priority to EP13804633.9A priority patent/EP2858747B1/de
Priority to CN201380042764.0A priority patent/CN104602806A/zh
Priority to KR1020157000400A priority patent/KR102217230B1/ko
Publication of US20130330257A1 publication Critical patent/US20130330257A1/en
Assigned to CALGON CARBON CORPORATION reassignment CALGON CARBON CORPORATION ASSIGNMENT OF ASSIGNORS INTEREST (SEE DOCUMENT FOR DETAILS). Assignors: MIMNA, RICHARD A.
Priority to US15/368,900 priority patent/US20170080402A1/en
Priority to AU2017235997A priority patent/AU2017235997A1/en
Priority to JP2018000627A priority patent/JP2018089624A/ja
Priority to HK18106174.5A priority patent/HK1246730A1/zh
Priority to AU2019204609A priority patent/AU2019204609B2/en
Priority to US16/659,120 priority patent/US11857942B2/en
Abandoned legal-status Critical Current

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    • B—PERFORMING OPERATIONS; TRANSPORTING
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    • B01D53/04—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 with stationary adsorbents
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    • 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
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    • B01J20/18—Synthetic zeolitic molecular sieves
    • B—PERFORMING OPERATIONS; TRANSPORTING
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    • B01J20/20—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material comprising free carbon; comprising carbon obtained by carbonising processes
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    • B01J20/28004—Sorbent size or size distribution, e.g. particle size
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    • B01D2257/602—Mercury or mercury compounds
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Definitions

  • Mercury is a known environmental hazard and leads to health problems for both humans and non-human animal species. Approximately 50 tons per year are released into the atmosphere in the United States, and a significant fraction of the release comes from emissions from coal burning facilities such as electric utilities. To safeguard the health of the public and to protect the environment, the utility industry is continuing to develop, test, and implement systems to reduce the level of mercury emissions from its plants. In the combustion of carbonaceous materials, it is desirable to have a process wherein mercury and other undesirable compounds are captured and retained after the combustion phase so that they are not released into the atmosphere.
  • Activated Carbon Injection ACI
  • Activated carbon is a highly porous, non-toxic, readily available material that has a high affinity for mercury vapor. This technology is already established for use with municipal incinerators. Although the ACI technology is effective for mercury removal, the short contact time between the activated carbon and the flue gas stream results in an inefficient use of the full adsorption capacity of the activated carbon. Mercury is adsorbed while the carbon is conveyed in the flue gas stream along with fly ash from the boiler. The carbon and fly ash are then removed by a particulate capture device such as an Electrostatic Precipitator (ESP) or baghouse.
  • ESP Electrostatic Precipitator
  • a mercury adsorptive material comprising an adsorptive material having a volumetric iodine number of greater than 450 mg/cc based on the gravimetric iodine number determined using standard test method (ASTM) D-4607 or an equivalent thereof and the apparent density determined using (ASTM) D-2854 or an equivalent thereof.
  • the volumetric iodine number is about 500 mg/cc to about 650 mg/cc.
  • the adsorptive material can be any material known in the art including, but not limited to activated carbon, reactivated carbon, graphite, graphene, carbon black, zeolite, silica, silica gel, clay, and combinations thereof.
  • the adsorptive material has a mean particle diameter (MPD) of about 1 ⁇ m to about 30 ⁇ m.
  • the mercury adsorptive material may include one or more oxidizing agent, such as, but not limited to, chlorine, bromine, iodine, ammonium bromide, ammonium chloride, calcium hypochlorite, calcium hypobromite, calcium hypoiodite, calcium chloride, calcium bromide, calcium iodide, magnesium chloride, magnesium bromide, magnesium iodide, sodium chloride, sodium bromide, sodium iodide, potassium tri-chloride, potassium tri-bromide, potassium tri-iodide, and combinations thereof, and the one or more oxidizing agent may be about 5 wt.
  • the mercury adsorptive material may include one or more nitrogen source such as, for example, ammonium containing compounds, ammonia containing compounds, amines containing compounds, amides containing compounds, imines containing compounds, quaternary ammonium containing compounds, and combinations thereof, and the one or more nitrogen source may be about 5 wt. % to about 50 wt. % of a total adsorptive material.
