JP2002502927A - 排ガス中のNOxの還元機構 - Google Patents
排ガス中のNOxの還元機構Info
- Publication number
- JP2002502927A JP2002502927A JP2000530293A JP2000530293A JP2002502927A JP 2002502927 A JP2002502927 A JP 2002502927A JP 2000530293 A JP2000530293 A JP 2000530293A JP 2000530293 A JP2000530293 A JP 2000530293A JP 2002502927 A JP2002502927 A JP 2002502927A
- Authority
- JP
- Japan
- Prior art keywords
- scr
- catalyst
- gas
- nox
- gas stream
- 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- Withdrawn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
- 230000007246 mechanism Effects 0.000 title claims abstract description 27
- 230000009467 reduction Effects 0.000 title abstract description 5
- 239000003054 catalyst Substances 0.000 claims abstract description 79
- 239000007789 gas Substances 0.000 claims abstract description 54
- 239000013618 particulate matter Substances 0.000 claims abstract description 18
- 239000003638 chemical reducing agent Substances 0.000 claims abstract description 15
- 230000003647 oxidation Effects 0.000 claims abstract description 13
- 238000007254 oxidation reaction Methods 0.000 claims abstract description 13
- 238000000034 method Methods 0.000 claims description 25
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical group [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 claims description 14
- 239000012530 fluid Substances 0.000 claims description 12
- 239000000203 mixture Substances 0.000 claims description 7
- 238000001816 cooling Methods 0.000 claims description 6
- 229910052697 platinum Inorganic materials 0.000 claims description 6
- 238000011144 upstream manufacturing Methods 0.000 claims description 6
- 239000000356 contaminant Substances 0.000 claims description 5
- 239000011236 particulate material Substances 0.000 claims description 2
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 claims 1
- 239000003546 flue gas Substances 0.000 claims 1
- 230000001590 oxidative effect Effects 0.000 claims 1
- 239000000126 substance Substances 0.000 claims 1
- 238000006243 chemical reaction Methods 0.000 abstract description 22
- 239000000567 combustion gas Substances 0.000 abstract description 3
- 238000012360 testing method Methods 0.000 description 22
- 238000002347 injection Methods 0.000 description 14
- 239000007924 injection Substances 0.000 description 14
- 238000012937 correction Methods 0.000 description 12
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 6
- XSQUKJJJFZCRTK-UHFFFAOYSA-N Urea Chemical compound NC(N)=O XSQUKJJJFZCRTK-UHFFFAOYSA-N 0.000 description 5
- 229930195733 hydrocarbon Natural products 0.000 description 5
- 150000002430 hydrocarbons Chemical class 0.000 description 5
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 description 4
- 239000004202 carbamide Substances 0.000 description 4
- 230000008859 change Effects 0.000 description 4
- 239000002283 diesel fuel Substances 0.000 description 4
- 229910010413 TiO 2 Inorganic materials 0.000 description 3
- 238000010531 catalytic reduction reaction Methods 0.000 description 3
- 239000003344 environmental pollutant Substances 0.000 description 3
- 231100000719 pollutant Toxicity 0.000 description 3
- 238000006722 reduction reaction Methods 0.000 description 3
- 229910021536 Zeolite Inorganic materials 0.000 description 2
- 229910021529 ammonia Inorganic materials 0.000 description 2
- 230000009286 beneficial effect Effects 0.000 description 2
- 239000000919 ceramic Substances 0.000 description 2
