EP2231828A2 - Autothermes verfahren zur kontinuierlichen vergasung von kohlenstoffreichen substanzen - Google Patents
Autothermes verfahren zur kontinuierlichen vergasung von kohlenstoffreichen substanzenInfo
- Publication number
- EP2231828A2 EP2231828A2 EP08864268A EP08864268A EP2231828A2 EP 2231828 A2 EP2231828 A2 EP 2231828A2 EP 08864268 A EP08864268 A EP 08864268A EP 08864268 A EP08864268 A EP 08864268A EP 2231828 A2 EP2231828 A2 EP 2231828A2
- Authority
- EP
- European Patent Office
- Prior art keywords
- zone
- bulk material
- gas
- carbon
- substances
- 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.)
- Withdrawn
Links
- 238000000034 method Methods 0.000 title claims abstract description 104
- 229910052799 carbon Inorganic materials 0.000 title claims abstract description 55
- 239000000126 substance Substances 0.000 title claims abstract description 55
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 title claims abstract description 53
- 238000002309 gasification Methods 0.000 title claims abstract description 39
- 239000007789 gas Substances 0.000 claims abstract description 132
- 230000003647 oxidation Effects 0.000 claims abstract description 44
- 238000007254 oxidation reaction Methods 0.000 claims abstract description 44
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims abstract description 26
- 239000001301 oxygen Substances 0.000 claims abstract description 26
- 229910052760 oxygen Inorganic materials 0.000 claims abstract description 26
- 238000001816 cooling Methods 0.000 claims abstract description 17
- 238000001354 calcination Methods 0.000 claims abstract description 11
- 239000000047 product Substances 0.000 claims abstract description 10
- 239000007795 chemical reaction product Substances 0.000 claims abstract description 7
- 230000000630 rising effect Effects 0.000 claims abstract description 3
- 239000013590 bulk material Substances 0.000 claims description 71
- 230000008569 process Effects 0.000 claims description 61
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 30
- 239000000203 mixture Substances 0.000 claims description 22
- 239000000428 dust Substances 0.000 claims description 17
- 239000003575 carbonaceous material Substances 0.000 claims description 13
- 238000006243 chemical reaction Methods 0.000 claims description 13
- 239000000463 material Substances 0.000 claims description 12
- 239000002245 particle Substances 0.000 claims description 12
- 238000001035 drying Methods 0.000 claims description 11
- 238000010438 heat treatment Methods 0.000 claims description 9
- 239000004033 plastic Substances 0.000 claims description 9
- 229920003023 plastic Polymers 0.000 claims description 9
- 230000001174 ascending effect Effects 0.000 claims description 8
- 239000002956 ash Substances 0.000 claims description 8
- 238000002485 combustion reaction Methods 0.000 claims description 8
- 239000003921 oil Substances 0.000 claims description 7
- 238000011084 recovery Methods 0.000 claims description 7
- 239000000446 fuel Substances 0.000 claims description 6
- 238000004064 recycling Methods 0.000 claims description 6
- 239000010881 fly ash Substances 0.000 claims description 5
- 239000002918 waste heat Substances 0.000 claims description 5
- 239000010426 asphalt Substances 0.000 claims description 3
- 229910052500 inorganic mineral Inorganic materials 0.000 claims description 3
- 239000011707 mineral Substances 0.000 claims description 3
- 239000002689 soil Substances 0.000 claims description 3
- 239000000919 ceramic Substances 0.000 claims description 2
- 239000007769 metal material Substances 0.000 claims description 2
- 239000002243 precursor Substances 0.000 claims description 2
- 239000002920 hazardous waste Substances 0.000 claims 2
- 238000001704 evaporation Methods 0.000 claims 1
- 230000008020 evaporation Effects 0.000 claims 1
- 230000005484 gravity Effects 0.000 claims 1
- 230000001737 promoting effect Effects 0.000 claims 1
- 239000002023 wood Substances 0.000 claims 1
- 230000015572 biosynthetic process Effects 0.000 description 27
- 238000003786 synthesis reaction Methods 0.000 description 19
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 8
- 229910002091 carbon monoxide Inorganic materials 0.000 description 7
- 229910052739 hydrogen Inorganic materials 0.000 description 7
- 239000004071 soot Substances 0.000 description 7
- 238000001914 filtration Methods 0.000 description 6
- 238000010304 firing Methods 0.000 description 6
- 229910001385 heavy metal Inorganic materials 0.000 description 6
- 150000002430 hydrocarbons Chemical class 0.000 description 6
- 239000002609 medium Substances 0.000 description 6
- 235000008733 Citrus aurantifolia Nutrition 0.000 description 5
- 235000019738 Limestone Nutrition 0.000 description 5
- 235000011941 Tilia x europaea Nutrition 0.000 description 5
- 239000000969 carrier Substances 0.000 description 5
- 239000003245 coal Substances 0.000 description 5
- 238000007872 degassing Methods 0.000 description 5
- 239000004571 lime Substances 0.000 description 5
- 239000006028 limestone Substances 0.000 description 5
- 230000008901 benefit Effects 0.000 description 4
- 239000000460 chlorine Substances 0.000 description 4
- 230000004992 fission Effects 0.000 description 4
- 239000003546 flue gas Substances 0.000 description 4
- 229930195733 hydrocarbon Natural products 0.000 description 4
