JP6340101B1 - 触媒担持用基材及び触媒担体 - Google Patents
触媒担持用基材及び触媒担体 Download PDFInfo
- Publication number
- JP6340101B1 JP6340101B1 JP2017036612A JP2017036612A JP6340101B1 JP 6340101 B1 JP6340101 B1 JP 6340101B1 JP 2017036612 A JP2017036612 A JP 2017036612A JP 2017036612 A JP2017036612 A JP 2017036612A JP 6340101 B1 JP6340101 B1 JP 6340101B1
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- Prior art keywords
- mass
- oxide film
- alumina
- catalyst
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- 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.)
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- 239000003054 catalyst Substances 0.000 title claims abstract description 76
- 239000000758 substrate Substances 0.000 title claims description 15
- 239000011888 foil Substances 0.000 claims abstract description 91
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims abstract description 66
- 238000000746 purification Methods 0.000 claims abstract description 32
- 239000000463 material Substances 0.000 claims abstract description 12
- 229910052751 metal Inorganic materials 0.000 claims abstract description 6
- 239000002184 metal Substances 0.000 claims abstract description 6
- 229910001220 stainless steel Inorganic materials 0.000 claims description 38
- 239000010935 stainless steel Substances 0.000 claims description 38
- 229910052804 chromium Inorganic materials 0.000 claims description 7
- 229910052782 aluminium Inorganic materials 0.000 claims description 6
- 229910052742 iron Inorganic materials 0.000 claims description 6
- 238000002485 combustion reaction Methods 0.000 claims description 3
- 230000003628 erosive effect Effects 0.000 abstract description 26
- 239000006104 solid solution Substances 0.000 abstract 1
- 239000007789 gas Substances 0.000 description 61
- MWUXSHHQAYIFBG-UHFFFAOYSA-N Nitric oxide Chemical compound O=[N] MWUXSHHQAYIFBG-UHFFFAOYSA-N 0.000 description 20
- 238000010438 heat treatment Methods 0.000 description 15
- 230000003647 oxidation Effects 0.000 description 11
- 238000007254 oxidation reaction Methods 0.000 description 11
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 description 10
- 230000006866 deterioration Effects 0.000 description 8
- 230000003197 catalytic effect Effects 0.000 description 6
- 230000000052 comparative effect Effects 0.000 description 6
- 238000012986 modification Methods 0.000 description 6
- 230000004048 modification Effects 0.000 description 6
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 6
- 229910021529 ammonia Inorganic materials 0.000 description 5
- 230000001965 increasing effect Effects 0.000 description 5
- 230000002829 reductive effect Effects 0.000 description 5
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 4
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 description 4
- 238000005219 brazing Methods 0.000 description 4
- 230000007423 decrease Effects 0.000 description 4
- 230000000694 effects Effects 0.000 description 4
- 238000011156 evaluation Methods 0.000 description 4
- 238000004519 manufacturing process Methods 0.000 description 4
- 238000000034 method Methods 0.000 description 4
- 229910052760 oxygen Inorganic materials 0.000 description 4
- 238000012360 testing method Methods 0.000 description 4
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 3
- 239000002585 base Substances 0.000 description 3