- 230000000052 comparative effect Effects 0.000 description 2
- 230000009849 deactivation Effects 0.000 description 2
- 238000013461 design Methods 0.000 description 2
- HNPSIPDUKPIQMN-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical compound O=[Si]=O.O=[Al]O[Al]=O HNPSIPDUKPIQMN-UHFFFAOYSA-N 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- QJGQUHMNIGDVPM-UHFFFAOYSA-N nitrogen group Chemical group [N] QJGQUHMNIGDVPM-UHFFFAOYSA-N 0.000 description 2
- 238000000746 purification Methods 0.000 description 2
- 229910052723 transition metal Inorganic materials 0.000 description 2
- 150000003624 transition metals Chemical class 0.000 description 2
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 2
- 239000010457 zeolite Substances 0.000 description 2
- 229910018072 Al 2 O 3 Inorganic materials 0.000 description 1
- 239000004215 Carbon black (E152) Substances 0.000 description 1
- 230000002745 absorbent Effects 0.000 description 1
- 239000002250 absorbent Substances 0.000 description 1
- 238000009825 accumulation Methods 0.000 description 1
- 230000002411 adverse Effects 0.000 description 1
- BVCZEBOGSOYJJT-UHFFFAOYSA-N ammonium carbamate Chemical compound [NH4+].NC([O-])=O BVCZEBOGSOYJJT-UHFFFAOYSA-N 0.000 description 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
- 239000006227 byproduct Substances 0.000 description 1
- KXDHJXZQYSOELW-UHFFFAOYSA-N carbonic acid monoamide Natural products NC(O)=O KXDHJXZQYSOELW-UHFFFAOYSA-N 0.000 description 1
- 238000002485 combustion reaction Methods 0.000 description 1
- 239000004744 fabric Substances 0.000 description 1
- 239000000446 fuel Substances 0.000 description 1
- 239000003502 gasoline Substances 0.000 description 1
- 238000009434 installation Methods 0.000 description 1
- 229910052751 metal Inorganic materials 0.000 description 1
- 239000002184 metal Substances 0.000 description 1
- 238000002156 mixing Methods 0.000 description 1
- 239000003345 natural gas Substances 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
- 229910052760 oxygen Inorganic materials 0.000 description 1
- 230000002035 prolonged effect Effects 0.000 description 1
- 229910052761 rare earth metal Inorganic materials 0.000 description 1
- 230000001105 regulatory effect Effects 0.000 description 1
- 239000000779 smoke Substances 0.000 description 1
- 239000000758 substrate Substances 0.000 description 1
- 238000013519 translation Methods 0.000 description 1
- 229910052720 vanadium Inorganic materials 0.000 description 1
- LEONUFNNVUYDNQ-UHFFFAOYSA-N vanadium atom Chemical compound [V] LEONUFNNVUYDNQ-UHFFFAOYSA-N 0.000 description 1
Classifications
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- F01N—GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL COMBUSTION ENGINES
- F01N9/00—Electrical control of exhaust gas treating apparatus
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- 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
- B01D53/92—Chemical or biological purification of waste gases of engine exhaust gases
- B01D53/94—Chemical or biological purification of waste gases of engine exhaust gases by catalytic processes
- B01D53/9404—Removing only nitrogen compounds
- B01D53/9409—Nitrogen oxides
- B01D53/9431—Processes characterised by a specific device
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- B—PERFORMING OPERATIONS; TRANSPORTING
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- 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
- B01D53/92—Chemical or biological purification of waste gases of engine exhaust gases