- 239000001257 hydrogen Substances 0.000 description 4
- 238000010248 power generation Methods 0.000 description 4
- 239000000376 reactant Substances 0.000 description 4
- 238000000926 separation method Methods 0.000 description 4
- 239000006163 transport media Substances 0.000 description 4
- 239000002699 waste material Substances 0.000 description 4
- 239000002028 Biomass Substances 0.000 description 3
- ZAMOUSCENKQFHK-UHFFFAOYSA-N Chlorine atom Chemical compound [Cl] ZAMOUSCENKQFHK-UHFFFAOYSA-N 0.000 description 3
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 3
- 229910052801 chlorine Inorganic materials 0.000 description 3
- 238000011109 contamination Methods 0.000 description 3
- 238000005516 engineering process Methods 0.000 description 3
- 239000003344 environmental pollutant Substances 0.000 description 3
- 229910052736 halogen Inorganic materials 0.000 description 3
- 150000002367 halogens Chemical class 0.000 description 3
- 238000004519 manufacturing process Methods 0.000 description 3
- 238000002156 mixing Methods 0.000 description 3
- 231100000719 pollutant Toxicity 0.000 description 3
- 238000001179 sorption measurement Methods 0.000 description 3
- 238000012546 transfer Methods 0.000 description 3
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 2
- VEXZGXHMUGYJMC-UHFFFAOYSA-N Hydrochloric acid Chemical compound Cl VEXZGXHMUGYJMC-UHFFFAOYSA-N 0.000 description 2
- 238000005299 abrasion Methods 0.000 description 2
- 150000001721 carbon Chemical class 0.000 description 2
- 150000001722 carbon compounds Chemical class 0.000 description 2
- 238000004140 cleaning Methods 0.000 description 2
- 238000003776 cleavage reaction Methods 0.000 description 2
- 238000005260 corrosion Methods 0.000 description 2
- 230000007797 corrosion Effects 0.000 description 2
- 238000000354 decomposition reaction Methods 0.000 description 2
- 150000002013 dioxins Chemical class 0.000 description 2
- 239000013505 freshwater Substances 0.000 description 2
- 239000002737 fuel gas Substances 0.000 description 2
- 150000002240 furans Chemical class 0.000 description 2
- IXCSERBJSXMMFS-UHFFFAOYSA-N hydrogen chloride Substances Cl.Cl IXCSERBJSXMMFS-UHFFFAOYSA-N 0.000 description 2
- 229910000041 hydrogen chloride Inorganic materials 0.000 description 2
- 238000002844 melting Methods 0.000 description 2
- 230000008018 melting Effects 0.000 description 2
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 2
- 150000002894 organic compounds Chemical class 0.000 description 2
- 229920000642 polymer Polymers 0.000 description 2
- 238000010791 quenching Methods 0.000 description 2
- 230000007017 scission Effects 0.000 description 2
- 238000012216 screening Methods 0.000 description 2
- 238000007789 sealing Methods 0.000 description 2
- 239000007858 starting material Substances 0.000 description 2
- 241000093804 Berzelia galpinii Species 0.000 description 1
- 239000005997 Calcium carbide Substances 0.000 description 1
- 239000004215 Carbon black (E152) Substances 0.000 description 1
- 241000196324 Embryophyta Species 0.000 description 1
- 229910000604 Ferrochrome Inorganic materials 0.000 description 1
- 229910000519 Ferrosilicon Inorganic materials 0.000 description 1
- PXGOKWXKJXAPGV-UHFFFAOYSA-N Fluorine Chemical compound FF PXGOKWXKJXAPGV-UHFFFAOYSA-N 0.000 description 1
- 238000009825 accumulation Methods 0.000 description 1
- 230000009471 action Effects 0.000 description 1
- 238000004458 analytical method Methods 0.000 description 1
- RHZUVFJBSILHOK-UHFFFAOYSA-N anthracen-1-ylmethanolate Chemical compound C1=CC=C2C=C3C(C[O-])=CC=CC3=CC2=C1 RHZUVFJBSILHOK-UHFFFAOYSA-N 0.000 description 1
- 239000003830 anthracite Substances 0.000 description 1
- 230000006399 behavior Effects 0.000 description 1
- 239000006227 byproduct Substances 0.000 description 1
- 230000008859 change Effects 0.000 description 1
- 150000001805 chlorine compounds Chemical class 0.000 description 1
- 239000000571 coke Substances 0.000 description 1
- 150000001875 compounds Chemical class 0.000 description 1
- 230000003750 conditioning effect Effects 0.000 description 1
- 238000010276 construction Methods 0.000 description 1
- 239000000356 contaminant Substances 0.000 description 1
- 238000011161 development Methods 0.000 description 1
- 239000003814 drug Substances 0.000 description 1
- 229940079593 drug Drugs 0.000 description 1
- 230000008030 elimination Effects 0.000 description 1
- 238000003379 elimination reaction Methods 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 230000002349 favourable effect Effects 0.000 description 1
- 238000011049 filling Methods 0.000 description 1
- 239000010419 fine particle Substances 0.000 description 1
- 230000024703 flight behavior Effects 0.000 description 1
- 239000011737 fluorine Substances 0.000 description 1
- 229910052731 fluorine Inorganic materials 0.000 description 1
- 150000002222 fluorine compounds Chemical class 0.000 description 1
- 239000000295 fuel oil Substances 0.000 description 1
- 238000005469 granulation Methods 0.000 description 1
- 230000003179 granulation Effects 0.000 description 1
- 150000004820 halides Chemical class 0.000 description 1
- 239000010763 heavy fuel oil Substances 0.000 description 1
- 150000002431 hydrogen Chemical class 0.000 description 1
- 239000000543 intermediate Substances 0.000 description 1
- 239000013067 intermediate product Substances 0.000 description 1