- 239000013078 crystal Substances 0.000 description 3
- 238000005259 measurement Methods 0.000 description 3
- 230000001590 oxidative effect Effects 0.000 description 3
- 239000001301 oxygen Substances 0.000 description 3
- 230000036961 partial effect Effects 0.000 description 3
- 239000002245 particle Substances 0.000 description 3
- 238000012545 processing Methods 0.000 description 3
- 229910052761 rare earth metal Inorganic materials 0.000 description 3
- WTHDKMILWLGDKL-UHFFFAOYSA-N urea;hydrate Chemical compound O.NC(N)=O WTHDKMILWLGDKL-UHFFFAOYSA-N 0.000 description 3
- MGWGWNFMUOTEHG-UHFFFAOYSA-N 4-(3,5-dimethylphenyl)-1,3-thiazol-2-amine Chemical compound CC1=CC(C)=CC(C=2N=C(N)SC=2)=C1 MGWGWNFMUOTEHG-UHFFFAOYSA-N 0.000 description 2
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 2
- UQSXHKLRYXJYBZ-UHFFFAOYSA-N Iron oxide Chemical compound [Fe]=O UQSXHKLRYXJYBZ-UHFFFAOYSA-N 0.000 description 2
- XSQUKJJJFZCRTK-UHFFFAOYSA-N Urea Chemical compound NC(N)=O XSQUKJJJFZCRTK-UHFFFAOYSA-N 0.000 description 2
- 229910052783 alkali metal Inorganic materials 0.000 description 2
- 150000001340 alkali metals Chemical class 0.000 description 2
- 229910052788 barium Inorganic materials 0.000 description 2
- 230000015572 biosynthetic process Effects 0.000 description 2
- 238000007664 blowing Methods 0.000 description 2
- 229910052791 calcium Inorganic materials 0.000 description 2
- 239000004202 carbamide Substances 0.000 description 2
- 229910002092 carbon dioxide Inorganic materials 0.000 description 2
- 239000001569 carbon dioxide Substances 0.000 description 2
- 229910002091 carbon monoxide Inorganic materials 0.000 description 2
- 239000000969 carrier Substances 0.000 description 2
- 238000011161 development Methods 0.000 description 2
- 230000018109 developmental process Effects 0.000 description 2
- 229910052735 hafnium Inorganic materials 0.000 description 2
- 229910000765 intermetallic Inorganic materials 0.000 description 2
- 229910052749 magnesium Inorganic materials 0.000 description 2
- 229910052758 niobium Inorganic materials 0.000 description 2
- 229910052757 nitrogen Inorganic materials 0.000 description 2
- JCXJVPUVTGWSNB-UHFFFAOYSA-N nitrogen dioxide Inorganic materials O=[N]=O JCXJVPUVTGWSNB-UHFFFAOYSA-N 0.000 description 2
- 238000001556 precipitation Methods 0.000 description 2
- 239000002243 precursor Substances 0.000 description 2
- 239000007787 solid Substances 0.000 description 2
- 229910052719 titanium Inorganic materials 0.000 description 2
- 238000011144 upstream manufacturing Methods 0.000 description 2
- 238000004804 winding Methods 0.000 description 2
- 229910052726 zirconium Inorganic materials 0.000 description 2
- 229910018072 Al 2 O 3 Inorganic materials 0.000 description 1
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 1
- 229910001122 Mischmetal Inorganic materials 0.000 description 1
- 229910000831 Steel Inorganic materials 0.000 description 1
- 238000002441 X-ray diffraction Methods 0.000 description 1
- 239000000654 additive Substances 0.000 description 1
- 230000000996 additive effect Effects 0.000 description 1
- 230000002411 adverse Effects 0.000 description 1
- 230000005540 biological transmission Effects 0.000 description 1
- 238000011088 calibration curve Methods 0.000 description 1