- B01D53/94—Chemical or biological purification of waste gases of engine exhaust gases by catalytic processes
- B01D53/9445—Simultaneously removing carbon monoxide, hydrocarbons or nitrogen oxides making use of three-way catalysts [TWC] or four-way-catalysts [FWC]
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/16—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of arsenic, antimony, bismuth, vanadium, niobium, tantalum, polonium, chromium, molybdenum, tungsten, manganese, technetium or rhenium
- B01J23/24—Chromium, molybdenum or tungsten
- B01J23/30—Tungsten
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/38—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals
- B01J23/40—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals of the platinum group metals
- B01J23/42—Platinum
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J35/00—Catalysts, in general, characterised by their form or physical properties
- B01J35/19—Catalysts containing parts with different compositions
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- F01N—GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL COMBUSTION ENGINES
- F01N13/00—Exhaust or silencing apparatus characterised by constructional features ; Exhaust or silencing apparatus, or parts thereof, having pertinent characteristics not provided for in, or of interest apart from, groups F01N1/00 - F01N5/00, F01N9/00, F01N11/00
- F01N13/009—Exhaust or silencing apparatus characterised by constructional features ; Exhaust or silencing apparatus, or parts thereof, having pertinent characteristics not provided for in, or of interest apart from, groups F01N1/00 - F01N5/00, F01N9/00, F01N11/00 having two or more separate purifying devices arranged in series
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- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
- F01N—GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL COMBUSTION ENGINES
- F01N3/00—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust
- F01N3/02—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for cooling, or for removing solid constituents of, exhaust
- F01N3/021—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for cooling, or for removing solid constituents of, exhaust by means of filters
- F01N3/023—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for cooling, or for removing solid constituents of, exhaust by means of filters using means for regenerating the filters, e.g. by burning trapped particles
- F01N3/0231—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for cooling, or for removing solid constituents of, exhaust by means of filters using means for regenerating the filters, e.g. by burning trapped particles using special exhaust apparatus upstream of the filter for producing nitrogen dioxide, e.g. for continuous filter regeneration systems [CRT]
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- F01N3/00—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust
- F01N3/02—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for cooling, or for removing solid constituents of, exhaust
- F01N3/021—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for cooling, or for removing solid constituents of, exhaust by means of filters
- F01N3/023—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for cooling, or for removing solid constituents of, exhaust by means of filters using means for regenerating the filters, e.g. by burning trapped particles
