JP2011519725A - Pd−au合金触媒を備えたリーンバーン内燃エンジンの排気システム - Google Patents
Pd−au合金触媒を備えたリーンバーン内燃エンジンの排気システム Download PDFInfo
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- 239000003054 catalyst Substances 0.000 title claims abstract description 129
- 229910001020 Au alloy Inorganic materials 0.000 title claims abstract description 24
- 238000002485 combustion reaction Methods 0.000 title claims abstract description 9
- 239000010931 gold Substances 0.000 claims abstract description 61
- 229910044991 metal oxide Inorganic materials 0.000 claims abstract description 29
- 150000004706 metal oxides Chemical class 0.000 claims abstract description 29
- 239000000203 mixture Substances 0.000 claims abstract description 25
- PCHJSUWPFVWCPO-UHFFFAOYSA-N gold Chemical compound [Au] PCHJSUWPFVWCPO-UHFFFAOYSA-N 0.000 claims abstract description 13
- 229910001252 Pd alloy Inorganic materials 0.000 claims abstract description 12
- KDLHZDBZIXYQEI-UHFFFAOYSA-N palladium Substances [Pd] KDLHZDBZIXYQEI-UHFFFAOYSA-N 0.000 claims description 106
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 claims description 79
- 229910052763 palladium Inorganic materials 0.000 claims description 31
- 229910052697 platinum Inorganic materials 0.000 claims description 30
- 238000007254 oxidation reaction Methods 0.000 claims description 26
- 230000003647 oxidation Effects 0.000 claims description 25
- 229910052737 gold Inorganic materials 0.000 claims description 15
- 239000000758 substrate Substances 0.000 claims description 9
- 229910000510 noble metal Inorganic materials 0.000 claims description 5
- 239000003353 gold alloy Substances 0.000 claims description 4
- 238000011144 upstream manufacturing Methods 0.000 claims description 3
- 239000006096 absorbing agent Substances 0.000 claims 1
- 238000012805 post-processing Methods 0.000 claims 1
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 24
- 229910002091 carbon monoxide Inorganic materials 0.000 description 24
- 230000000694 effects Effects 0.000 description 17
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 description 16
- 229910052717 sulfur Inorganic materials 0.000 description 16
- 239000011593 sulfur Substances 0.000 description 16
- 239000007789 gas Substances 0.000 description 15
- 229930195733 hydrocarbon Natural products 0.000 description 14
- 150000002430 hydrocarbons Chemical class 0.000 description 14
- 238000000034 method Methods 0.000 description 12
- 229910018072 Al 2 O 3 Inorganic materials 0.000 description 9
- 229910045601 alloy Inorganic materials 0.000 description 9
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- 239000000446 fuel Substances 0.000 description 7
- 239000000463 material Substances 0.000 description 7
- 230000010718 Oxidation Activity Effects 0.000 description 6
- MWUXSHHQAYIFBG-UHFFFAOYSA-N Nitric oxide Chemical compound O=[N] MWUXSHHQAYIFBG-UHFFFAOYSA-N 0.000 description 5
- 230000032683 aging Effects 0.000 description 5
- 238000006243 chemical reaction Methods 0.000 description 5
- 229910052751 metal Inorganic materials 0.000 description 5
- 239000002184 metal Substances 0.000 description 5
- HBEQXAKJSGXAIQ-UHFFFAOYSA-N oxopalladium Chemical compound [Pd]=O HBEQXAKJSGXAIQ-UHFFFAOYSA-N 0.000 description 5
- 230000009257 reactivity Effects 0.000 description 5
- 230000008929 regeneration Effects 0.000 description 5
- 238000011069 regeneration method Methods 0.000 description 5
- RAHZWNYVWXNFOC-UHFFFAOYSA-N Sulphur dioxide Chemical compound O=S=O RAHZWNYVWXNFOC-UHFFFAOYSA-N 0.000 description 4