- 229910052799 carbon Inorganic materials 0.000 description 1
- 238000010531 catalytic reduction reaction Methods 0.000 description 1
- 238000006243 chemical reaction Methods 0.000 description 1
- 239000011248 coating agent Substances 0.000 description 1
- 238000000576 coating method Methods 0.000 description 1
- 238000005097 cold rolling Methods 0.000 description 1
- 239000000470 constituent Substances 0.000 description 1
- 229910052593 corundum Inorganic materials 0.000 description 1
- 239000010431 corundum Substances 0.000 description 1
- 230000001186 cumulative effect Effects 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 238000009792 diffusion process Methods 0.000 description 1
- 238000009826 distribution Methods 0.000 description 1
- 230000002708 enhancing effect Effects 0.000 description 1
- 238000010304 firing Methods 0.000 description 1
- 235000021060 food property Nutrition 0.000 description 1
- 239000000446 fuel Substances 0.000 description 1
- 230000012447 hatching Effects 0.000 description 1
- 229930195733 hydrocarbon Natural products 0.000 description 1
- 150000002430 hydrocarbons Chemical class 0.000 description 1
- 239000001257 hydrogen Substances 0.000 description 1
- 229910052739 hydrogen Inorganic materials 0.000 description 1
- 230000003301 hydrolyzing effect Effects 0.000 description 1
- 230000001771 impaired effect Effects 0.000 description 1
- 239000012535 impurity Substances 0.000 description 1
- LIKBJVNGSGBSGK-UHFFFAOYSA-N iron(3+);oxygen(2-) Chemical compound [O-2].[O-2].[O-2].[Fe+3].[Fe+3] LIKBJVNGSGBSGK-UHFFFAOYSA-N 0.000 description 1
- SZVJSHCCFOBDDC-UHFFFAOYSA-N iron(II,III) oxide Inorganic materials O=[Fe]O[Fe]O[Fe]=O SZVJSHCCFOBDDC-UHFFFAOYSA-N 0.000 description 1
- 238000005304 joining Methods 0.000 description 1
- 230000000670 limiting effect Effects 0.000 description 1
- 229910052748 manganese Inorganic materials 0.000 description 1
- 230000003287 optical effect Effects 0.000 description 1
- 239000013618 particulate matter Substances 0.000 description 1
- 230000035699 permeability Effects 0.000 description 1
- 230000010363 phase shift Effects 0.000 description 1
- 238000003825 pressing Methods 0.000 description 1
- 230000008929 regeneration Effects 0.000 description 1
- 238000011069 regeneration method Methods 0.000 description 1
- 238000011160 research Methods 0.000 description 1
- 229920006395 saturated elastomer Polymers 0.000 description 1
- 229910052710 silicon Inorganic materials 0.000 description 1
- 238000004544 sputter deposition Methods 0.000 description 1
- 239000010959 steel Substances 0.000 description 1
- 230000004580 weight loss Effects 0.000 description 1
- 229910052727 yttrium Inorganic materials 0.000 description 1
Classifications
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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
- F01N3/28—Construction of catalytic reactors
- F01N3/2803—Construction of catalytic reactors characterised by structure, by material or by manufacturing of catalyst support
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- F01N3/281—Metallic honeycomb monoliths made of stacked or rolled sheets, foils or plates
- F01N3/2814—Metallic honeycomb monoliths made of stacked or rolled sheets, foils or plates all sheets, plates or foils being corrugated
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- B01J23/70—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper
