EP2552569A1 - Verfahren zur verarbeitung eines von schwefelkomponenten zu reinigenden kohlendioxidreichen gases - Google Patents

Verfahren zur verarbeitung eines von schwefelkomponenten zu reinigenden kohlendioxidreichen gases

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Publication number
EP2552569A1
EP2552569A1 EP11712170A EP11712170A EP2552569A1 EP 2552569 A1 EP2552569 A1 EP 2552569A1 EP 11712170 A EP11712170 A EP 11712170A EP 11712170 A EP11712170 A EP 11712170A EP 2552569 A1 EP2552569 A1 EP 2552569A1
Authority
EP
European Patent Office
Prior art keywords
gas
carbon dioxide
sulfur
claus
hydrogen sulfide
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
EP11712170A
Other languages
German (de)
English (en)
French (fr)
Inventor
Johannes Menzel
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.)
ThyssenKrupp Industrial Solutions AG
Original Assignee
ThyssenKrupp Uhde GmbH
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 ThyssenKrupp Uhde GmbH filed Critical ThyssenKrupp Uhde GmbH
Publication of EP2552569A1 publication Critical patent/EP2552569A1/de
Ceased legal-status Critical Current

Links

Classifications

    • 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
    • B01D53/14—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 absorption
    • B01D53/1418—Recovery of products
    • 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
    • B01D53/14—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 absorption
    • B01D53/1425—Regeneration of liquid absorbents
    • 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
    • B01D53/14—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 absorption
    • B01D53/1456—Removing acid components
    • B01D53/1462—Removing mixtures of hydrogen sulfide and carbon dioxide
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B17/00—Sulfur; Compounds thereof
    • C01B17/02—Preparation of sulfur; Purification
    • C01B17/04—Preparation of sulfur; Purification from gaseous sulfur compounds including gaseous sulfides
    • C01B17/0404—Preparation of sulfur; Purification from gaseous sulfur compounds including gaseous sulfides by processes comprising a dry catalytic conversion of hydrogen sulfide-containing gases, e.g. the Claus process
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B17/00—Sulfur; Compounds thereof
    • C01B17/02—Preparation of sulfur; Purification
    • C01B17/04—Preparation of sulfur; Purification from gaseous sulfur compounds including gaseous sulfides
    • C01B17/0404—Preparation of sulfur; Purification from gaseous sulfur compounds including gaseous sulfides by processes comprising a dry catalytic conversion of hydrogen sulfide-containing gases, e.g. the Claus process
    • C01B17/0408—Pretreatment of the hydrogen sulfide containing gases
    • 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
    • B01D2257/304—Hydrogen sulfide
    • 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
    • B01D2257/306—Organic sulfur compounds, e.g. mercaptans
    • 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
    • B01D2257/308—Carbonoxysulfide COS
    • 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
    • B01D53/77—Liquid phase processes
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02C—CAPTURE, STORAGE, SEQUESTRATION OR DISPOSAL OF GREENHOUSE GASES [GHG]
    • Y02C20/00—Capture or disposal of greenhouse gases
    • Y02C20/40—Capture or disposal of greenhouse gases of CO2
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P20/00—Technologies relating to chemical industry
    • Y02P20/10—Process efficiency
    • Y02P20/133—Renewable energy sources, e.g. sunlight
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P20/00—Technologies relating to chemical industry
    • Y02P20/151—Reduction of greenhouse gas [GHG] emissions, e.g. CO2