- F01N3/025—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for cooling, or for removing solid constituents of, exhaust by means of filters using means for regenerating the filters, e.g. by burning trapped particles using fuel burner or by adding fuel to exhaust
- F01N3/0253—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for cooling, or for removing solid constituents of, exhaust by means of filters using means for regenerating the filters, e.g. by burning trapped particles using fuel burner or by adding fuel to exhaust adding fuel to exhaust gases
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- F01N3/00—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust
- F01N3/08—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous
- F01N3/10—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous by thermal or catalytic conversion of noxious components of exhaust
- F01N3/105—General auxiliary catalysts, e.g. upstream or downstream of the main catalyst
- F01N3/106—Auxiliary oxidation catalysts
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- F01N3/00—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust
- F01N3/08—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous
- F01N3/10—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous by thermal or catalytic conversion of noxious components of exhaust
- F01N3/18—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous by thermal or catalytic conversion of noxious components of exhaust characterised by methods of operation; Control
- F01N3/20—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous by thermal or catalytic conversion of noxious components of exhaust characterised by methods of operation; Control specially adapted for catalytic conversion ; Methods of operation or control of catalytic converters
- F01N3/2006—Periodically heating or cooling catalytic reactors, e.g. at cold starting or overheating
- F01N3/2046—Periodically cooling catalytic reactors
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- F01N3/00—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust
- F01N3/08—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous
- F01N3/10—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous by thermal or catalytic conversion of noxious components of exhaust
- F01N3/18—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous by thermal or catalytic conversion of noxious components of exhaust characterised by methods of operation; Control
- F01N3/20—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous by thermal or catalytic conversion of noxious components of exhaust characterised by methods of operation; Control specially adapted for catalytic conversion ; Methods of operation or control of catalytic converters
- F01N3/2066—Selective catalytic reduction [SCR]
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- F01N3/00—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust
- F01N3/08—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous
- F01N3/10—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous by thermal or catalytic conversion of noxious components of exhaust
- F01N3/24—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous by thermal or catalytic conversion of noxious components of exhaust characterised by constructional aspects of converting apparatus
- F01N3/28—Construction of catalytic reactors
- F01N3/2882—Catalytic reactors combined or associated with other devices, e.g. exhaust silencers or other exhaust purification devices