- B01J23/76—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper combined with metals, oxides or hydroxides provided for in groups B01J23/02 - B01J23/36
- B01J23/84—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper combined with metals, oxides or hydroxides provided for in groups B01J23/02 - B01J23/36 with arsenic, antimony, bismuth, vanadium, niobium, tantalum, polonium, chromium, molybdenum, tungsten, manganese, technetium or rhenium
- B01J23/85—Chromium, molybdenum or tungsten
- B01J23/88—Molybdenum
- B01J23/887—Molybdenum containing in addition other metals, oxides or hydroxides provided for in groups B01J23/02 - B01J23/36
- B01J23/8878—Chromium
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- F01N3/2066—Selective catalytic reduction [SCR]
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- 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
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- F01N3/08—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous
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- 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
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- B01J21/00—Catalysts comprising the elements, oxides, or hydroxides of magnesium, boron, aluminium, carbon, silicon, titanium, zirconium, or hafnium
- B01J21/02—Boron or aluminium; Oxides or hydroxides thereof
- B01J21/04—Alumina
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- F01N2330/38—Honeycomb supports characterised by their structural details flow channels with means to enhance flow mixing,(e.g. protrusions or projections)
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- F01N2330/00—Structure of catalyst support or particle filter
- F01N2330/30—Honeycomb supports characterised by their structural details
- F01N2330/42—Honeycomb supports characterised by their structural details made of three or more different sheets, foils or plates stacked one on the other
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- F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
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- F01N2510/00—Surface coverings
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- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
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- F01N2510/06—Surface coverings for exhaust purification, e.g. catalytic reaction
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- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
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- F01N2510/00—Surface coverings
- F01N2510/06—Surface coverings for exhaust purification, e.g. catalytic reaction
- F01N2510/068—Surface coverings for exhaust purification, e.g. catalytic reaction characterised by the distribution of the catalytic coatings
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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
- F01N2510/00—Surface coverings
- F01N2510/06—Surface coverings for exhaust purification, e.g. catalytic reaction
- F01N2510/068—Surface coverings for exhaust purification, e.g. catalytic reaction characterised by the distribution of the catalytic coatings