Definitions

  • the invention relates to a method for processing a technical component of carbon dioxide-rich gas to be purified from sulfur components, in which a technical component of sulfur components to be purified technical gas is purified by a gas scrubber, and the loaded solvent is freed by a regeneration of carbon dioxide and hydrogen sulfide, said at least one acid gas fraction is obtained, which has a higher content of sulfur components, and the fraction with the highest hydrogen sulfide (H 2 S) content is fed to a Claus plant followed by Claus process gas hydrogenation, and at least one carbon dioxide laden, low-sulfur acid sour gas fraction from the Regeneration device, which compared to the fraction with the highest hydrogen sulfide (H 2 S) content has a reduced sulfur content, is brought together with the hydrogenated Claus process gas to a common process gas stream, the further processing or a he is fed back into the process.
  • a technical component of sulfur components to be purified technical gas is purified by a gas scrubber, and the loaded solvent is freed by a regeneration of carbon dioxide
  • H 2 S hydrogen sulfide
  • COS carbonyl sulfide
  • HN hydrogen cyanide
  • Suitable acid gas absorbing solvents are, for example, propylene carbonate, N-methylpyrrolidone, alkylated polyethylene glycol ethers and methanol.
  • Chemically absorbing solvents can also be used, but they have only a low absorption capacity for organic sulfur compounds. Examples of chemically absorbing solvents are ethanolamines or alkali salt solutions.
  • acid gases are usually fed to a Claus plant in which a partial flow of the separated hydrogen sulfide to Sulfur dioxide is burned and this is then converted according to the Claus reaction with the residual stream of hydrogen sulfide to sulfur.
  • the sulfur can be used in many different ways.
  • the technical gases to be cleaned often contain in addition to the sulfur components, such as hydrogen sulfide (H 2 S), carbon dioxide (COS), mercaptans and higher levels of carbon dioxide (C0 2 ).
  • High levels of carbon dioxide arise, for example, in synthesis gas processes, in which the carbon monoxide formed in the synthesis gas production is converted by a CO conversion into carbon dioxide, so that these technical gases often contain large amounts of carbon dioxide.
  • the proportion of carbon dioxide can be up to 50% by volume (% by volume) in the converted synthesis gas.
  • the content of sulfur components in the converted synthesis gas can be very low, depending on the starting material for synthesis gas production, with levels below 0.1 vol .-% are possible.
  • DE 10332427 A1 teaches a process for the removal of hydrogen sulfide and other sour gas components from under pressure technical gases by means of a physical detergent and the recovery of sulfur from hydrogen sulfide using a Claus plant.
  • the technical gases to be purified are freed in the process by gas scrubbing with suitable absorbent solvents from the acid gases contained therein and the loaded absorbent fed to a regeneration.
  • the gas scrubbing is carried out in several stages, wherein the individual regeneration stages have pressure levels which are different from each other and also lower pressure relative to the absorption, so that an acid gas enriched in sulfur components is obtained. This gives various fractions of sour gas, which may also differ in the content of sour gas and the type of sour gases.
  • a hydrogenation is carried out behind the actual Claus process, is hydrogenated by the sulfur dioxide present in the process and converted into hydrogen sulfide.
  • This hydrogenation is usually a necessary process step to prepare the Claus process gas for the so-called Claus process gas treatment.
  • a gas scrubbing whether physically or chemically, it can not be avoided that in addition to the sulfur components, which must be removed from the synthesis gas, and a significant proportion of the carbon dioxide to be cleaned in the scrubbed gas is washed out of the feed gas, so that the acid gases released again in the regeneration device of the gas scrub often consist to a large extent of carbon dioxide.
  • the invention solves this problem by a method in which, on the one hand, only the hydrogen sulfide-rich sour gas fraction is fed into a Claus plant and the still contained in the Claus plant leaving Claus residual sulfur compounds contained by subsequent hydrogenation almost completely to hydrogen sulfide (H 2 S) are hydrogenated, so that a hydrogenated Claus residual gas is obtained, and on the other hand, at least one of the carbon dioxide-rich, low-sulfur sour gas fractions from the regeneration device, which compared to the fraction with the highest hydrogen sulfide (H 2 S) content a reduced Have sulfur content, with the hydrogenated Claus process gas to a common process gas stream is brought together, which is fed to a further processing or a return to the process.
  • the further processing of the merged fractions can be arbitrary.
  • At least one carbon dioxide laden, low-sulfur acid sour gas fraction from the regeneration device, which compared to the fraction with the highest hydrogen sulfide (H 2 S) content has a reduced sulfur content is merged with the hydrogenated Claus process gas to a common process gas stream, which further processing or returned to the process.