- 238000005259 measurement Methods 0.000 description 1
- 150000001247 metal acetylides Chemical group 0.000 description 1
- 238000013508 migration Methods 0.000 description 1
- 230000005012 migration Effects 0.000 description 1
- 239000003345 natural gas Substances 0.000 description 1
- 238000006386 neutralization reaction Methods 0.000 description 1
- 229910052757 nitrogen Inorganic materials 0.000 description 1
- 239000011368 organic material Substances 0.000 description 1
- 238000013021 overheating Methods 0.000 description 1
- 230000001590 oxidative effect Effects 0.000 description 1
- 239000002006 petroleum coke Substances 0.000 description 1
- 231100000614 poison Toxicity 0.000 description 1
- 230000002265 prevention Effects 0.000 description 1
- 238000000197 pyrolysis Methods 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
- 238000010008 shearing Methods 0.000 description 1
- 238000005245 sintering Methods 0.000 description 1
- 238000001228 spectrum Methods 0.000 description 1
- 230000003068 static effect Effects 0.000 description 1
- 239000004575 stone Substances 0.000 description 1
- 239000008400 supply water Substances 0.000 description 1
- 230000002194 synthesizing effect Effects 0.000 description 1
- CLZWAWBPWVRRGI-UHFFFAOYSA-N tert-butyl 2-[2-[2-[2-[bis[2-[(2-methylpropan-2-yl)oxy]-2-oxoethyl]amino]-5-bromophenoxy]ethoxy]-4-methyl-n-[2-[(2-methylpropan-2-yl)oxy]-2-oxoethyl]anilino]acetate Chemical compound CC1=CC=C(N(CC(=O)OC(C)(C)C)CC(=O)OC(C)(C)C)C(OCCOC=2C(=CC=C(Br)C=2)N(CC(=O)OC(C)(C)C)CC(=O)OC(C)(C)C)=C1 CLZWAWBPWVRRGI-UHFFFAOYSA-N 0.000 description 1
- 239000003440 toxic substance Substances 0.000 description 1
Classifications
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
- C10J3/00—Production of combustible gases containing carbon monoxide from solid carbonaceous fuels
- C10J3/02—Fixed-bed gasification of lump fuel
- C10J3/20—Apparatus; Plants
- C10J3/22—Arrangements or dispositions of valves or flues
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
- C10J3/00—Production of combustible gases containing carbon monoxide from solid carbonaceous fuels
- C10J3/58—Production of combustible gases containing carbon monoxide from solid carbonaceous fuels combined with pre-distillation of the fuel
- C10J3/60—Processes
- C10J3/64—Processes with decomposition of the distillation products
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
- C10J3/00—Production of combustible gases containing carbon monoxide from solid carbonaceous fuels
- C10J3/72—Other features
- C10J3/721—Multistage gasification, e.g. plural parallel or serial gasification stages
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
- C10J2200/00—Details of gasification apparatus
- C10J2200/15—Details of feeding means
- C10J2200/152—Nozzles or lances for introducing gas, liquids or suspensions
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
- C10J2300/00—Details of gasification processes
- C10J2300/09—Details of the feed, e.g. feeding of spent catalyst, inert gas or halogens
- C10J2300/0913—Carbonaceous raw material
- C10J2300/093—Coal
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
- C10J2300/00—Details of gasification processes
- C10J2300/09—Details of the feed, e.g. feeding of spent catalyst, inert gas or halogens
- C10J2300/0913—Carbonaceous raw material
- C10J2300/0946—Waste, e.g. MSW, tires, glass, tar sand, peat, paper, lignite, oil shale
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
- C10J2300/00—Details of gasification processes
- C10J2300/09—Details of the feed, e.g. feeding of spent catalyst, inert gas or halogens
- C10J2300/0953—Gasifying agents
- C10J2300/0956—Air or oxygen enriched air
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
- C10J2300/00—Details of gasification processes
- C10J2300/09—Details of the feed, e.g. feeding of spent catalyst, inert gas or halogens
- C10J2300/0953—Gasifying agents
- C10J2300/0959—Oxygen
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
- C10J2300/00—Details of gasification processes
- C10J2300/09—Details of the feed, e.g. feeding of spent catalyst, inert gas or halogens
- C10J2300/0953—Gasifying agents
- C10J2300/0973—Water
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
- C10J2300/00—Details of gasification processes
- C10J2300/09—Details of the feed, e.g. feeding of spent catalyst, inert gas or halogens
- C10J2300/0983—Additives
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
- C10J2300/00—Details of gasification processes
- C10J2300/09—Details of the feed, e.g. feeding of spent catalyst, inert gas or halogens
- C10J2300/0983—Additives
- C10J2300/0993—Inert particles, e.g. as heat exchange medium in a fluidized or moving bed, heat carriers, sand
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
- C10J2300/00—Details of gasification processes
- C10J2300/09—Details of the feed, e.g. feeding of spent catalyst, inert gas or halogens
- C10J2300/0983—Additives
- C10J2300/0996—Calcium-containing inorganic materials, e.g. lime
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
- C10J2300/00—Details of gasification processes
- C10J2300/16—Integration of gasification processes with another plant or parts within the plant
- C10J2300/1671—Integration of gasification processes with another plant or parts within the plant with the production of electricity
