WO2006051650A1 - Appareil et procédé servant à enlever du mercure - Google Patents

Appareil et procédé servant à enlever du mercure Download PDF

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Publication number
WO2006051650A1
WO2006051650A1 PCT/JP2005/017156 JP2005017156W WO2006051650A1 WO 2006051650 A1 WO2006051650 A1 WO 2006051650A1 JP 2005017156 W JP2005017156 W JP 2005017156W WO 2006051650 A1 WO2006051650 A1 WO 2006051650A1
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WO
WIPO (PCT)
Prior art keywords
mercury
gas
treated
exhaust gas
iron
Prior art date
Application number
PCT/JP2005/017156
Other languages
English (en)
Japanese (ja)
Inventor
Hiroyuki Akiho
Shigeo Ito
Takashi Kiga
Noriyuki Iiyama
Kenji Takano
Original Assignee
Central Research Institute Of Electric Power Industry
Ishikawajima-Harima Heavy Industries Co., Ltd.
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 Central Research Institute Of Electric Power Industry, Ishikawajima-Harima Heavy Industries Co., Ltd. filed Critical Central Research Institute Of Electric Power Industry
Publication of WO2006051650A1 publication Critical patent/WO2006051650A1/fr

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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
    • F23J15/02—Arrangements of devices for treating smoke or fumes of purifiers, e.g. for removing noxious material
    • F23J15/04—Arrangements of devices for treating smoke or fumes of purifiers, e.g. for removing noxious material using washing fluids
    • 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
    • B01D2257/00—Components to be removed
    • B01D2257/60—Heavy metals or heavy metal compounds
    • B01D2257/602—Mercury or mercury compounds
    • 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