  • the number of carbon dioxide-laden, low-hydrogen sulfide fractions from the regeneration device, which compared to the fraction with the highest hydrogen sulfide (H 2 S) content have a reduced sulfur content can be arbitrary in principle.
  • the hydrogenated Claus process gas can be supplied.
  • at least one sour gas fraction from the regeneration device which has a reduced sulfur content compared to the fraction with the highest hydrogen sulfide (H 2 S) content, must be combined with the hydrogenated Claus process gas to form a common process gas stream which is subject to further processing or recycling the process is fed.
  • the separation is carried out in at least two sour gas fractions in that the laden with acid gas from the gas scrubber before being fed into a regeneration column is first led to carbon dioxide depletion in at least one Austriebscut in which a carbon dioxide rich sour gas fraction and a with the in the regeneration column, a further depleted in carbon dioxide and enriched in sulfur components sour gas fraction is obtained, which is performed for combustion with an oxygen-containing gas in the Claus burner.
  • the depletion of the loaded solvent to carbon dioxide is preferably carried out in two to four flash stages, which are upstream of the regeneration column in the flow direction made. However, any number of flash stages can be used.
  • the process of absorption, expansion in the flash stage, and regeneration may be arbitrary and is known in the art.
  • the amount of sulfur components in the sulfur component-enriched substream supplied to the burner of the Claus reactor is typically 20 to 40 percent of the total sulfur removed from the feed gas.
  • the recombined from the Claus residual gas and the carbon dioxide laden, low-sulfur sour gas residual gas stream is returned by means of a compressor for gas recirculation in the absorption column located in the main gas flow. This will do that Returned carbon dioxide in the first absorption column and finally carried out with the product gas from the process.
  • the hydrogen sulfide (H 2 S) still present in the combined process gas stream is passed into at least one further gas scrubber with an absorption column, so that a virtually sulfur-free Claus residual gas is obtained.
  • the solvent used for the absorption is preferred in at least one sour gas scrubbing a physical solvent with a high selectivity for sulfur components, in particular hydrogen sulfide (H 2 S), compared to carbon dioxide (C0 2 ).
  • suitable physical solvents are Morphysorb ® (mixture containing N-formylmorpholine and N-acetylmorpholine), Selexol ® (mixture containing dimethyl ether of polyethylene glycols), N-methylpyrrolidone (NMP), methanol or propylene carbonate. This can be used in at least one of the absorption columns for gas scrubbing or hydrogenation subsequent absorption columns, or for several or ultimately for all absorption columns.
  • a selectively acting chemical solvent which is suitable for a selective removal of sulfur components to carbon dioxide (C0 2 ), in aqueous solution.
  • chemical solvents include methyldiethanolamine (MDEA), Flexsorb ® (mixture containing hindered amines), or alkali metal salt solutions (for example potash solutions).
  • MDEA methyldiethanolamine
  • Flexsorb ® mixture containing hindered amines
  • alkali metal salt solutions for example potash solutions
  • the carbon dioxide content of the technical gas to be purified may be arbitrary.
  • the content of carbon dioxide in the feed gas may be 30 to 50% by volume.
  • the application of the method according to the invention is particularly advantageous when the sulfur component content is small compared to the carbon dioxide content.
  • gases can be purified whose content of sulfur components at 0.1 to 1 volume percent hydrogen sulfide (or molar equivalent).
  • the technical gas to be purified may also contain ammonia.
  • the technical gas for desulfurization to be purified may be, for example, synthesis gas from a CO conversion. At the zu Purification technical gas for desulfurization may also be, for example, natural gas.
  • the number of sour gas fractions into which the sour gas released in the regeneration, consisting of sulfur components and carbon dioxide (C0 2 ), is separated can be arbitrary.
  • the fraction with the highest hydrogen sulfide (H 2 S) content is fed to the Claus burner of a Claus plant, so that the number of fractions, compared to the fraction with the highest hydrogen sulfide (H 2 S) content a have reduced sulfur content, may also be arbitrary.
  • These can in principle all be combined with the hydrogenated Claus residual gas and fed to a use which does not lie in the region of the Claus plant.
  • the number of selected fractions, which are used in a non-Claus plant, can ultimately be arbitrary.
  • the further use can in principle be of any kind.
  • a further embodiment of the invention is behind the hydrogenation and the merger of the hydrogenated Claus residual gas with the low-sulfur, carbon dioxide-rich fraction, another gas scrubbing, so that one obtains a desulfurized Claus process gas or Claus residual gas, which led by way of example in an afterburning becomes.
  • S0 2 sulfur dioxide
  • an additional fuel gas can be used.