  • the one or more nitrogen source may be ammonium iodide, ammonium bromide, or ammonium chloride, amine halides, a quaternary ammonium halides, organo-halides, and combinations thereof.
  • the mercury adsorptive material may include an alkaline agent such as, but not limited to, calcium carbonate, calcium oxide, calcium hydroxide, magnesium carbonate, magnesium hydroxide, magnesium oxide, sodium carbonate, sodium bicarbonate, trisodium hydrogendicarbonate dihydrate, and combinations thereof, and the alkaline agent may be provided at a concentration of greater than or equal to about 0.15 equivalents per 100 grams of absorptive material.
  • inventions are directed to a system for removing mercury from flue gas including an adsorptive material having a volumetric iodine number of greater than 450 mg/cc based on the gravimetric iodine number determined using standard test method (ASTM) D-4607 or an equivalent thereof and the apparent density determined using (ASTM) D-2854 or an equivalent thereof.
  • the volumetric iodine number is about 500 mg/cc to about 650 mg/cc.
  • the system can be any material known in the art including, but not limited to activated carbon, reactivated carbon, graphite, graphene, zeolite, silica, silica gel, clay, and combinations thereof.
  • the adsorptive material has a mean particle diameter (MPD) of about 1 ⁇ m to about 30 ⁇ m.
  • the system may include one or more oxidizing agent, such as, but not limited to, chlorine, bromine, iodine, ammonium bromide, ammonium chloride, calcium hypochlorite, calcium hypobromite, calcium hypoiodite, calcium chloride, calcium bromide, calcium iodide, magnesium chloride, magnesium bromide, magnesium iodide, sodium chloride, sodium bromide, sodium iodide, potassium tri-chloride, potassium tri-bromide, potassium tri-iodide, and combinations thereof, and the one or more oxidizing agent may be about 5 wt.
  • the system may include one or more nitrogen source such as, for example, ammonium containing compounds, ammonia containing compounds, amines containing compounds, amides containing compounds, imines containing compounds, quaternary ammonium containing compounds, and combinations thereof, and the one or more nitrogen source may be about 5 wt. % to about 50 wt. % of a total adsorptive material.
  • the one or more nitrogen source may be ammonium iodide, ammonium bromide, or ammonium chloride, amine halides, a quaternary ammonium halides, organo-halides, and combinations thereof.
  • the system may include an alkaline agent such as, but not limited to, calcium carbonate, calcium oxide, calcium hydroxide, magnesium carbonate, magnesium hydroxide, magnesium oxide, sodium carbonate, sodium bicarbonate, trisodium hydrogendicarbonate dihydrate, and combinations thereof, and the alkaline agent may be provided at a concentration of greater than or equal to about 0.15 equivalents per 100 grams of absorptive material.
  • an alkaline agent such as, but not limited to, calcium carbonate, calcium oxide, calcium hydroxide, magnesium carbonate, magnesium hydroxide, magnesium oxide, sodium carbonate, sodium bicarbonate, trisodium hydrogendicarbonate dihydrate, and combinations thereof, and the alkaline agent may be provided at a concentration of greater than or equal to about 0.15 equivalents per 100 grams of absorptive material.
  • Further embodiments are directed to a method for mercury removal including the step of injecting an adsorptive material having a volumetric iodine number of greater than 450 mg/cc based on the gravimetric iodine number determined using standard test method (ASTM) D-4607 or an equivalent thereof and the apparent density determined using (ASTM) D-2854 or an equivalent thereof into a flue gas stream.
  • the adsorptive material may have a volumetric iodine number is about 500 mg/cc to about 650 mg/cc.
  • the adsorptive material may be, for example, activated carbon, reactivated carbon, graphite, graphene, zeolite, silica, silica gel, clay, and combinations thereof and may have a mean particle diameter (MPD) of about 1 ⁇ m to about 30 ⁇ m.
  • the adsorptive material may further include any of the additives described above.
  • FIG. 1 is a graph showing the relationship between gravimetric iodine number and adsorption of mercury.
  • FIG. 2 is a graph showing the relationship between volumetric iodine number and adsorption of mercury for an adsorbent.
  • combustion chamber is a reference to “one or more combustion chambers” and equivalents thereof known to those skilled in the art, and so forth.