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
- C10J2300/00—Details of gasification processes
- C10J2300/16—Integration of gasification processes with another plant or parts within the plant
- C10J2300/1671—Integration of gasification processes with another plant or parts within the plant with the production of electricity
- C10J2300/1675—Integration of gasification processes with another plant or parts within the plant with the production of electricity making use of a steam turbine
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- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
- C10J2300/00—Details of gasification processes
- C10J2300/16—Integration of gasification processes with another plant or parts within the plant
- C10J2300/1687—Integration of gasification processes with another plant or parts within the plant with steam generation
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- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
- C10J2300/00—Details of gasification processes
- C10J2300/16—Integration of gasification processes with another plant or parts within the plant
- C10J2300/1693—Integration of gasification processes with another plant or parts within the plant with storage facilities for intermediate, feed and/or product
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
- C10J2300/00—Details of gasification processes
- C10J2300/18—Details of the gasification process, e.g. loops, autothermal operation
- C10J2300/1807—Recycle loops, e.g. gas, solids, heating medium, water
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- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
- C10J2300/00—Details of gasification processes
- C10J2300/18—Details of the gasification process, e.g. loops, autothermal operation
- C10J2300/1838—Autothermal gasification by injection of oxygen or steam
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- 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
- Y02P20/129—Energy recovery, e.g. by cogeneration, H2recovery or pressure recovery turbines
Definitions
- the present invention relates to an autothermal process for the continuous gasification of carbonaceous substances in a vertical process space with a calcination zone and an oxidation zone in which the calcined carbonaceous substances oxidize with oxygen-containing gas, wherein the gaseous reaction products are withdrawn at the top of the vertical reaction space, the vertical process space is formed in the form of a vertical shaft furnace, which is continuously flowed through from top to bottom by a circulated bulk material, which itself is not oxidized, and the carbon-rich substances are added to the bulk material before entering the furnace.
- Such methods have been known for a long time and are carried out, for example, in countercurrent gasifiers in which coal products or even biomass, which is moved to the bottom of the carburetor, is flowed around in countercurrent to the resulting process gases.
- the resulting process gases can be burned immediately or used for synthesizing processes.
- a disadvantage of the method described is that it can be carried out autothermally by the supplied carbon-rich substances, but the process gases depend to a large extent on the respectively supplied carbon-rich substances and accordingly the process is difficult to control. Completely unsuitable is the method for contaminated carbon-rich substances such. As fluorine and chlorine-containing plastics, contaminated waste, drugs or the like.
- the method of the type mentioned in principle is also used for coal gasification, wherein the use of coal usually the expression of a calcination zone can be omitted.
- autothermal gasification processes which supply carbon monoxide-rich gases whose hydrogen content is determined by the hydrogen content of the carbon carriers used and, if appropriate, by the metered addition of water into the gasification process and is optionally adjustable.
- the heat energy required for the gasification is obtained from the partial oxidation of the raw materials used.
- the object of the present invention is to improve a method of the type mentioned in that it reacts insensitive to the use of different qualities of the carbon-rich substances, without increasing the cost considerably.
- the object is achieved by a method of the type mentioned, in which the oxygen-containing gas is at least partially introduced below the oxidation zone, whereby the ascending gas flow is promoted, below the oxidation zone by the rising gases, the bulk material and ash products in a heat recovery zone to cooled to 450 0 C and further the oxygen-containing gas is at least partially introduced at the lower end of the vertical shaft furnace and in a Nachkühl- zone below the heat recovery zone in countercurrent, the bulk material before removal from the furnace for energy recycling up to a temperature of below 100 0 C is cooled.
- the carbon-rich substances can be autothermally gasified, without any special requirements would exist on the quality of the used carbonaceous substances. It is only to be noted that the amount of carbonaceous substances supplied is sufficient to maintain the autothermal equilibrium in the vertical shaft furnace. It has been shown that the carbon-rich substances with edge lengths of up to 40 cm can be added without hampering the process.