  • For use in the further process flow is an example of processing of the combined fractions by means of an additional Claus plant and downstream of the Claus plant hydrogenation.
  • the invention has the advantage that acid gas fractions with a reduced content of hydrogen sulfide need not be fed into the Claus burner a Claus plant or reaction chamber of a Claus plant, but combined with the residual gas of a Claus plant and fed to further use can be. This contributes accordingly to an improved economy of the entire process.
  • the device of the invention will be explained with reference to two drawings, these drawings are only exemplary embodiments of the construction of the device according to the invention.
  • FIG. 1 shows an embodiment according to the invention in which hydrogenated Claus residual gas from a Claus process is combined with the carbon dioxide-rich sour gas fraction from a gas scrubber and the combined gas stream is returned to the gas scrubbing process.
  • FIG. Figure 2 shows an embodiment of the invention in which the hydrogenated Claus residual gas is combined with the carbon dioxide-rich sour gas fraction from a gas scrubber and the combined gas stream is re-gas scrubbed with post-combustion.
  • FIG. 1 shows a process flow according to the invention in which a feed gas (1a) to be cleaned is fed to a gas scrubber (2).
  • a sulfur-containing feed gas (1a) is passed to a absorption column (2) for gas scrubbing in which it is brought into contact with an absorbent solvent cooled by a heat exchanger (2a).
  • the loaded solvent is inventively preheated by heat exchangers (4a, 4b), and in a Austriebs inherenter (5) out.
  • a carbon dioxide-laden, low-sulfur acid sour gas fraction (6) and a carbon dioxide-depleted laden with sulfur components loaded solvent (7) This is passed into a regeneration column (8), which is heated here by way of example with a reboiler (8a), and freed from the sour gas enriched in sulfur components by heating and venting. This gives a carbon dioxide depleted, enriched with sulfur components sour gas (9), and a regenerated solvent (10).
  • the sour gas (9) is passed through a condenser (9a) in a Claus plant (11). Condensed vapors (9b) are recycled to the regeneration column (8).
  • the carbon dioxide laden, low sulfur acid sour gas fraction (6) coming from the flash tank (5) has a lower
  • This Claus process gas (12) is passed into a hydrogenation stage (13) in which the remaining sulfur compounds in the Claus process gas (12) are hydrogenated with hydrogen (13a, H 2 ) to hydrogen sulfide (H 2 S).
  • the hydrogenated Claus process gas (14) is combined via a valve (6a) with the carbon dioxide-laden, low-sulfur sour gas (6) and via a compressor for the gas recirculation (14a) and a heat exchanger (14b) in the feed gas (1a) and thus in returned the process.
  • the carbon dioxide (C0 2 ) is discharged from the process with the product gas (1b).
  • FIG. 2 shows an embodiment according to the invention in which the hydrogenated Claus residual gas (14) is combined with the carbon dioxide-rich sour gas fraction (12) from a gas scrubber (2) and fed to a further gas scrubber (15) with an afterburning (16).
  • the feed gas (1 a) to be purified is first freed of sulfur compounds by gas scrubbing (2) with subsequent regeneration (6,9), whereby a carbon dioxide-laden, low-sulfur sour gas (6) and a carbon dioxide-depleted, enriched with hydrogen sulfide Sour gas (9) can be obtained.
  • the enriched in carbon dioxide, enriched with hydrogen sulfide acid gas (9) is passed into a Claus process (11) in which the carbon dioxide depleted enriched with hydrogen sulfide acid gas (9) by partial combustion to sulfur dioxide (S0 2 ) and its subsequent post-reaction is converted with the remaining hydrogen sulfide (H 2 S) into sulfur (11b, S), which is discharged and reused.
  • the Claus process gas (12) obtained from the Claus process (11) contains the remaining sulfur mainly as sulfur dioxide (S0 2 ).
  • This Claus process gas (12) is passed into a hydrogenation stage (13) in which the remaining sulfur compounds in the Claus process gas (12) are hydrogenated with hydrogen (13a) to hydrogen sulfide (H 2 S).
  • a hydrogenated Claus process gas (14) is obtained which, according to the invention, is combined with the carbon dioxide-laden, low-sulfur sour gas (6) and is passed through a gas scrubber (15) with a subsequent regeneration device (16).
  • the sour gas (15e) depleted in sulfur compounds from the additional gas scrubber (15) is passed to afterburning (17) in which the remaining sulfur compounds are burned with an oxygen-containing gas (17a) and optionally with a fuel gas (17b) and the exhaust gas (18 ) is conducted into the atmosphere.
  • the hydrogen sulfide-rich Claus residual gas (19) from the regeneration device (16) is recycled to the carbon dioxide-depleted hydrogen sulfide enriched sour gas (9) prior to the Claus process (11).
EP11712170A 2010-03-29 2011-03-22 Verfahren zur verarbeitung eines von schwefelkomponenten zu reinigenden kohlendioxidreichen gases Ceased EP2552569A1 (de)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
DE102010013279A DE102010013279B3 (de) 2010-03-29 2010-03-29 Verfahren und Vorrichtung zur Verarbeitung eines kohlendioxidreichen Sauergases in einem Claus-Prozess
PCT/EP2011/001397 WO2011120647A1 (de) 2010-03-29 2011-03-22 Verfahren zur verarbeitung eines von schwefelkomponenten zu reinigenden kohlendioxidreichen gases