  • the term “about” means plus or minus 10% of the numerical value of the number with which it is being used. Therefore, about 50% means in the range of 45%-55%.
  • Embodiments of the invention are directed to mercury sorbents having enhanced mercury removal capabilities in flue gas streams.
  • Such mercury sorbents have include a mercury adsorptive material having an iodine number of greater than 300 mg/g, and in other embodiments, the mercury adsorptive material may have an iodine number from about 700 mg/g to about 1500 mg/g. In still other embodiments, these mercury sorbents may include one or more additives that may further enhance the effectiveness of the mercury adsorptive material.
  • the mercury adsorptive material of the sorbent composition of various embodiments may include any material having an affinity for mercury.
  • the mercury adsorptive material may be a porous sorbent having an affinity for mercury including, but not limited to, activated carbon, reactivated carbon, graphite, graphene, zeolite, silica, silica gel, clay, and combinations thereof, and in particular embodiments, the mercury adsorptive material may be activated carbon.
  • the mercury adsorptive material may have any mean particle diameter (MPD).
  • the MPD of the mercury adsorptive material may be from about 0.1 ⁇ m to about 100 ⁇ m, and in other embodiments, the MPD may be about 1 ⁇ m to about 30 ⁇ m. In still other embodiments, the MPD of the mercury adsorptive material may be less than about 15 ⁇ m, and in some particular embodiments, the MPD may be about 2 ⁇ m to about 10 ⁇ m, about 4 ⁇ m to about 8 ⁇ m, or about 5 ⁇ m or about 6 ⁇ m. In certain embodiments, the mercury adsorptive materials may have an MPD of less than about 12 ⁇ m, or in some embodiments, less than 7 ⁇ m, which may provide increased selectivity for mercury oxidation.
  • the mercury adsorbent may have high activity as determined by having an iodine number of greater than 300 mg/g.
  • Iodine number is used to characterize the performance of adsorptive materials based on the adsorption of iodine from solution. This provides an indication of the pore volume of the adsorbent material. More specifically, iodine number is defined as the milligrams of iodine adsorbed by one gram of carbon when the iodine concentration in the residual filtrate is 0.02 normal. Greater amounts of adsorbed iodine indicates that the activated carbon has a higher surface area for adsorption and a higher degree of activation activity level.
  • iodine number can refer to either a gravimetric iodine number or a volumetric iodine number.
  • Gravimetric iodine number can be determined using standard test method (ASTM) D-4607, which is hereby incorporated by reference in its entirety, or equivalent thereof.
  • Volumetric iodine number is a product of the gravimetric iodine number (mg of iodine adsorbed/gram of carbon) and the apparent density of the activated carbon (grams of carbon/cc of carbon), which an apparent density can be determined using ASTM D-2854, which is hereby incorporated by reference in its entirety, or an equivalent thereof.
  • the apparent density can be determined using mercury porosimetry test ASTM 4284-12 to determine the void volume via mercury intrusion volume at 1 pound per square inch actual pressure. This intrusion volume defines the void volume of the carbon sample to allow calculation of the carbon particle density, and the apparent density is then calculated by correcting this particle density for the void fraction in a dense packed container of the carbon sample.
  • the void fraction is 40% for a typical 3 fold range in particle size for the sample.
  • Adsorbent materials typically used for mercury adsorption have an iodine number, based on the gravimetric iodine number, of about 300 mg/g to about 400 mg/g, which is thought to provide equivalent performance in mercury adsorption characteristics to adsorptive materials having higher iodine numbers.
  • Various embodiments of the invention are directed to mercury sorbents that include adsorbent materials having gravimetric iodine number for greater than 400 mg/g, greater than 500 mg/g, greater than 600 mg/g, greater than 700 mg/g, greater than 800 mg/g, greater than 900 mg/g, and so on or any gravimetric iodine number therebetween.
  • the adsorptive material may have an iodine number of from about 500 mg/g to about 1500 mg/g, about 700 mg/g to about 1200 mg/g, or about 800 mg/g to about 1100 mg/g, or any gravimetric iodine number between these exemplary ranges.
  • mercury adsorbents exhibiting an iodine number within these exemplary ranges may be an activated carbon or carbonaceous char.