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2255/00—Catalysts
- B01D2255/10—Noble metals or compounds thereof
- B01D2255/102—Platinum group metals
- B01D2255/1021—Platinum
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- B—PERFORMING OPERATIONS; TRANSPORTING
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- B01D2258/00—Sources of waste gases
- B01D2258/01—Engine exhaust gases
- B01D2258/012—Diesel engines and lean burn gasoline engines
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- F01N2250/00—Combinations of different methods of purification
- F01N2250/02—Combinations of different methods of purification filtering and catalytic conversion
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- F01N2260/00—Exhaust treating devices having provisions not otherwise provided for
- F01N2260/02—Exhaust treating devices having provisions not otherwise provided for for cooling the device
- F01N2260/022—Exhaust treating devices having provisions not otherwise provided for for cooling the device using air
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- F01N2260/00—Exhaust treating devices having provisions not otherwise provided for
- F01N2260/02—Exhaust treating devices having provisions not otherwise provided for for cooling the device
- F01N2260/024—Exhaust treating devices having provisions not otherwise provided for for cooling the device using a liquid
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- F01N2270/00—Mixing air with exhaust gases
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- F01N2330/00—Structure of catalyst support or particle filter
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- F01N2570/00—Exhaust treating apparatus eliminating, absorbing or adsorbing specific elements or compounds
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- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
- F01N—GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL COMBUSTION ENGINES
- F01N3/00—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust
- F01N3/08—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous
- F01N3/10—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous by thermal or catalytic conversion of noxious components of exhaust
- F01N3/24—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous by thermal or catalytic conversion of noxious components of exhaust characterised by constructional aspects of converting apparatus
- F01N3/30—Arrangements for supply of additional air
- F01N3/32—Arrangements for supply of additional air using air pump
-
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Abstract
Description
リン直噴(GDI)からのリーン排ガス、中のNOxの選択的接触還元における
改良に関する。
十分に確立されており、高温の排ガスを、窒素系還元剤、特にアンモニアまたは
尿素、の存在下で触媒上を通過させる方法であるとしてその概要を説明できる。
この方法は、約250℃で、または白金触媒を使用してかなり高い温度で、排ガ
スのNOx含有量を約20〜25%低減させるのに有効であるが、白金触媒は高
温操作中にNH3をNOxに酸化する傾向がある。我々は、SCR機構は、自動
車エンジン、特に大型またはヘビーデューティーディーゼルエンジン、の排気に
関するNOx還元用に提案されていると考えるが、この機構ではその様な還元剤
を車両上に貯蔵する必要があり、現時点では商業的に受け入れられるとは考えら
れない。 我々は、SCR機構の性能を大幅に改良できれば、その用途が拡大し、自動車
にも応用できるであろうと考える。本発明の目的は、SCR機構におけるNOx
の転化を大幅に改良し、SCR機構を使用して他の汚染物質の抑制を改善するこ
とである。
ィルター、還元剤流体の供給源、および該供給源の下流のSCR触媒、をこの順
序で組み合わせて含んでなる、改良されたSCR触媒機構を提供する。
ための改良された方法であって、 その様なガス流を、ガス流中のNOの少なくとも一部をNO2に転化するのに
有効な条件下で酸化触媒上を通過させること、 該粒子状物質の少なくとも一部を除去すること、 NO2含有量が高くなったガス流に還元剤流体を添加し、ガス混合物を形成す
ること、そして ガス混合物をSCR触媒上を通過させること、を含んでなる方法を提供する。
ジンからのリーン(高酸素濃度)排ガスから放出されるNOxを大幅に低減する
機会を与えるが、本発明は、他の法規制されている汚染物質、特に炭化水素およ
び粒子状物質、のレベルを非常に効果的に下げることもできる。
例えばトラックまたはバスのエンジン、から排出されるガスに特に応用できると