- the bulk material which on the one hand assumes the function of a heat transfer medium. Furthermore, it acts as a transport medium that promotes the carbon-rich substances into the oxidation zone to their final gasification and then promotes the gasification residues as ash to exit at the bottom of the vertical shaft furnace. It is of further importance that a bulk material is permeable to gas, and in this way allows the ascending gas flow, resulting in a heat exchange between the bulk material as the heat transfer medium and the ascending gas flow in the individual reaction zones.
- the bulk material flow is cooled in a waste heat zone by direct cooling with oxygen-containing gas to a self-temperature of about 450 0 C, wherein in the event that the method This is preferably done in the region of the waste heat zone, wherein the resulting water vapor rises and participates in the synthesis gas reaction in the region of the oxidation zone.
- the oxygen-containing gas is at least partially supplied to the lower end of the vertical shaft furnace, so that in a Nachkühlzone below the waste heat zone in countercurrent of the bulk material before removal from the furnace until is cooled to a temperature of below 100 0 C.
- a Nachkühlzone below the waste heat zone in countercurrent of the bulk material before removal from the furnace until is cooled to a temperature of below 100 0 C.
- the grain size should preferably not be greater than 20 cm and more preferably in a range between 1 and 8 cm.
- the granulation of the bulk material prevents sticking or caking of plastic substances by mechanical shearing, so that complete gasification of all supplied carbonaceous substances in the oxidation zone is achieved.
- At least partially mineral, ceramic or metallic material with the aforementioned grain size and / or mineral calcinates such as.
- CaO used, but also precursors of calcine, such as. B. limestone.
- CaO has the advantage that it is also suitable for binding halogens contained in the substance streams, which are mixed with the KaI- react and occur as harmless chlorides or fluorides.
- the accumulating dust can also be completely or partially recycled into the bulk material cycle.
- the temperature in the oxidation zone is preferably set so low that no complete burning of the limestone occurs, but only a formation of a thin CaO layer on the limestone elements is achieved, so that the ability to bind the halogens is maintained without generating large quantities of CaO.
- Limestone itself has an increased mechanical resistance to CaO.
- Possible heavy metals which enter the process as contamination of the material stream, can generally remain in the circulation of the bulk material, but if they accumulate in the filter dust, partial streams can be removed from the process and disposed of.
- the bulk material flow is increased by means of the ascending Gases in a development of the method o- countercurrently ber endeavour of calcining under heating to a characteristic temperature 20-100 0 C in a drying zone first dried and subsequently by further heating to the ER of the calcining zone rich on a self temperature 100-450 0 C Pre-degassed in a Vorentgasungszone.
- the energy required for drying and pre-degassing is provided by the ascending gas stream which is countercurrently cooled to lower temperatures before being withdrawn at the top of the vertical shaft furnace.
- the flow of bulk material and carbon-rich substances is then heated to an own temperature of up to 1200 ° C.
- the gas produced after being drawn off at the top of the vertical shaft furnace is treated in an air flow after-gasification zone in the presence of water vapor.
- the withdrawn gas consists of a gas mixture of the resulting gas in the oxidation zone, at least CO and H 2 , and gas from the Vorentgasungszone, in addition to gaseous
- Hydrocarbon compounds and soot can be mixed with the gas.
- the resulting gases When using air as the oxidizing gas, the resulting gases also contain a corresponding nitrogen content.
- the soot is due to the fact that in the Vorentgasungszone at a relatively low temperature already uses a decay of the hydrocarbon compounds, but the existing temperatures or residence times are not sufficient to allow complete decomposition into the ideal reaction gases CO, H 2 and hydrocarbon having a chain length less than C 4 .
- the residual air after-gasifier then disassembles the longer-chain hydrocarbons that are still present, so that an ideal synthesis gas of CO, H 2 and hydrocarbons with a chain length smaller C 4 is subsequently obtained as the end product of the process.
- This synthesis gas can be used in a variety of known applications.
- the combustion in a combustion chamber may be mentioned, wherein the resulting hot gas for the drive of hot gas turbines and / or steam turbines for power generation and / or water vapor can be used as a heating medium in thermal processes.
- the synthesis gas can be purified by filtration and / or gas cooling and used as a heating gas in thermal processes, for example, for firing Kalzinierschachtöfen and / or for power generation in gas engines.
- a major advantage is that the synthesis gases can also be generated from biomass and thus the CO ⁇ balance z. B. in lime production can be significantly improved, while in such processes so far only limited biomass with certain properties could be used.
- Purified syngas is also suitable for cleavage into its components by partial liquefaction, and recovery of the pure gas-containing components may also be accomplished by pressure-swing adsorption technology applications.
- the purified synthesis gas or one of its components can also be used wholly or partly for the synthesis of chemical base or intermediates, regardless of which starting material as carbonaceous substance has been initially added to the process.
- the mentioned presence of water vapor in the air stream post-gasification zone is achieved by adding water or steam or by the water vapor escaping in the drying zone.