  • adsorbent materials for mercury adsorption may have a volumetric iodine number from about 350 mg/cc to about 800 mg/cc.
  • the volumetric iodine number may be greater than 400 mg/cc, greater than 500 mg/cc, greater than 600 mg/cc, greater than 700 mg/cc, and so on or any volumetric iodine number therebetween.
  • the adsorptive material may have a volumetric iodine number of from about 350 mg/cc to about 650 mg/cc, about 400 mg/cc to about 600 mg/cc, about 500 mg/cc to about 600 mg/cc, about 500 mg/cc to about 700 mg/cc, or any volumetric iodine number between these ranges.
  • mercury adsorbents exhibiting an iodine number within these exemplary ranges may be an activated carbon or carbonaceous char, and in certain embodiments, these activated carbon or carbonaceous chars exhibiting a volumetric iodine number of 400 mg/cc or greater may be combined with activated carbons and carbonaceous chars exhibiting a volumetric iodine number that is less than 400 mg/cc.
  • adsorbent materials having an iodine number within these exemplary ranges may provide improved adsorption over adsorbent materials having a gravimetric iodine number within the commonly used range of about 300 mg/g to about 400 mg/g.
  • about one half as much activated carbon having a gravimetric iodine number between about 700 mg/g to about 1200 mg/g or a volumetric iodine number of about 500 mg/cc to about 2200 mg/cc may be necessary to adsorb the amount of mercury adsorbed by conventional activated carbon.
  • certain embodiments are directed to methods in which about 5 lbs/hr to about 10 lbs/hr of activated carbon having an iodine number of from about 700 mg/g to about 1200 mg/g or a volumetric iodine number of about 500 mg/cc to about 2200 mg/cc can adsorb an equivalent amount of mercury as about 15 lbs/hr of an activated carbon having an gravimetric iodine number of about 500 mg/g (see, Example 1).
  • any of the adsorptive materials described above may be treated with one or more oxidizing agents that enhance mercury adsorption.
  • the oxidizing agent may be a halogen salt including inorganic halogen salts, which for bromine may include bromides, bromates, and hypobromites, for iodine may include iodides, iodates, and hypoiodites, and for chlorine may be chlorides, chlorates, and hypochlorites.
  • the inorganic halogen salt may be an alkali metal or an alkaline earth element containing halogen salt where the inorganic halogen salt is associated with an alkali metal such as lithium, sodium, and potassium or alkaline earth metal such as magnesium, and calcium counterion.
  • Non-limiting examples of inorganic halogen salts including alkali metal and alkali earth metal counterions include calcium hypochlorite, calcium hypobromite, calcium hypoiodite, calcium chloride, calcium bromide, calcium iodide, magnesium chloride, magnesium bromide, magnesium iodide, sodium chloride, sodium bromide, sodium iodide, potassium tri-chloride, potassium tri-bromide, potassium tri-iodide, and the like.
  • the oxidizing agents may be included in the composition at any concentration, and in some embodiments, no oxidizing agent may be included in the compositions embodied by the invention. In embodiments in which oxidizing agents are included, the amount of oxidizing agent may be from about 5 wt.
  • % or greater about 10 wt. % or greater, about 15 wt. % or greater, about 20 wt. % or greater, about 25 wt. % or greater, about 30 wt. % or greater, about 40 wt. % or greater of the total sorbent, or about 5 wt. % to about 50 wt. %, about 10 wt. % to about 40 wt. %, about 20 wt. % to about 30 wt. %, or any amount therebetween.
  • any of the adsorptive materials described above may be treated with one or more nitrogen source.
  • the nitrogen source of such agents may be any nitrogen sources are known in the art and can include, for example, ammonium, ammonia, amines, amides, imines, quaternary ammonium, and the like.
  • the agent may be, for example, chlorine, bromine, iodine, ammonium halide, such as, ammonium iodide, ammonium bromide, or ammonium chloride, an amine halide, a quaternary ammonium halide, or an organo-halide and combinations thereof.
  • the nitrogen containing agent may be ammonium halide, amine halide, or quaternary ammonium halide, and in certain embodiments, the agent may be an ammonium halide such as ammonium bromide.