  • the present invention relates to a mercury removal apparatus and method.
  • Japanese Patent Application Laid-Open No. 10-216476 discloses several exhaust gas treatment apparatus powers S for removing zero-valent mercury Hg in exhaust gas, which is an object to be treated.
  • the exhaust gas treatment device shown in FIG. 3 is an exhaust gas treatment device equipped with a two-column wet desulfurization device comprising a cooling tower and an absorption tower.
  • mercury removal agents such as sodium hypochlorite, copper chloride, manganese chloride, iron chloride, chelating agent, coal ash, etc. are added to the circulating water of the cooling tower placed in the previous stage, so that This product converts and removes the mercury Hg G into water-soluble divalent mercury Hg 2+ .
  • Patent Document 1 Japanese Patent Laid-Open No. 10-216476
  • the exhaust gas treatment apparatus of Patent Document 1 has the following problems.
  • the present invention has been made in view of the above-described circumstances, and aims to suppress and reduce the amount of mercury oxidant used and to separate and remove zero-valent mercury gas at a sufficient removal rate for the gas to be processed. It is a life.
  • zero-valent mercury gas is converted into water-soluble divalent mercury gas and separated from the gas to be treated.
  • the apparatus for removal comprises a reaction separation means for bringing an aqueous solution containing a mercury oxidant composed of trivalent iron Fe 3+ and having a pH of about 1 or less into contact with the gas to be treated.
  • Adopt means for bringing an aqueous solution containing a mercury oxidant composed of trivalent iron Fe 3+ and having a pH of about 1 or less into contact with the gas to be treated.
  • the reaction separating means includes a nozzle for spraying an aqueous solution onto the gas to be treated, and after contacting the gas to be treated by the nozzle.
  • a recovery container for recovering the aqueous solution of the aqueous solution, a circulation pump for supplying the aqueous solution recovered in the recovery container to the nozzle, a mercury oxidant addition device for adding a mercury oxidant to the aqueous solution, and the recovery container A pH meter that measures the pH of the aqueous solution, and a pH adjuster addition unit that adds a pH adjuster to the aqueous solution so that the pH of the aqueous solution sprayed from the nozzle is 1 or less based on the measurement result of the pH meter T ⁇ ⁇
  • the solution method is adopted.
  • the nozzle, the recovery container, and the circulation pump constitute a cooling tower arranged in the preceding stage in the two-column type wet desulfurization apparatus.
  • the reaction separation means adopts the solution means that the cooling tower is configured with a pH measuring device, a pH adjuster addition unit, and a mercury oxidizer addition device.
  • the mercury oxidizing agent is iron chloride FeCl containing iron Fe 3+ as a component.
  • any one of the above first to fourth means is adopted. If the pH adjuster is hydrochloric acid HC1, the solution is adopted.
  • the above-described solving means is adopted in which any one of the above first to fifth means is that the gas to be treated is combustion exhaust gas from a combustion furnace.
  • a method of converting zero-valent mercury gas into water-soluble divalent mercury gas and separating it from the gas to be treated is removed.
  • the zero-valent mercury gas is converted to the divalent mercury gas by contacting an aqueous solution containing a mercury oxidizer containing trivalent iron Fe 3+ and having a pH of about 1 or less with the gas to be treated.
  • a solution is adopted that is dissolved in an aqueous solution and separated and removed from the gas to be treated.
  • a pH adjuster and a mercury oxidant for reducing the pH to about 1 or less are used in a two-stage wet desulfurization apparatus.
  • a solution is adopted in which zero-valent mercury gas is separated and removed from the gas to be treated by adding it to the washing water or circulating water of the cooling tower.
  • a solution is used in which the mercury oxidizer is iron chloride FeCl containing trivalent iron Fe 3+ as a component.
  • any one of the above first to third methods is adopted. If the pH adjuster is hydrochloric acid HC1, the solution is adopted.
  • any one of the above first to fourth means is adopted. If the gas to be treated is combustion exhaust gas from a combustion furnace, the solution is adopted. .
  • the invention's effect is adopted.
  • the zero-valent mercury gas is divalent mercury by bringing an aqueous solution of a mercury oxidizing agent containing trivalent iron Fe 3+ into a pH 1 or lower and bringing it into gas-liquid contact with the gas to be treated. Since it is converted into a gas and dissolved in an aqueous solution and separated from the gas to be treated, zero-valent mercury gas can be separated from the gas to be treated with a sufficient removal rate while suppressing the amount of mercury oxidizing agent used.
  • FIG. 1 is a system diagram of an exhaust gas treatment apparatus to which a mercury removal apparatus according to an embodiment of the present invention is applied.
  • FIG. 2 is a block diagram showing a detailed configuration of a mercury removing apparatus according to an embodiment of the present invention.