- 150000001335 aliphatic alkanes Chemical class 0.000 description 4
- 230000008901 benefit Effects 0.000 description 4
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 4
- 229910003445 palladium oxide Inorganic materials 0.000 description 4
- 229910002710 Au-Pd Inorganic materials 0.000 description 3
- 238000005275 alloying Methods 0.000 description 3
- 230000015572 biosynthetic process Effects 0.000 description 3
- 239000013618 particulate matter Substances 0.000 description 3
- 150000003839 salts Chemical class 0.000 description 3
- 239000004071 soot Substances 0.000 description 3
- 230000019635 sulfation Effects 0.000 description 3
- 238000005670 sulfation reaction Methods 0.000 description 3
- 229910002058 ternary alloy Inorganic materials 0.000 description 3
- 238000003878 thermal aging Methods 0.000 description 3
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 description 2
- 150000001336 alkenes Chemical class 0.000 description 2
- 239000000919 ceramic Substances 0.000 description 2
- 230000000052 comparative effect Effects 0.000 description 2
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- 238000007906 compression Methods 0.000 description 2
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- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 2
- 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 1
- VEXZGXHMUGYJMC-UHFFFAOYSA-M Chloride anion Chemical compound [Cl-] VEXZGXHMUGYJMC-UHFFFAOYSA-M 0.000 description 1
- 241000208125 Nicotiana Species 0.000 description 1
- 235000002637 Nicotiana tabacum Nutrition 0.000 description 1
- 239000011865 Pt-based catalyst Substances 0.000 description 1
- 229910018879 Pt—Pd Inorganic materials 0.000 description 1
- KJTLSVCANCCWHF-UHFFFAOYSA-N Ruthenium Chemical compound [Ru] KJTLSVCANCCWHF-UHFFFAOYSA-N 0.000 description 1
- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 description 1
- QAOWNCQODCNURD-UHFFFAOYSA-L Sulfate Chemical compound [O-]S([O-])(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-L 0.000 description 1
- 238000002441 X-ray diffraction Methods 0.000 description 1
- 229910021536 Zeolite Inorganic materials 0.000 description 1
- 239000002250 absorbent Substances 0.000 description 1
- 230000002745 absorbent Effects 0.000 description 1
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- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 1
- 238000004458 analytical method Methods 0.000 description 1
- 229910052788 barium Inorganic materials 0.000 description 1
- DSAJWYNOEDNPEQ-UHFFFAOYSA-N barium atom Chemical compound [Ba] DSAJWYNOEDNPEQ-UHFFFAOYSA-N 0.000 description 1
- 229910052728 basic metal Inorganic materials 0.000 description 1
- 150000003818 basic metals Chemical class 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 239000003225 biodiesel Substances 0.000 description 1
- -1 bioethanol Substances 0.000 description 1
- 229910052797 bismuth Inorganic materials 0.000 description 1
- JCXGWMGPZLAOME-UHFFFAOYSA-N bismuth atom Chemical compound [Bi] JCXGWMGPZLAOME-UHFFFAOYSA-N 0.000 description 1
- 229910052792 caesium Inorganic materials 0.000 description 1
- TVFDJXOCXUVLDH-UHFFFAOYSA-N caesium atom Chemical compound [Cs] TVFDJXOCXUVLDH-UHFFFAOYSA-N 0.000 description 1
- 229910002092 carbon dioxide Inorganic materials 0.000 description 1
- 239000001569 carbon dioxide Substances 0.000 description 1
- 230000003197 catalytic effect Effects 0.000 description 1
- 239000003638 chemical reducing agent Substances 0.000 description 1
- 239000011248 coating agent Substances 0.000 description 1