  • the nitrogen containing agent may be provided about 5 wt. % or greater, about 10 wt. % or greater, about 15 wt. % or greater, about 20 wt. % or greater, about 25 wt. % or greater, about 30 wt. % or greater, about 40 wt. % or greater of the total sorbent, or about 5 wt. % to about 50 wt. %, about 10 wt. % to about 40 wt. %, about 20 wt. % to about 30 wt. %, or any amount therebetween.
  • ammonium halide, amine halide, or quaternary ammonium halide may be absent in some embodiments, in other embodiments, the ammonium halide, amine halide, or quaternary ammonium halide may be the only additive included in the sorbent composition, and in still other embodiments, the ammonium halide, amine halide, or quaternary ammonium halide may be combined with other agents such as, for example, halide salts, halide metal salts, alkaline agents, and the like to prepare a composition or sorbent encompassed by the invention.
  • sorbent may include at least one of a halogen salt such as sodium bromide (NaBr), potassium bromide (KBr), or ammonium bromide (NH 4 Br).
  • the adsorbent material may be combined with an acid gas suppression agent such as, for example, alkaline agent.
  • an acid gas suppression agent such as, for example, alkaline agent.
  • alkaline agents are known in the art and currently used to remove sulfur oxide species from flue gas and any such alkaline agent may be used in the invention.
  • the alkaline additive may be alkali oxides, alkaline earth oxides, hydroxides, carbonates, bicarbonates, phosphates, silicates, aluminates, and combinations thereof
  • the alkaline agent may be calcium carbonate (CaCO 3 ; limestone), calcium oxide (CaO; lime), calcium hydroxide (Ca(OH) 2 ; slaked lime); magnesium carbonate (MgCO 3 ; dolomite), magnesium hydroxide (Mg(OH) 2 ), magnesium oxide (MgO), sodium carbonate (Na 2 CO 3 ), sodium bicarbonate (NaHCO 3 ), trisodium hydrogendicarbonate dihydrate (Na 3 H(CO 3 ) 2 .2H 2 O; trona), and combinations thereof.
  • the alkaline agent may be provided at a concentration greater than or equal to about 0.15 equivalents per 100 grams of absorptive material, wherein one equivalent of the alkaline agent is defined as the amount required to produce one mole of hydroxyl ions or to react with one mole of hydrogen ions.
  • such alkaline agents may have a relatively high surface area such as, for example, above 100 m 2 /g for neat materials. High surface area materials may provide improved kinetics and capabilities for acid gas or SO x mitigation while complementing halogen compounds and other added oxidants to provide oxidation of elemental mercury.
  • alkaline agents are highly polar materials that may associate and bond with water
  • alkaline agents may be combined with the primary mercury sorbent as a physical admixture and may not generally be present on the sorbent surface or contained within the sorbent pore structure.
  • the mercury adsorptive material may be treated to enhance the hydrophobicity of the adsorptive materials with, for example, one or more hydrophobicity enhancement agents that impede the adsorption and transport of water or other treatments of the sorbent that achieve similar results.
  • the mercury adsorptive material may be treated with an amount of one or more elemental halogen that can form a permanent bond with the surface.
  • the elemental halogen may be any halogen such as fluorine (F), chlorine (Cl), or bromine (Br), and in certain embodiments, the elemental halogen may be fluorine (F).
  • the mercury adsorptive material may be treated with a hydrophobicity enhancement agent such as a fluorine salt, organo-fluorine compound, or fluorinated polymer, such as, TEFLON®.
  • treatment may be effectuated by grinding the mercury adsorptive material with the organo-fluorine compound or fluorinated polymer.
  • carbon sorbents used as the mercury adsorptive material may be treated with mineral acids such as but not limited to, hydrochloric acid, nitric acid, boric acid, and sulfuric acid, under high temperature, e.g., greater than about 400° C. or greater than 600° C. or greater than 800° C.
  • concentration of the acid is not critical to such treatments and concentrations as low as 1.0 percent by weight or less may be used.
  • such treatment may enhance hydrophobicity and decreased activity for the catalytic oxidation of sulfur dioxide to sulfuric acid in the presence of oxygen and water.
  • Evidence of such treatments can be found in a high contact pH and a reduced tendency for the carbon alone to decompose hydrogen peroxide when compared to the same carbon without such treatments.