Publications (1)

Publication Number Publication Date
EP2552569A1 true EP2552569A1 (de) 2013-02-06

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Family Applications (2)

Application Number Title Priority Date Filing Date
EP11712170A Ceased EP2552569A1 (de) 2010-03-29 2011-03-22 Verfahren zur verarbeitung eines von schwefelkomponenten zu reinigenden kohlendioxidreichen gases
EP11724531.6A Active EP2552570B1 (de) 2010-03-29 2011-03-22 Verfahren und vorrichtung zur verarbeitung eines kohlendioxidreichen sauergases in einem claus-prozess

Family Applications After (1)

Application Number Title Priority Date Filing Date
EP11724531.6A Active EP2552570B1 (de) 2010-03-29 2011-03-22 Verfahren und vorrichtung zur verarbeitung eines kohlendioxidreichen sauergases in einem claus-prozess

Country Status (12)

Country Link
US (2) US8568676B2 (pt)
EP (2) EP2552569A1 (pt)
KR (2) KR20130057975A (pt)
CN (2) CN102821830B (pt)
AU (2) AU2011234876A1 (pt)
BR (2) BR112012024493A2 (pt)
CA (2) CA2792812A1 (pt)
DE (1) DE102010013279B3 (pt)
RU (2) RU2545273C2 (pt)
TW (2) TW201210930A (pt)
WO (2) WO2011120647A1 (pt)
ZA (1) ZA201207560B (pt)

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