- F01N2510/0682—Surface coverings for exhaust purification, e.g. catalytic reaction characterised by the distribution of the catalytic coatings having a discontinuous, uneven or partially overlapping coating of catalytic material, e.g. higher amount of material upstream than downstream or vice versa
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- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Mechanical Engineering (AREA)
- General Engineering & Computer Science (AREA)
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Abstract
Description
(Selective Catalytic Reduction;以下SCRと略記)が実用化されている。
α-アルミナは、Al2O3の分子式で表され、代表的なコランダム結晶構造(六方晶)を有しており、排ガスに含まれるパーティクルに対して優れた耐風食性を発揮する。このため、酸化皮膜に含まれるα-アルミナの下限値は30質量%とした。一方、ステンレス箔に特殊熱処理を施すと、Fe酸化物が必然的に形成され、加熱条件によってはγ、θ、χ、δ、η、κアルミナのうち少なくとも1種類以上のアルミナ及び/又はCr酸化物が形成されるため、酸化皮膜の全てをα-アルミナに形成することはできない。このため、酸化皮膜に含まれるα-アルミナの上限値は99.5質量%とした。さらに、α-アルミナが50%以上であると、酸化皮膜の硬度が増加し、より優れた耐風食性を得られる。このため、より好ましい下限値は50%である。また、上限値が99%以下であると、酸化皮膜の靭性が向上して亀裂や剥離が発生しにくくなるので、より好ましい上限値は99%とした。
(実施例1)
酸化皮膜に含まれるα-アルミナの含有量を調整して、それぞれの触媒担体について耐風食性を評価した。各種の触媒担体をディーゼル排ガス処理設備に設けられるDOCに適用し、20万(km)相当の走行試験を行った後に、触媒担体の風食性、浄化性能を評価した。風食性については、試験前後の触媒担体の重量を比較し、重量減少が1質量%以下の場合には風食性が良好であるとして○で評価し、1.0質量%超の場合には風食性が不良であるとして×で評価した。浄化性能については、初期性能に対する最終性能の劣化率で評価し、劣化率が30%以下の場合には、浄化性能の劣化が小さいとして○で評価し、劣化率が30%以上の場合には、浄化性能の劣化が大きいとして×で評価した。初期性能は、触媒温度が900℃になっている間の累積時間が1時間になった時に測定した浄化性能とした。浄化性能はCO、HC、NOxの浄化率で測定した。最終性能は、触媒温度が900℃になっている間の累積時間が500時間になった時に測定した浄化性能とした。表1は、これらの試験結果を纏めた表であり、添加元素の欄に記載した「REM」はミッシュメタルの略である。
上述の実施形態では、工程S3のロウ付け処理の後に工程S4の特殊熱処理を実施したが、本発明はこれに限るものではなく、工程S4の前に、酸素分圧10−2Pa程度の真空中や、水素、一酸化炭素等の還元雰囲気中で焼成して、ステンレス箔の表面状態を特殊熱処理の前に整えておいてもよい。これにより、上述の酸化皮膜の付与を効率的に実施できる場合がある。
上述の実施形態では、各フィンFを千鳥状に配置したが、本発明はこれに限るものではなく、軸方向の前後で波の位相が異なるオフセット構造を備えていれば他の構成であってもよい。例えば、図5に図示するように、軸方向に対して傾斜する傾斜方向にフィンFを並設したオフセット構造を有する波箔にも本願発明は適用することができる。この場合、各フィンFのガス入り側の端面(露出端面に相当する)に耐風食性に優れた酸化皮膜を形成することができる。また、図6に図示する波箔にも本願発明は適用することができる。すなわち、波箔に一対のスリットSを形成し、これらの一対のスリットSに挟まれた領域を下方に押し下げることにより、上に凸のフィンF1及び下に凸のフィンF2を形成したオフセット構造にも本願発明は適用することができる。この場合、フィンF1のガス入り側端面と、フィンF2のガス入り側端面とに耐風食性に優れた酸化皮膜を形成することができる。
上述の実施形態では、触媒担体1をディーゼル排ガスを浄化する浄化装置に用いる例について説明したが、本発明はこれに限るものではなく、ガソリンの燃焼排ガスを浄化する浄化装置にも適用することができる。
平箔40には間欠的に複数の開口部が形成されていてもよい。ハニカム体10の各流路に流入した排ガスは各開口部を通過して径方向に隣接する別の流路に分岐流入するため、乱流が発生し易くなり、排ガスの浄化性能を高めることができる。また、特殊熱処理を実施した際に各開口部をガスが通過して、これらの開口部における主として下流側の縁の部分に本願発明の酸化皮膜を形成することができる。
10 ハニカム体
20 外筒
30 波箔
40 平箔
F フィン
Claims (8)
- 金属製の平箔と波箔とを積層したハニカム体を含む排ガス浄化用の触媒担持用基材において、
ガス入側に向かって露出する露出端面を含む所定範囲には厚みが0.1μm以上10μm以下の酸化皮膜が形成されており、
この酸化皮膜は、α-アルミナからなる第1のアルミナと、Fe酸化物とを少なくとも含み、
前記α-アルミナには、Feが固溶したα-アルミナとFeが固溶していないα-アルミナとが含まれており、
前記酸化皮膜において、前記第1のアルミナの含有量は30質量%以上99.5質量%以下であり、前記Fe酸化物の含有量は0.5質量%以上40質量%以下であり、Feの含有量は7質量%超35質量%以下であり、
前記所定範囲は、前記露出端面からガスの流れる方向に向かって少なくとも2mmの範囲である
ことを特徴とする触媒担持用基材。 - 前記酸化皮膜は、さらに、第2のアルミナ及びCr酸化物のうち少なくとも1種を含み、
前記第2のアルミナは、γ、θ、χ、δ、η及びκアルミナのうち少なくとも1種類以上からなることを特徴とする請求項1に記載の触媒担持用基材。 - 前記酸化皮膜の厚みをT(μm)、Feの前記酸化皮膜における含有量をG(質量%)としたとき、T(μm)及びG(質量%)の積が4.0超20.0以下であることを特徴とする請求項1又は2に記載の触媒担持用基材。
- 前記波箔は、前記ハニカム体の軸方向の前後で波の位相が互いに異なるオフセット部を有しており、
前記所定範囲における酸化皮膜は、前記オフセット部に形成されていることを特徴とする請求項1乃至3のうちいずれか一つに記載の触媒担持用基材。 - 前記波箔はステンレス箔であり、少なくともFe,Cr,およびAlが含有されており、前記波箔及び前記波箔に形成された前記酸化皮膜には、Feが60質量%以上85質量%以下、Crが9質量%以上30質量%以下、Alが1.5質量%以上13質量%以下であることを特徴とする請求項1乃至4のうちいずれか一つに記載の触媒担持用基材。
- 請求項1乃至5のうちいずれか一つに記載の触媒担持用基材と、
前記平箔及び前記波箔に担持された触媒と、を有することを特徴とする触媒担体。 - ディーゼル排ガスを浄化する浄化装置に用いられることを特徴とする請求項6に記載の触媒担体。
- ガソリンの燃焼排ガスを浄化する浄化装置に用いられることを特徴とする請求項6に記載の触媒担体。
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