  • the adsorbent material may be combined with an oxidizing agent, nitrogen containing compound, hydrophobicity agent, acid gas suppression agent, or other mercury removal agent (collectively, “additives”) in any way known in the art.
  • the one or more additive may be introduced onto the surface of the adsorbent material by impregnation in which the adsorbent material is immersed in a liquid mixture of additives or the liquid mixture of additives is sprayed or otherwise applied to the adsorbent material.
  • Such impregnation processes result in an adsorbent material in which the additives are dispersed on the surface of the adsorbent material.
  • treatment of the adsorbent material may be combined with one or more additive as a dry admixture in which particles of adsorbent are separated and apart from particles of additive having substantially the same size.
  • one or more additive may be provided by co-milling activated carbon with one or more additive to a mean particle diameter (MPD) of less than or equal to about 12 ⁇ m, less than or equal to about 10 ⁇ m, or less than about 7 ⁇ m.
  • MPD mean particle diameter
  • reducing the mean particle diameter of the sorbent and additives by co-milling allows for a close localization of the sorbent and the additives, but the additives are not contained within the sorbent pore structure.
  • Co-milling may be carried out by any means.
  • the co-milling may be carried out using bowl mills, roller mills, ball mills, jet mills or other mills or any grinding device known to those skilled in the art for reducing the particle size of dry solids.
  • the small MPD may improve the selectivity of mercury adsorption as the halide effectively oxidizes the mercury.
  • dry admixtures of adsorbent materials and additive may allow for a higher percentage of active halide and alkaline agents to be included in the injected sorbent.
  • Mercury adsorbents that are impregnated with an additive by treating with an aqueous solution of the additive can only retain a small percentage of the additive on the surface of the adsorbent, and impregnation tends to clog the pores of porous mercury adsorbents reducing the surface area available for mercury adsorption.
  • the percentage of additive in a dry mixture may be greater than about 10 wt. %, greater than about 15 wt. %, greater than about 20 wt. %, or greater than about 30 wt. % and up to about 50 wt. %, up to about 60 wt. %, or up to about 70 wt. % without exhibiting a reduction in mercury adsorption efficiency.
  • adsorptive material and additives may be combined by any method.
  • an adsorptive material and one or more additive may be combined by blending or mixing the materials into a single mercury sorbent that can then be injected into a flue gas stream.
  • combining may occur during use such that the adsorptive material and the one or more additive are held in different reservoirs and injected simultaneously into a flue gas stream.
  • FIG. 1 For example, the sorbents of various embodiments may be used in flue gas streams having no or extremely low SO 3 content or flue gas streams containing high concentrations of other acid gases such as HCl, HF, or NO x species.
  • the mercury adsorptive material and one or more additive may be combined prior to injection into the flue gas stream by, for example, mixing or blending, the mercury adsorptive material with the one or more additives.
  • the mercury adsorptive material and one or more additives may be injected separately into the flue gas stream and combined in the flue gas stream itself.
  • the mercury adsorbent material and the one or more additives may be introduced into a flue gas stream in different portions of the flue gas stream. For example, in some embodiments, all adsorbent materials and additives may be introduced into the flue gas stream simultaneously and at the same portion of the flue gas stream.
  • an additive such as, for example, a halide salt may be introduced into a boiler or a upstream portion of the flue gas stream and the adsorbent and one or more additional additives may be introduced into the flue gas stream either simultaneously or separately in one or more downstream portions of the flue gas stream.
  • Activated carbons of various activity levels were investigated for their ability to remove mercury from flue gas. Activity was based on the gravimetric iodine number (ASTM D-4607) and volumetric iodine number which the gravimetric iodine number converted to a volumetric basis using the density of the granular material (ASTM D2854). Carbons were all approximately 7 um in size and were injected into test flue gas upstream of the electrostatic precipitator (ESP) either alone or in a dry admixture with 30% w/w ammonium bromide. Results are reported based on lbs/hr required to remove 90% of the mercury in the flue gas stream.
  • ESP electrostatic precipitator
  • FIGS. 1 and 2 shows performance curves for base carbons (no additive) and the base carbon in a dry admixture of 30% w/w ammonium bromide.