考えられるが、その用途に限定すべきではない。他の用途には、LDD(ライト
デューティーディーゼル)、GDI、CNG(圧縮天然ガス)エンジン、船また
は固定供給源があろう。しかし、簡潔にするために、本説明の大部分はその様な
自動車用エンジンに関する。
未燃焼燃料の含有量は低いので、この工程は一般的には必要とは考えられないも
のである)が、SCR機構によるNOxからN2への転化率を増加するのに特に
有効であることを見出した。我々は、ガス中の炭化水素レベルを最少に抑えるこ
とも、NOからNO2への転化に有用であると考える。これは、触媒により、お
よび/またはエンジン設計により、または管理により達成できる。NO2/NO
比は、本発明により特定のSCR触媒に対して最も有益なその様な比に調節し、
COおよび炭化水素はSCR触媒の前に酸化されるのが望ましい。例えば、我々
の予備試験結果から、遷移金属/ゼオライトSCR触媒ではすべてのNOをNO 2 に転化するのが望ましいのに対し、希土類元素系SCR触媒では、ある程度の
NOが存在するとして、高比率が望ましく、他の遷移金属系触媒では、実質的に
NOまたはNO2のみであるよりも、ガス混合物が明らかに優れていることが分
かる。さらに驚くべきことに、粒子状物質フィルターを取り入れることにより、
NOxの転化率がさらに高くなる。
ば、セラミックまたは金属製の、スルー−フローハニカム担体上に担持されたP
t触媒が特に好適である。好適な触媒は、例えば、必要なNO2/NO比に応じ
て1〜150gPt/ft3(0.035〜5.3gPt/リットル)触媒体積を
含むPt/Al2O3触媒である。その様な触媒は、有利な効果があるか、また
は少なくとも重大な悪影響が無ければ、他の成分も含むことができる。
るのが好都合である。例えば、本発明の試験では、圧縮NH3の供給を制御する
のに質量制御装置を使用し、排気管中に取り付けた輪状注入装置リングを通して
圧縮NH3を注入した。注入装置リングは、その周囲に配置された複数の注入口
を有する。本出願者は、ポンプおよび注入装置ノズルを包含する従来のディーゼ
ル燃料注入機構を使用して尿素を注入した。圧縮空気の流れもノズルの周りに注
入し、これによって良好な混合および冷却を行なった。
びディーゼル燃料を包む炭化水素、を包含する他の還元剤流体も考えられる。無
論、ディーゼル燃料はディーゼルエンジン自動車上に積載されているが、ディー
ゼル燃料はNH3程選択的な還元性が無く、現時点では好ましくない。
る。現在好ましい触媒は、スルー−フローハニカム担体上に担持されたV2O5 /WO3/TiO2触媒である。その様な触媒は、以下に説明する試験で良好な
性能を示し、市販されているが、長時間の高温運転により、触媒失活を引き起こ
すことがあることが分かった。ほとんどすべてがターボチャージャーを備えてい
るヘビーデューティーディーゼルエンジンは、高負荷および/または高速条件下
で500℃を超える排ガスを生じることがあり、その様な温度は触媒失活を引き
起こすのに十分である。従って、本発明の一実施態様では、SCR触媒の上流に
冷却手段を備える。冷却手段は、高い触媒温度を感知するか、または他の、あま
り直接的ではないが、高い触媒温度につながりそうな条件を確認することにより
、効果的に作動させることができる。好適な冷却手段は、SCR触媒の上流にお
ける水噴射、または空気注入を包含し、例えばエンジンターボチャージャーを利
用し、新鮮な取入れ空気の流れをエンジンにバイパスさせる。しかし、我々は、
水噴射を使用すると触媒の活性低下が起こり、ターボチャージャーを改良して空
気注入を行なうと、触媒全体の空間速度が高くなり、NOx転化率を下げる傾向
があることを観察している。好ましくは、SCR触媒を160℃〜450℃に維
持する。 我々は、本発明が、その現在好ましい実施態様で、NOからNO2へ
の不完全転化に依存することができると考えている。従って、酸化触媒は、また
は酸化触媒と粒子状物質トラップ(使用する場合)が一緒に、市販のバナジア型
触媒に対して、SCR触媒に入るガス流のNOとNO2の体積比を約4:1〜約
1:3にする。上記の様に、他のSCR触媒は異なったNO/NO2比でより優
れた性能を発揮する。我々は、NO/NO2比を調整してNOx還元を改良する
方法が提案されているとは考えていない。
型の粒子状物質は、NO2の存在下で比較的低い温度で「燃焼」させることによ
り、粒子状物質トラップから除去できることを発見した。実際、その様な粒子状
物質トラップを取り入れることにより、粒子状物質の蓄積、その結果生じる閉塞
および背圧の問題を引き起こさずに、排ガスを浄化し、同時にNOxの一部を還
元することができる。好適な粒子状物質トラップは一般的に市販されており、一
般的にセラミックから製造されるウォール−フローフィルターと呼ばれる型のト
ラップが好ましいが、織布また不織布の耐熱性布地を包含する他のデザインの粒
子状物質トラップも使用できる。
て通過し得るNH3またはその誘導体を除去するのが望ましい。当業者は好適な
浄化触媒を入手することができる。
ン(乗用車および実用車)への応用であり、排ガス後処理機構の体積および重量
を、好適な管理機構で、大幅に低減することができる。
す結果を参照しながら、以下に説明する。
販の10リットルヘビーデューティーディーゼルエンジンで行なった。
、エンジンの排気機構に取り付けた。SCR触媒の上流にNH3を様々な比率で
注入した。NH3は圧縮ガスのシリンダーから供給し、通常の質量流量制御装置
を使用し、実験注入リングへのNH3ガスの流量を調整した。注入リングは、直
径10cmの輪状リングであり、排ガス流の方向にガスを注入するための20個の
小さな注入口が配置されている。SCR触媒の前後にNOx分析系を取り付けて
NOx転化率を測定し、排ガス温度との関係を図1に示す。エンジン速度を一定
に維持し、作用させるトルクを変えることにより、温度を変化させた。
00%の異なったNH3注入量で、複数の試験を行なった。軽い負荷に対応する
低温では、転化率は約25%であり、最高転化率は、化学量論的(100%)な
量のNH3を325〜400℃の触媒温度で加える必要があり、約90%に達す
るのが容易に分かる。しかし、化学量論的なNH3注入の約70%を超えると、
NH3は未反応のままSCR触媒をすり抜け、汚染物質の問題をさらに引き起こ
すことを確認した。
径26.67cm、長さ15.24cm)、10gPt/ft3(0.35g/リットル
)触媒体積を含む白金酸化触媒を挿入することにより試験装置を修正した。同等
の試験を行ない、図2にプロットする結果から、225℃でも、NOxの転化率
は25%から>60%に増加することを観察した。最大転化率は95%を超えて
いた。この試験でも、下記の試験でも、NH3のすり抜けは観察されなかった。
同じ条件下で、100%NH3注入およびSCR触媒上40,000〜70,0
00hr−1の空間速度で試験を行なった。結果を図3にプロットする。驚くべ
きことに、NOx転化率が劇的に改良され、225℃で90%を超え、350℃
で100%に達した。さらに、無論、ディーゼルエンジンから排出される最も良
く目に見える汚染物質である粒子状物質も抑制された。
試験を行なった。この試験により、67%粒子状物質、89%HCおよび87%
NOx転化率が得られ、結果を図4にプロットする。
に示す優れた結果が確認された。
中のNOをNO2に転化し、その後、粒子状物質をフィルター中に捕獲し、粒子
状物質をNO2との反応により酸化する、ディーゼルエンジンの排ガスを浄化す
る方法を開示している。その後、排ガスはNOx吸収剤に、または一実施態様で
はNOx転化触媒に供給される。排ガス中の未燃焼炭化水素およびCOは、ゼオ
ライト中に捕獲され、放出されてNOx転化触媒上でNOxと反応する。 SCR(選択的接触還元)と呼ばれる技術は、工業的設備の燃焼ガスに関して
十分に確立されており、高温の排ガスを、窒素系還元剤、特にアンモニアまたは
尿素、の存在下で触媒上を通過させる方法であるとしてその概要を説明できる。