  • FIG. 3 is an experimental result showing the effectiveness of using trivalent iron Fe 3+ as a component as a mercury oxidizing agent in an embodiment of the present invention.
  • FIG. 4 is an experimental result showing the effect of pH on the Hg capture rate when using iron chloride FeCl having excellent oxidation performance against zero-valent mercury Hg according to an embodiment of the present invention. is there.
  • FIG. 5 is an experimental result showing the dependence of the Hg G trapping rate on the concentration of trivalent iron Fe 3+ in one embodiment of the present invention.
  • FIG. 6 In one embodiment of the present invention, simulation according to the circulation rate of an aqueous solution of salted pig iron FeCl
  • FIG. 7 is an experimental result showing the influence of gas-liquid contact on the simulated combustion exhaust gas in one embodiment of the present invention.
  • FIG. 1 is a system diagram of an exhaust gas treatment apparatus to which the mercury removal apparatus according to this embodiment is applied.
  • this exhaust gas treatment device is composed of a boiler 1, a denitration device 2, an electric dust collector 3, a two-column desulfurization device 4 and a chimney 5.
  • the boiler 1 is for generating steam for power generation at, for example, a thermal power plant, and generates steam using oil, natural gas, coal, or the like as fuel. Exhaust gas generated by burning such fuel in the boiler 1 is supplied from the boiler 1 to the denitration device 2.
  • the denitration apparatus 2 removes nitrogen oxides NOx contained in the exhaust gas. This The denitrification apparatus 2 decomposes nitrogen oxides NOx into nitrogen N and water HO, for example, by causing ammonia to act on exhaust gas in the presence of a catalyst.
  • the electric dust collector 3 is
  • the double tower type desulfurization apparatus 4 is a double tower type wet desulfurization apparatus that wet-removes sulfur oxide SOx contained in the exhaust gas, and as shown in the drawing, the cooling tower 4A arranged in the preceding stage and the absorption arranged in the latter stage. It is composed of power with Tower 4B.
  • the cooling tower 4A has both a function of cooling the exhaust gas using circulating water and a function as a mercury removing apparatus according to the present embodiment.
  • the cooling tower in a general two-column desulfurization apparatus aims at cooling and dust removal of exhaust gas
  • the circulating water is general water, but the circulating water W in this embodiment cools and removes the exhaust gas.
  • This is an aqueous solution containing a mercury oxidizer containing iron Fe 3+ as a component.
  • the use of such an aqueous solution as the circulating water W is one of the features of this embodiment.
  • the mercury oxidizer is preferably salted pig iron FeCl, but contains trivalent iron Fe 3+ as a component.
  • the washing water for the cooling tower 4A may be an aqueous solution containing a mercury oxidizing agent.
  • FIG. 2 is a block diagram showing a detailed configuration of the cooling tower 4A, that is, the mercury removing apparatus according to the present embodiment.
  • this mercury removal device is composed of a tower body 6 (collection container), a spray nozzle 7, a circulation pump 8, a pH meter 9, a pH adjuster addition device 10, a mercury oxidant addition device 11 Isometric composition.
  • the tower body 6 is, for example, a hollow cylindrical container.
  • a spray nozzle 7 that injects the circulating water downwards in the upper part of the tower, and a sealed structure that receives and collects the circulating water in the lower part of the inside. It has become.
  • This mercury removal device has the essential components for a cooling tower, that is, the main body 6, the spray nozzle 7 and the circulation pump 8. Agent addition device 10 and mercury oxidant addition device 11 are added.
  • an exhaust gas inlet 6a is provided at the side of the tower body 6, and a treated gas outlet 6b is provided at the upper part.
  • the exhaust gas taken into the tower body 6 from the inlet 6a The circulating water injected from the swell 7 moves upward while making gas-liquid contact, and is discharged to the outside of the tower main body 6 as a treated gas.
  • the spray nozzle 7 is arranged with a spread at the upper part in the tower body 6 so that the circulating water is in uniform gas-liquid contact with the exhaust gas in a wide area in the tower body 6.
  • the circulation pump 8 pumps out the circulating water accumulated in the lower part of the tower body 6 and supplies it to the spray nozzle 7.
  • the circulating pump 8 is continuously operated with respect to the exhaust gas that is continuously supplied into the tower body 6 due to the continuous operation of the thermal power plant, the circulating water is sequentially supplied from the spray nozzle 7 to the exhaust gas. Injected, gas-liquid contact between exhaust gas and circulating water is continuously performed.
  • the pH measuring device 9 is provided between the circulation pump 8 and the spray nozzle 7.
  • the pH measuring device 9 measures the pH value of the circulating water supplied from the circulation pump 8 to the spray nozzle 7, that is, the circulating water injected into the exhaust gas, and outputs the pH value to the pH adjuster adding device 10 as pH information.