- 238000000576 coating method Methods 0.000 description 1
- 238000000354 decomposition reaction Methods 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 238000009792 diffusion process Methods 0.000 description 1
- 239000012895 dilution Substances 0.000 description 1
- 238000010790 dilution Methods 0.000 description 1
- HNPSIPDUKPIQMN-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical compound O=[Si]=O.O=[Al]O[Al]=O HNPSIPDUKPIQMN-UHFFFAOYSA-N 0.000 description 1
- 239000000706 filtrate Substances 0.000 description 1
- 238000010304 firing Methods 0.000 description 1
- 229910052739 hydrogen Inorganic materials 0.000 description 1
- 238000005470 impregnation Methods 0.000 description 1
- 229910052741 iridium Inorganic materials 0.000 description 1
- GKOZUEZYRPOHIO-UHFFFAOYSA-N iridium atom Chemical compound [Ir] GKOZUEZYRPOHIO-UHFFFAOYSA-N 0.000 description 1
- 239000002923 metal particle Substances 0.000 description 1
- 239000011859 microparticle Substances 0.000 description 1
- 238000002156 mixing Methods 0.000 description 1
- UYXRCZUOJAYSQR-UHFFFAOYSA-N nitric acid;platinum Chemical compound [Pt].O[N+]([O-])=O UYXRCZUOJAYSQR-UHFFFAOYSA-N 0.000 description 1
- JCXJVPUVTGWSNB-UHFFFAOYSA-N nitrogen dioxide Inorganic materials O=[N]=O JCXJVPUVTGWSNB-UHFFFAOYSA-N 0.000 description 1
- 229910052762 osmium Inorganic materials 0.000 description 1
- SYQBFIAQOQZEGI-UHFFFAOYSA-N osmium atom Chemical compound [Os] SYQBFIAQOQZEGI-UHFFFAOYSA-N 0.000 description 1
- 239000010412 oxide-supported catalyst Substances 0.000 description 1
- 229910052760 oxygen Inorganic materials 0.000 description 1
- 150000002940 palladium Chemical class 0.000 description 1
- GPNDARIEYHPYAY-UHFFFAOYSA-N palladium(ii) nitrate Chemical compound [Pd+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O GPNDARIEYHPYAY-UHFFFAOYSA-N 0.000 description 1
- 231100000572 poisoning Toxicity 0.000 description 1
- 230000000607 poisoning effect Effects 0.000 description 1
- 238000010248 power generation Methods 0.000 description 1
- 239000002244 precipitate Substances 0.000 description 1
- 238000011084 recovery Methods 0.000 description 1
- 230000009467 reduction Effects 0.000 description 1
- 229910052703 rhodium Inorganic materials 0.000 description 1
- 239000010948 rhodium Substances 0.000 description 1
- MHOVAHRLVXNVSD-UHFFFAOYSA-N rhodium atom Chemical compound [Rh] MHOVAHRLVXNVSD-UHFFFAOYSA-N 0.000 description 1
- 230000005070 ripening Effects 0.000 description 1
- 229910052707 ruthenium Inorganic materials 0.000 description 1
- 229910052709 silver Inorganic materials 0.000 description 1
- 239000004332 silver Substances 0.000 description 1
- 238000005245 sintering Methods 0.000 description 1
- 230000000391 smoking effect Effects 0.000 description 1
- 239000000243 solution Substances 0.000 description 1
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- 238000010998 test method Methods 0.000 description 1
- 238000004627 transmission electron microscopy Methods 0.000 description 1
- 229920001567 vinyl ester resin Polymers 0.000 description 1
- 125000000391 vinyl group Chemical group [H]C([*])=C([H])[H] 0.000 description 1
- 239000010457 zeolite Substances 0.000 description 1
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Abstract
Description
実施例1−準備
2.5重量%のほんの僅かな金属充填でAl2O3上に分散された一連のPd−Au触媒と、0:1〜1:0のPd:Auの原子組成が特徴付けられた。サンプルは次のように準備された。硝酸パラジウムと微粒子のアルミナ担体を含有するHAuCl4の水性混合物に塩基が添加され、担体上で金をAu0として加水分解し、沈殿させた。その懸濁液は適切な期間後、ろ過され、そのろ液は洗浄され、塩化物イオンを取り除き、その物質は乾燥され次に焼成された。この技術によって準備された触媒は本明細書で「フレッシュ」触媒と呼ばれる。