- the process can be carried out readily at pressures approaching the ambient pressure, whereby a pressure spectrum in the
- Range of -200 mbar to 1000 mbar (ü) has been found to be particularly useful.
- the vacuum can be applied, for example, by a suction device which is also used for removing the gaseous reaction products.
- all process zones are set from drying to aftercooling in a single chamber, so that no transport devices between the zones are necessary.
- material preferably arranged on the top of the vertical shaft furnace water-cooled Schure without fittings and moving parts is used. Additional emission sites, which may be necessary in other processes for conditioning the process as bulk material, reactant or substances involved, are eliminated.
- oxygen-containing gas and / or fuel are added in the oxidation zone. This happens when cheering, d. H. Starting the process, but also to control the location, size and temperature of the individual zones in the vertical shaft furnace. This can prevent individual zones from migrating, the temperature level for the process reaching unfavorable levels, or overheating and dissolving the edge zones, thus disrupting the process. Ideally, fuel addition is not necessary.
- Fig. 1 is a schematic representation of a
- FIG. 2 shows a schematic representation of the vertical shaft furnace from FIG. 1 with downstream utilization of the process gases.
- Fig. 1 shows a schematic representation of a vertical shaft furnace 100, which essentially corresponds in its construction to a calcination shaft furnace, as it is used industrially, for example, in firing or sintering processes. It is used in the implementation of the present method as a gasification reactor.
- the furnace 100 is continuously charged with a mixture of carbon-rich substances and refractory bulk material.
- the operation of the gaseous reactor is adjusted so that the process takes place au tothermically by the oxidation of the carbon-rich substances used, wherein the oxidation can be supported by a base load firing 5, 6, 7, in particular for starting the process.
- the vertical shaft furnace or gasification reactor 100 is controlled such that the gasification proceeds in seven different process zones.
- the carbon-rich substances mixed with the bulk material first pass into a drying zone A, in which they are dried at an inherent temperature of 20 to 100 ° C. They then enter a pre-degassing zone B in which they are at a natural temperature of
- 100 - 500 0 C are freed by degassing of volatile fractions.
- the vorentgasten carbon-rich substances reach under the action of the downwardly moving bulk material, which serves as a heat and transport medium, then in a calcination zone C in which a heating to a natural temperature of up to 1200 0 C takes place before in the subsequent oxidation zone D is gasified by supplying oxygen-containing gas at temperatures below 1,800 0 C any remaining carbon.
- the refractory bulk material is cooled with the ash portions in a heat recovery zone E by direct cooling with oxygen-containing gas and / or optionally by introducing water to produce steam at about 450 0 C, wherein the oxygen-containing gas previously below the Abhitzezone has heated in a post-cooling zone F in countercurrent to the bulk material, on the other hand by the countercurrent to the supplied in the bottom region of the vertical shaft furnace oxygen-containing gas for energy recycling to below 100 0 C is cooled.
- the supply line 8 of the oxygen-containing gas at the bottom of the vertical shaft furnace 100 also represents the beginning of the gaseous countercurrent, which extends through all the process zones described above.
- E is first heated in the aftercooling zone F and the following in the sense of gas moving direction Abhitzezone the oxygen-containing gas to about 450 0 C before it, optionally with further direct supply of oxygen-containing gas in the oxidation zone, the oxidation on the carbon compounds or of the carbon present in pure form accomplished.
- the reaction gases continue to rise upward and ensure the temperature level required in the calcination zone C.
- reaction gases flow through the pre-degassing zone B and with further cooling the drying zone A, wherein the gas after leaving the top of the bulk material column as a gas mixture of the synthesis gas CO and H2 from the oxidation state, water vapor and hydrocarbons, in particular from the Vorentgasungsphase B and in unfavorable cases, in addition to dust, may also contain soot, which is due to decomposition processes in the pre-degassing zone B.
- a Flugstromnachverngasungszone G is therefore provided in the upper part of the reactor, in which at temperatures of 500 - 1000 0 C by supplying oxygen in the presence of water vapor, the dust and soot-containing gases is thermally treated, so that it is of high quality Raw synthesis gas for material and / or thermal use can be provided strigg.
- This also includes carbon compounds with polymeric structures, the new process greatly reducing the formation of oily or tarry fission products by deliberately controlling the intrinsic temperature of the material or the fission products.
- the autothermal procedure by means of partial oxidation also results in no emission sources, so that the use of contaminated carbon-rich substances with, for example, increased heavy metal contents as they arise, for example, in varnished woods, is possible.
- suitable bulk material is in particular C a O, which is present in a particle size of at most 20 cm, the particle size range between 1 and 8 cm having proven to be particularly advantageous.
- the bulk material with this grain size not only serves as a heat and transport medium, but also ensures, with its mechanical properties during the wandering through of the vertical shaft furnace 100, that the carbon-rich substances do not agglomerate or cake. This is ensured by the mechanical abrasion of the constantly moving grain.
- the bulk material When using CaO, the bulk material also has the further advantage that it can be used as a reactant z.
- haloge- ne is available and insofar counteracts the formation of dioxins, furans or the like.