  • the pH adjuster addition device 10 supplies the pH adjuster to the circulating water so that the pH value of the circulating water measured by the pH meter 9 is maintained at about 1 or less.
  • This pH adjuster is preferably HC1 hydrochloride.
  • sulfuric acid HSO lowers the removal performance of zero-valent mercury gas.
  • Mercury oxidizer addition device 11 can be used for example,
  • the absorption tower 4B is for removing the oxalic acid SOx from the treated gas discharged from the cooling tower 4A (that is, the mercury removing device).
  • the absorption tower 4B separates the oxalic acid SOx as gypsum Ca SO into the absorption liquid by reacting the exhaust gas with an absorption liquid containing, for example, lime slurry.
  • the chimney 5 has an absorption tower 4B, that is, a two-column desulfurization device 4
  • the exhaust gas exhausted from the power is released to the high air outside.
  • Fig. 3 shows experimental results showing the effectiveness of using a trivalent iron Fe 3+ component as a mercury oxidant. More specifically, salty iron-iron FeCl containing trivalent iron Fe 3+ as a component, iron chloride FeCl containing divalent iron Fe 2+ as a component, tetravalent titanium Ti used in this embodiment. 4+
  • Salt-titanium TiCl as a component
  • Trivalent titanium Ti3 + Salt-titanium TiCl as a component
  • Trivalent titanium Aluminum 3 Aluminum A1C1 with Al 3+ as component
  • phosphoric acid HP with pentavalent phosphorus P 5+ as component
  • the 3rd liquid shows a high Hg G trapping rate, it repels salted iron iron FeCl containing divalent iron Fe2 +.
  • Trivalent iron Fe 3+ is zero-valent mercury Hg.
  • acidity that is, zero-valent mercury Hg.
  • FIG. 4 is an experimental result showing the influence of pH on the Hg trapping rate when iron chloride FeCl having excellent oxidation performance against zero-valent mercury Hg ° as described above is used.
  • the pH was adjusted by keeping it constant and adding HC1 hydrochloric acid.
  • the Hg capture rate hardly increases even when the chlorine C1 concentration, that is, the amount of HC1 added, is increased in the region below pHl. Therefore, the amount of salty pig iron FeCl used as the mercury oxidizer is minimized, and a high Hg capture rate is obtained.
  • the pH is preferable to set the pH to about 1 or less, preferably about 1 or less.
  • FIG. 5 is an experimental result showing the dependence of the Hg G trapping rate on the concentration of trivalent iron Fe 3+ .
  • the Hg capture rate was measured by circulating a mixed gas.
  • a counter-current spray type wet scrubber having the same configuration as the cooling tower 4A described above is used, and the circulation rate of the aqueous solution of iron chloride FeCl as the circulating water is 2 lZmin, 4 lZmin or 5 lZmi.
  • the Hg removal rate of the simulated combustion exhaust gas when switching to n is shown. According to the results of this experiment, it was confirmed that the simulated combustion exhaust gas having substantially the same composition as the exhaust gas of boiler 1 can achieve a Hg removal rate of nearly 80% regardless of the circulation amount. It was done.
  • FIG. 7 shows Experimental Examples 1 and 2 regarding the influence of gas-liquid contact on the simulated combustion exhaust gas.
  • each was filled with 100 ml of absorption liquid (aqueous solution of salted iron iron FeCl).
  • the absorption liquid volume of 100 ml indicates the number of publishing times
  • the absorption liquid volume of 300 ml indicates the publishing frequency of 3
  • the absorption liquid volume of 500 ml indicates the publishing frequency of 5 times.
  • the number of publishing times that is, simulated combustion exhaust gas Hg removal rate increases as the number of gas-liquid contact between the liquid and the absorbent (iron chloride FeCl aqueous solution) increases.
  • salted pig iron FeCl containing trivalent iron Fe 3+ as a component is converted to mercury acid.
  • An aqueous solution that is contained as a soot agent and that has a pH set to about 1 or less by adding a pH adjuster such as hydrochloric acid HC1 is gas-liquid contacted with the gas to be treated such as the exhaust gas (combustion exhaust gas) of boiler 1.
  • a pH adjuster such as hydrochloric acid HC1
  • this mercury removal apparatus is an essential component for the cooling tower, that is, a component for adding a function as a mercury removal apparatus to the tower body 6, the spray nozzle 7 and the circulation pump 8, ie, pH.
  • a measuring instrument 9, a pH adjuster addition device 10 and a mercury oxidant addition device 11 are added. Therefore, by adding a pH meter 9, pH adjuster addition device 10 and mercury oxidizer addition device 11 to an existing thermal power plant, a zero-valent mercury gas removal function can be realized. There are advantages to being able to introduce it easily.
  • Mercury oxidizer is not limited to iron chloride FeCl. It is a compound containing trivalent iron Fe 3+ as a component.
  • the pH adjuster is not limited to HC1 hydrochloric acid, but other ones may be used.
  • the gas to be treated is not limited to the combustion exhaust gas of the combustion furnace of the boiler 1.
  • the configuration of the mercury removal device is not limited to the above embodiment. ⁇ . Any other configuration may be used as long as it can achieve good gas-liquid contact between the gas to be treated and the aqueous solution of the mercury oxidizing agent.