  • FIG. 1 shows the relationship of gravimetric iodine number (mg/g) to the amount of adsorbent required to reach 90% mercury removal
  • FIG. 2 shows the relationship between volumetric iodine number (mg/cc) and the amount of adsorbent required to 90% mercury removal.
  • Table 1 shows the apparent density and gravimetric iodine number used to calculate the volumetric iodine number.
  • 15.4 lbs/hr of carbon having an gravimetric iodine number of 462 mg/g and a volumetric iodine number of about 382 mg/cc is required to remove 90% of the mercury from the flue gas stream.
  • about 8.3 lbs/hr is required to remove 90% of the mercury from the flue gas stream with activated carbon having a gravimetric iodine number of 1150 mg/g and a volumetric iodine number of about 610 mg/cc. This provides an about 45% reduction in the amount of activated carbon required to remove 90% of the mercury from a flue gas stream when the activity as determined by iodine number is increased by 40%.
  • FIGS. 1 and 2 also show performance curves for carbons including 30% w/w additive (ammonium bromide) is combined with the activated carbon in a dry admixture before being injected into the flue gas upstream of the ESP.
  • a 40% reduction in the amount of activated carbon from 15.4 lbs/hr to 6.2 lbs/hr
  • ammonium bromide to the activated carbon having an gravimetric iodine number of 462 mg/g.
  • the adsorption of mercury is further enhanced by the introduction of adsorbent having higher activity based on iodine number.
  • 1.8 lbs/hr of activated carbon is necessary to remove 90% of the mercury from the flue gas when activated carbon having a gravimetric iodine number of 1150 mg/g and a volumetric iodine number of about 610 mg/cc. This represents a 60% reduction in the amount of activated carbon necessary to reduce the amount of mercury in a full gas stream by 90%.
  • the performance curves resulting from activated carbon ammonium bromide mixtures exhibit a non-linear relationship which could be indicative of a synergetic interaction between ammonium bromide addition and both volumetric and gravimetric iodine activity.
  • FIG. 2 also shows a non-linear decrease in the amount of carbon required when the volumetric iodine number is above about 500 mg/cc when ammonium bromide is present as an admix. Additionally in FIG. 2 . increasing the volume iodine value of the base carbon does not have a large effect on the performance of this material.
US13/841,315 2012-06-11 2013-03-15 Sorbents for removal of mercury Abandoned US20130330257A1 (en)

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US13/841,315 US20130330257A1 (en) 2012-06-11 2013-03-15 Sorbents for removal of mercury
KR1020157000400A KR102217230B1 (ko) 2012-06-11 2013-06-11 수은 제거용 흡착제
CN201710707005.1A CN107349902B (zh) 2012-06-11 2013-06-11 用于除汞的吸附剂
CN201380042764.0A CN104602806A (zh) 2012-06-11 2013-06-11 用于除汞的吸附剂
JP2015516277A JP6545616B2 (ja) 2012-06-11 2013-06-11 水銀を除去する吸着剤
PL13804633T PL2858747T3 (pl) 2012-06-11 2013-06-11 Sorbenty do usuwania rtęci
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MX2014014943A MX371091B (es) 2012-06-11 2013-06-11 Sorbentes para la eliminacion de mercurio.
AU2013274508A AU2013274508A1 (en) 2012-06-11 2013-06-11 Sorbents for removal of mercury
PCT/US2013/045061 WO2013188327A1 (en) 2012-06-11 2013-06-11 Sorbents for removal of mercury
EP13804633.9A EP2858747B1 (de) 2012-06-11 2013-06-11 Sorptionsmittel zur entfernung von quecksilber
CA2876269A CA2876269C (en) 2012-06-11 2013-06-11 Sorbents for removal of mercury
US15/368,900 US20170080402A1 (en) 2012-06-11 2016-12-05 Sorbents for removal of mercury
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JP2018000627A JP2018089624A (ja) 2012-06-11 2018-01-05 水銀を除去する吸着剤
HK18106174.5A HK1246730A1 (zh) 2012-06-11 2018-05-11 用於除汞的吸附劑
AU2019204609A AU2019204609B2 (en) 2012-06-11 2019-06-28 Sorbents for removal of mercury
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