- the formation of these toxic substances is also counteracted by the absence of oxygen as a reactant in the temperature range critical for the formation of these substances. It is particularly advantageous in this case to mix the bulk material with a fine material fraction whose particle size is in the millimeter range and below, for example in the order of magnitude of approximately less than 2 mm down to the micrometer range.
- Such fines have a very large reactive surface and are partially present as dust in the reaction gases, from which it can easily be filtered out.
- the bulk material is taken off at the bottom of the vertical shaft furnace 10 and returned to the vertical shaft furnace 10 by means of a circulation guide 13 while supplying new carbon-rich substances 14. Also in this area can fines z. B. be excreted by screening.
- the described method is advantageously carried out with a slight negative pressure, preferably in a range to -200 mbar, in a Overpressure ideally not more than 1000 mbar.
- a seal can be achieved solely by feeding the reactor via the bulk material column 1, which is loaded on the reactor bed owing to its static weight and thus communicating with the reactor filling 2 without further fittings.
- this is first fed to a bulk material template 3. By continuous decrease of the refractory Bulk material at the reactor bottom 4 this is continuously migrated.
- the mixture of refractory bulk material and carbon-rich substances automatically slips from the bulk material receiver 3 into the reactor without the need for fittings or other technical control devices.
- the height of the bulk column is chosen so that it ensures the sealing of the reactor gas phase to the atmosphere by their own pressure loss over the bed.
- the operation of the reactor in negative pressure is of particular advantage, since the escape of reactor gas is excluded.
- the entry of thermal energy takes place substantially in the oxidation zone D, wherein the mentioned basic performance by metering of oxygen 5 and fuel 6, such.
- fuel oil natural gas or purified synthesis gas from the present process is introduced via burner lances 7 as direct firing in the bed.
- the substantial energy input is produced by partial combustion of the previously calcined carbon-rich substances in the bulk material and by metering oxygen or else simple air over the reactor bottom 8.
- the task of the base load burner 7 is to ensure the reliable ignition of the reactants in the oxidation zone D.
- the generated hot gases which consist essentially of carbon monoxide, but also of hydrogen, flow upward through the reactor bed from the oxidation zone D and serve as energy carriers for heating the process zones formed above the oxidation zone D.
- the carbon-rich substances which in practice are mostly water-moist, evaporate the water they contain to a natural content. temperature of 100 0 C heated, while in the subsequent Vorentgasungszone B, the thermal elimination of polymeric or organic components. Due to the amount of energy required for the cleavage, the increase in the intrinsic temperature of the material here is limited to approximately 45O 0 C. In this zone, the hot gases from the underlying zones mix with the resulting gases from the thermal fission.
- the oxidation in the oxidation zone D is controlled so that a complete oxidation of the remaining non-gassed carbon to carbon monoxide is ensured. This control is carried out primarily by targeted adjustment of the flow rate through the continuous bulk material removal at the reactor bottom 4, but also by optionally setting the base load combustion 7 or a change in the proportion of carbon-rich substances in the bulk material template. 3
- water is supply 9 is preferably provided in the region of the Abhitzezone E, whereby the water transferred at temperatures above 450 0 C in superheated steam and fed through upward flow of the oxidation zone D. In countercurrent, the hot bulk material flow from the oxidation zone D is cooled.
- a gas cooling system 10 which consists essentially of water and small proportions of relatively high molecular weight organic compounds. These compounds do not affect the course of the process, but would make it difficult to dispose of the condensate mixture.
- the already mentioned efficient energy recycling is realized, wherein the refractory bulk material is cooled so far that ash fractions and fines can be separated via a screening device 12 or other separation device.
- the already mentioned circulation 13 of the coarse bulk material is carried out with mixing with new carbon-rich substances 14 on the bulk material template 3. Losses of coarse bulk material, for example due to mechanical abrasion, are compensated by a dosage 15 of fresh coarse bulk material.
- a gas burner 17 is provided. This can be operated with an excess of oxygen-containing gas 18 based on the fuel gas 19 in the burner 17 to ensure a subsequent gasification of soot particles and other organic fine particles in the synthesis gas.
- the filtered filter dust may still contain unfrozen soot particles, which are used by partial recycling 22 of the filter dust in the oxidation zone D. Due to the process, a large number of accompanying substances from the carbon-rich substances used are also bound in the filter dust by adsorption (eg heavy metals) and / or by reaction (eg as halides), so that the filter dust represents a desired contaminant sink in the process according to the invention. When corresponding carbon-containing substances are used, therefore, a discharge 23 of a partial flow of the filter dust from the process must be carried out, which must be disposed of.
- adsorption eg heavy metals
- reaction eg as halides
- the synthesis gas is preferably cooled by cooling to temperatures below
- a further advantageous procedure can be achieved in that part of the condensate mixture from the gas cooler is recirculated continuously as quench medium to the head of the gas cooler (at 25), whereby a more efficient gas cooling is achieved and at the same time wall deposits in the gas cooler are avoided.