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

Abstract

L'invention concerne un procédé servant à séparer et enlever du mercure gazeux ayant une valence de zéro d'un gaz à traiter, lequel comprend de mettre en contact le gaz à traiter avec une solution aqueuse ayant un pH inférieur ou égal à environ 1 et contenant un agent oxydant le mercure ayant du fer trivalent Fe3+ comme composant, pour de cette manière convertir le mercure gazeux ayant une valence de zéro en mercure divalent gazeux et le dissoudre simultanément dans la solution aqueuse. Le procédé ci-dessus permet la séparation et l'élimination de mercure gazeux ayant une valence de zéro d'un gaz à traiter avec un pourcentage d'élimination satisfaisant tout en limitant la quantité de l'agent oxydant le mercure à utiliser.
PCT/JP2005/017156 2004-11-15 2005-09-16 Appareil et procédé servant à enlever du mercure WO2006051650A1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
JP2004330577A JP2006136856A (ja) 2004-11-15 2004-11-15 水銀除去装置及び方法
JP2004-330577 2004-11-15

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WO2006051650A1 true WO2006051650A1 (fr) 2006-05-18

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Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN108435726A (zh) * 2018-03-30 2018-08-24 北京生态岛科技有限责任公司 一种含汞油池的清洗方法和系统
CN113578030A (zh) * 2020-04-30 2021-11-02 黄华丽 一种脱除烟气中汞的吸收剂浆液及其制备和脱除方法

Families Citing this family (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
ITMI20062524A1 (it) * 2006-12-28 2008-06-29 Itea Spa Processo per la purificazione di fumi di combustione
CN101981183A (zh) 2008-03-25 2011-02-23 三菱瓦斯化学株式会社 使用电喷射将基因转移入细胞的方法及用于所述方法的设备
JP2013039511A (ja) 2011-08-12 2013-02-28 Babcock Hitachi Kk 湿式排煙脱硫装置およびそれを備えた火力発電プラント

Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPS4845474A (fr) * 1971-10-13 1973-06-29
JPH08117555A (ja) * 1994-10-27 1996-05-14 Kanken Techno Kk 水銀蒸気の処理とそのシステム
JPH10216476A (ja) * 1997-01-31 1998-08-18 Kawasaki Heavy Ind Ltd 排ガス処理方法及び装置
JP2003240226A (ja) * 2002-02-18 2003-08-27 Mitsubishi Heavy Ind Ltd 排煙処理装置及び処理方法

Patent Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPS4845474A (fr) * 1971-10-13 1973-06-29
JPH08117555A (ja) * 1994-10-27 1996-05-14 Kanken Techno Kk 水銀蒸気の処理とそのシステム
JPH10216476A (ja) * 1997-01-31 1998-08-18 Kawasaki Heavy Ind Ltd 排ガス処理方法及び装置
JP2003240226A (ja) * 2002-02-18 2003-08-27 Mitsubishi Heavy Ind Ltd 排煙処理装置及び処理方法

Cited By (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN108435726A (zh) * 2018-03-30 2018-08-24 北京生态岛科技有限责任公司 一种含汞油池的清洗方法和系统
CN113578030A (zh) * 2020-04-30 2021-11-02 黄华丽 一种脱除烟气中汞的吸收剂浆液及其制备和脱除方法
CN113578030B (zh) * 2020-04-30 2024-01-26 黄华丽 一种脱除烟气中汞的吸收剂浆液及其制备和脱除方法

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