この方法は、約250℃で、または白金触媒を使用してかなり高い温度で、排ガ
スのNOx含有量を約20〜25%低減させるのに有効であるが、白金触媒は高
温操作中にNH3をNOxに酸化する傾向がある。我々は、SCR機構は、自動
車エンジン、特に大型またはヘビーデューティーディーゼルエンジン、の排気に
関するNOx還元用に提案されていると考えるが、この機構ではその様な還元剤
を車両上に貯蔵する必要があり、現時点では商業的に受け入れられるとは考えら
れない。 我々は、SCR機構の性能を大幅に改良できれば、その用途が拡大し、自動車
にも応用できるであろうと考える。本発明の目的は、SCR機構におけるNOx
の転化を大幅に改良し、SCR機構を使用して他の汚染物質の抑制を改善するこ
とである。
るのに効果的な酸化触媒、粒子状物質フィルター、還元剤流体の供給源、該粒子
状物質トラップの下流に配置された、該還元剤流体の注入手段、およびSCR触
媒、をこの順序で組み合わせて含んでなる、改良されたSCR触媒機構を提供す
る。
せるための改良された方法であって、その様なガス流を、ガス流中のNOの少な
くとも一部をNO2に転化し、ガス流のNO2含有量を増加させるのに有効な条
件下で酸化触媒上を通過させること、該粒子状物質の少なくとも一部を粒子状物
質トラップ中で除去すること、捕獲された粒子状物質をNO2と反応させること
、ガス流に還元剤流体を添加し、該トラップの下流にガス混合物を形成すること
、およびガス混合物をSCR触媒上を通過させること、を含んでなる方法を提供
する。
Claims (12)
- 【請求項1】 NOおよび粒子状物質を含む燃焼排ガスを処理する改良されたSCR機構であ
って、 前記NOx中のNOの少なくとも一部をNO2に効果的に転化する酸化触媒と
、粒子状物質トラップと、還元剤流体の供給源と、およびSCR触媒とをこの順
序で、かつ、組み合わせて含んでなる、SCR機構。 - 【請求項2】 還元性流体がNH3である、請求項1に記載のSCR機構。
- 【請求項3】 酸化触媒が、スルー−フローハニカム担体上に担持された白金触媒である、請
求項1または2に記載のSCR機構。 - 【請求項4】 粒子状物質フィルターがウォール−フローフィルターである、請求項1〜3の
いずれか一項に記載のSCR機構。 - 【請求項5】 SCR触媒の上流でガスを冷却する手段も含んでなる、請求項1〜4のいずれ
か一項に記載のSCR機構。 - 【請求項6】 前記ガス冷却手段が、高いSCR触媒温度が感知された時、または高い触媒温
度になりうると予想される条件が確認された時にのみ作動する様な制御手段をも
含んでなる、請求項5に記載のSCR機構。 - 【請求項7】 請求項1〜5のいずれか一項に記載のSCR機構を備えたディーゼルエンジン
。 - 【請求項8】 排ガス後処理機構の体積が低減される、請求項6に記載のライトデューティー
ディーゼルエンジン。 - 【請求項9】 ガス流中の、粒子状物質およびNOxを包含する汚染物質を低減させるための
方法であって、 その様なガス流を、ガス流中のNOの少なくとも一部をNO2に転化するのに
有効な条件下で酸化触媒上に通過させることと、 前記粒子状物質の少なくとも一部を除去すること、 NO2含有量が高くなったガス流に還元剤流体を添加して、ガス混合物を形成
すること、そして ガス混合物を、NOx還元条件下でSCR触媒上を通過させることとを含んで
なる、方法。 - 【請求項10】 前記ガス流が、ディーゼル、GDIまたはCNGエンジンからの排気である、
請求項9に記載の方法。 - 【請求項11】 ガスが、必要であればSCR触媒に到達する前に冷却される、請求項9または
10に記載の方法。 - 【請求項12】 ガス中のNOとNO2の比が、酸化触媒上でのNOの酸化によって、SCR触
媒に最適になる様に予め決定されたレベルに調節される、請求項9〜11のいず
れか一項に記載の方法。
Applications Claiming Priority (3)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
GBGB9802504.2A GB9802504D0 (en) | 1998-02-06 | 1998-02-06 | Improvements in emission control |
GB9802504.2 | 1998-02-06 | ||
PCT/GB1999/000292 WO1999039809A1 (en) | 1998-02-06 | 1999-01-28 | SYSTEM FOR NOx REDUCTION IN EXHAUST GASES |
Related Child Applications (1)
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JP2012138814A Withdrawn JP2012211586A (ja) | 1998-02-06 | 2012-06-20 | 排ガス中のNOxの還元機構 |
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JP2012211586A (ja) * | 1998-02-06 | 2012-11-01 | Johnson Matthey Plc | 排ガス中のNOxの還元機構 |
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Also Published As
Publication number | Publication date |
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US20090169451A1 (en) | 2009-07-02 |
CA2319483C (en) | 2007-04-24 |
US20100199646A1 (en) | 2010-08-12 |
AU2290299A (en) | 1999-08-23 |
JP2012211586A (ja) | 2012-11-01 |
EP1054722B1 (en) | 2001-12-05 |
JP2014058976A (ja) | 2014-04-03 |
DE69900548T2 (de) | 2002-05-23 |
EP1054722A1 (en) | 2000-11-29 |
US6805849B1 (en) | 2004-10-19 |
ATE209954T1 (de) | 2001-12-15 |
NO20003963L (no) | 2000-08-04 |
US7498010B2 (en) | 2009-03-03 |
US8142747B2 (en) | 2012-03-27 |
JP2011089521A (ja) | 2011-05-06 |
DK1054722T3 (da) | 2002-03-04 |
DE69900548D1 (de) | 2002-01-17 |
JP5847784B2 (ja) | 2016-01-27 |
WO1999039809A1 (en) | 1999-08-12 |
US20070240402A1 (en) | 2007-10-18 |
US8480986B2 (en) | 2013-07-09 |
US20040258594A1 (en) | 2004-12-23 |
CA2319483A1 (en) | 1999-08-12 |
GB9802504D0 (en) | 1998-04-01 |
JP5266439B2 (ja) | 2013-08-21 |
DE29923945U1 (de) | 2001-10-31 |
US20110286903A1 (en) | 2011-11-24 |
NO20003963D0 (no) | 2000-08-04 |
NO321171B1 (no) | 2006-03-27 |
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