- such purified synthesis gas can also be split into its components by means of air separation plants or pressure swing adsorption technology and / or used as fuel for power generation in gas engines.
- the synthesis gas produced in the fly-ash gasification zone can also be used for direct power generation and / or steam generation.
- the flue gas from the steam generator still contains significant dust components, which are separated via a flue gas filtration K.
- the flue gas is then optionally still on a flue gas cleaning L and / or Denox mich M out to meet the legal environmental requirements for the emission into the atmosphere.
- a lime shaft furnace with a clear diameter of 2.2 m and a shaft height of 14.1 m is operated with heavy fuel oil via burner lances as a basic firing in the oxidation zone.
- a refractory bulk material calcined lime in a grain size of 0.5 to 6 cm was used and in a continuous flow rate (see Table 1, column c) over the lime shaft furnace from top to bottom recirculated, while the carbon-rich substance (see Table 1, Column a) was admixed to this circulation stream before entry into the upper furnace area as a continuous stream (see Table 1, column b).
- the basic firing (see Table 1, columns d and e) was set so that a gas temperature of 600 to 700 0 C was established at the gas outlet of the lime kiln.
- the condensate mixture obtained in the gas cooler which consisted essentially of water and small amounts of organic oils, was buffered.
- the carbon-rich substances used in the embodiments 1 to 7 are shown in their composition and quality of Table 2 and columns a to e.
- the resulting in the embodiments gas was detected after the gas cooler via a gas flow measurement and analyzed by an online calorific value.
- the average gas flow rate is shown in Table 3, column a, and the lower calorific value in Table 3, column b.
- the resulting flow rates of the aqueous condensate phase from the gas cooling (Table 3, column c) and the oil phase from the gas cooling (Table 3, column d) were determined.
- the resulting ash was continuously screened from the coarse bulk material downstream of the reactor outlet and the fine fraction (particle size ⁇ 3 mm) was recorded. The determined mass flow is shown in Table 3, column e. Table 3
- the resulting in the embodiments gas was analyzed after gas cooling via an online analysis of its components.
- the gas compositions are shown in Table 4, columns a to e.
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PCT/EP2008/010999 WO2009080336A2 (de) | 2007-12-20 | 2008-12-22 | Autothermes verfahren zur kontinuierlichen vergasung von kohlenstoffreichen substanzen |
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2007
- 2007-12-20 DE DE102007062414A patent/DE102007062414B4/de not_active Expired - Fee Related
-
2008
- 2008-12-22 US US12/809,350 patent/US8632614B2/en not_active Expired - Fee Related
- 2008-12-22 AU AU2008340602A patent/AU2008340602B2/en not_active Ceased
- 2008-12-22 RU RU2010129542/05A patent/RU2471856C2/ru not_active IP Right Cessation
- 2008-12-22 UA UAA201008501A patent/UA97305C2/uk unknown
- 2008-12-22 EP EP08864268A patent/EP2231828A2/de not_active Withdrawn
- 2008-12-22 KR KR1020107015842A patent/KR101304154B1/ko not_active IP Right Cessation
- 2008-12-22 CN CN200880121676.9A patent/CN101903501B/zh not_active Expired - Fee Related
- 2008-12-22 WO PCT/EP2008/010999 patent/WO2009080336A2/de active Application Filing
- 2008-12-22 JP JP2010538491A patent/JP2011506711A/ja active Pending
- 2008-12-22 BR BRPI0821292-9A patent/BRPI0821292A2/pt active Search and Examination
- 2008-12-22 CA CA2710168A patent/CA2710168C/en not_active Expired - Fee Related
-
2010
- 2010-06-01 ZA ZA2010/03910A patent/ZA201003910B/en unknown
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2011
- 2011-03-14 HK HK11102528.4A patent/HK1148550A1/zh not_active IP Right Cessation
Non-Patent Citations (2)
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None * |
See also references of WO2009080336A2 * |
Also Published As
Publication number | Publication date |
---|---|
WO2009080336A2 (de) | 2009-07-02 |
RU2471856C2 (ru) | 2013-01-10 |
RU2010129542A (ru) | 2012-01-27 |
CA2710168C (en) | 2013-10-22 |
JP2011506711A (ja) | 2011-03-03 |
ZA201003910B (en) | 2011-02-23 |
DE102007062414B4 (de) | 2009-12-24 |
AU2008340602A1 (en) | 2009-07-02 |
CN101903501B (zh) | 2014-04-23 |
UA97305C2 (uk) | 2012-01-25 |
BRPI0821292A2 (pt) | 2015-06-16 |
CA2710168A1 (en) | 2009-07-02 |
AU2008340602B2 (en) | 2014-06-19 |
WO2009080336A3 (de) | 2010-02-18 |
HK1148550A1 (zh) | 2011-09-09 |
CN101903501A (zh) | 2010-12-01 |
DE102007062414A1 (de) | 2009-07-02 |
KR20100096251A (ko) | 2010-09-01 |
KR101304154B1 (ko) | 2013-09-04 |
US20110005136A1 (en) | 2011-01-13 |
US8632614B2 (en) | 2014-01-21 |
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