実施例1によって準備された触媒と同じように、水性白金とパラジウム塩の混合物と担体の含浸により準備、乾燥、焼成された1.7Pt−0.8Pd/Al2O3触媒が標準(物質)用として使用された。
実施例1の方法によって準備されたフレッシュ触媒と参照用のPt:Pd触媒は48時間空気中で650℃、750℃又は800℃で熟成された。
リーン水熱熟成(LHA)は750℃で4.5%水、残りは空気中で48時間行われた。
触媒は次の入口ガス混合物(1000ppm CO,900ppm HC(C3H6 又は C1としてn―C8H18)、200ppm NO、2ppm SO2、12%O2、4.5%CO2、4.5%H2O そして残りN2)を使用して合成触媒活性テスト(SCAT)装置で試験した。
実施例2又は3によって準備した熟成された触媒の硫黄熟成が、触媒の15〜400mgS/g(2〜50g/Lに相当)をガス流中の100−150ppmのSO2と共に300℃で実施例4のSCAT装置を使用して、望ましい暴露レベルまで行われた。硫黄熟成を施した触媒は500℃で20分間、実施例4で表されたそのフルガス混合物の中で再生された。
表3は、実施例1によって準備され、750℃で実施例2によって熟成され(実施例6によって硫黄熟成を施された)及び実施例4によって試験された(炭化水素としてC3H6を使用して)触媒について行われた活性テストの結果を示している。T80とT50は、その触媒がCO又は炭化水素(HC)をそれぞれ80%又は50%の変換効率で酸化させる温度であることを理解できる。
表4は、実施例1によって準備されたフレッシュPdだけの触媒、実施例2、3、5によって準備された熟成された2Au−0.5Pd/Al2O3触媒の活性を比較した結果を示している。テストは実施例4に従って行われた(炭化水素としてC3H6を使用した)。
図3と4は、実施例1と参照に従って準備され、実施例2によって750℃で熟成させた触媒と参照触媒に対して行われた実施例4(炭化水素としてn―C8H18を使用した)によるテスト方法の結果を示す。図3から、1.7Pt−0.8Pd、2Au−0.5Pd及び1.7Au−0.8Pdの触媒に対するアルカンの変換活性は類似しているが、Pdだけの触媒は著しく活性が小さく、Auだけの触媒は更に活性が小さいことが理解できる。
実施例1によって準備されたPd−Au/Al2O3のサンプルを白金硝酸水溶液と共に湿式含浸し、望ましいPt充填を行った。その結果生じる物質を次に乾燥し、焼成した。
実施例10によって準備されたPt−Pd−Au/Al2O3の触媒を実施例2によって750℃で熟成し、実施例4と5に従って試験した。その結果は表5に示しており、その結果から全てのクリーンな触媒の活性は類似していることが理解される。しかし、硫黄暴露に続いて、0.5Pt−0.8Pd−1.2Auと0.2Pt−0.8Pd−1.5Auのサンプルは活性において大変類似した損失を示すが、0.9Pt−0.8Pd−0.8Auのサンプルは、前者の二つの触媒のいずれと比べても、約20℃、より良いCOT80値と約10℃、より良いHCT50値を有する。増加するAu含有量は硫黄再生活性を改善するが、耐硫黄性は減少する。試験される物質のいずれも合金であるかどうかは現時点では知られていない。しかし、Pd−AuにPtを大量に添加することの僅かな利点はあるように見えるが、著しいコスト対利点がないように見える。
Claims (13)
- リーンバーン内燃エンジンと排気システムを備えてなる装置であって、
前記排気システムが、一以上の触媒後処理構成材を備えてなり、
前記一以上の触媒後処理構成材が、金属酸化物担体上に、パラジウムと金とからなる合金を含んでなる触媒組成物を含んでなるものである、装置。 - 前記触媒組成物におけるAu:Pdの原子比率が9:1〜1:9である、請求項1に記載された装置。
- 前記触媒組成物におけるAu:Pdの原子比率が5:1〜1:5である、請求項2に記載された装置。
- 前記触媒組成物においてAu:Pdの原子比率が2:1〜1:2である、請求項2又は3に記載された装置。
- 前記触媒組成物に存在する貴金属の重量%が0.5〜10.0である、請求項1〜4の何れか一項に記載された装置。
- 前記触媒組成物において存在する貴金属の重量%が1.0〜5.0である、請求項5に記載された装置。
- 前記触媒組成物が、前記パラジウムと金の合金から、分離され、かつ、区別された金属酸化物担体上に配置された白金を含んでなる、請求項1〜6の何れか一項に記載された装置。
- 前記白金含有金属酸化物担体がパラジウムも含んでなる、請求項7に記載された装置。
- 第一金属酸化物担体における金とパラジウムと、及び第二金属酸化物担体における白金と任意のパラジウムが同じウオッシュコート層で配置されてなる、請求項7又は8に記載された装置。
- 前記第二金属酸化物担体上における白金と任意のパラジウムが、前記第一金属酸化物担体におけるパラジウムと金の合金を含んでなるオーバーレイヤーの下に、層中に配置されてなる、請求項7又は8に記載された装置。
- 前記第二金属酸化物担体における白金と任意のパラジウムが、前記第一金属酸化物担体における金とパラジウムの合金を含んでなる領域の上流に、基材モノリスの上流の領域に配置されてなる、請求項7又は8に記載された装置。
- 少なくとも一つの触媒後処理構成材が、酸化触媒、リーンNOx触媒又はNOx吸収材を備えてなる、請求項1〜12の何れか一項に記載された装置。
- 前記触媒後処理構成材が、フィルター基材モノリス又はフロースルー基材モノリスを備えてなる、請求項1〜12の何れか一項に記載された装置。
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GB0809233.0 | 2008-05-21 | ||
PCT/GB2009/050485 WO2009136206A1 (en) | 2008-05-09 | 2009-05-08 | Exhaust system for lean-burn internal combustion engine comprising pd-au-alloy catalyst |
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DE (1) | DE112009001056T5 (ja) |
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GB0808427D0 (en) | 2008-06-18 |
BRPI0911802A2 (pt) | 2015-10-06 |
DE112009001056T5 (de) | 2011-03-10 |
RU2010150354A (ru) | 2012-06-20 |
GB201015800D0 (en) | 2010-10-27 |
CN102015075B (zh) | 2013-12-25 |
GB2471409B (en) | 2013-03-06 |
RU2506988C2 (ru) | 2014-02-20 |
KR20110010720A (ko) | 2011-02-07 |
US8551411B2 (en) | 2013-10-08 |
US20110173959A1 (en) | 2011-07-21 |
EP2274074B1 (en) | 2013-04-24 |
EP2274074A1 (en) | 2011-01-19 |
WO2009136206A1 (en) | 2009-11-12 |
CN102015075A (zh) | 2011-04-13 |
KR101553425B1 (ko) | 2015-09-15 |
GB2471409A (en) | 2010-12-29 |
GB0809233D0 (en) | 2008-06-25 |
JP5771521B2 (ja) | 2015-09-02 |
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