JP2016522739A - Nox吸蔵触媒の脱硫 - Google Patents
Nox吸蔵触媒の脱硫 Download PDFInfo
- Publication number
- JP2016522739A JP2016522739A JP2016509399A JP2016509399A JP2016522739A JP 2016522739 A JP2016522739 A JP 2016522739A JP 2016509399 A JP2016509399 A JP 2016509399A JP 2016509399 A JP2016509399 A JP 2016509399A JP 2016522739 A JP2016522739 A JP 2016522739A
- Authority
- JP
- Japan
- Prior art keywords
- desulfurization
- storage catalyst
- catalyst
- cerium
- oxide
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Ceased
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- 239000003054 catalyst Substances 0.000 title claims abstract description 113
- 238000006477 desulfuration reaction Methods 0.000 title claims abstract description 49
- 230000023556 desulfurization Effects 0.000 title claims abstract description 49
- 238000000034 method Methods 0.000 claims abstract description 30
- 230000018537 nitric oxide storage Effects 0.000 claims abstract description 24
- MWUXSHHQAYIFBG-UHFFFAOYSA-N Nitric oxide Chemical compound O=[N] MWUXSHHQAYIFBG-UHFFFAOYSA-N 0.000 claims description 209
- 239000007789 gas Substances 0.000 claims description 41
- 239000000446 fuel Substances 0.000 claims description 29
- 239000011232 storage material Substances 0.000 claims description 23
- 239000000463 material Substances 0.000 claims description 13
- 229910052784 alkaline earth metal Inorganic materials 0.000 claims description 12
- 150000001342 alkaline earth metals Chemical class 0.000 claims description 12
- 229910052684 Cerium Inorganic materials 0.000 claims description 11
- GWXLDORMOJMVQZ-UHFFFAOYSA-N cerium Chemical compound [Ce] GWXLDORMOJMVQZ-UHFFFAOYSA-N 0.000 claims description 11
- 238000002485 combustion reaction Methods 0.000 claims description 11
- 229910000420 cerium oxide Inorganic materials 0.000 claims description 9
- BMMGVYCKOGBVEV-UHFFFAOYSA-N oxo(oxoceriooxy)cerium Chemical compound [Ce]=O.O=[Ce]=O BMMGVYCKOGBVEV-UHFFFAOYSA-N 0.000 claims description 9
- RCFVMJKOEJFGTM-UHFFFAOYSA-N cerium zirconium Chemical compound [Zr].[Ce] RCFVMJKOEJFGTM-UHFFFAOYSA-N 0.000 claims description 4
- 238000000746 purification Methods 0.000 claims description 4
- 229910052788 barium Inorganic materials 0.000 claims description 3
- DSAJWYNOEDNPEQ-UHFFFAOYSA-N barium atom Chemical compound [Ba] DSAJWYNOEDNPEQ-UHFFFAOYSA-N 0.000 claims description 2
- 229910052791 calcium Inorganic materials 0.000 claims description 2
- 229910052749 magnesium Inorganic materials 0.000 claims description 2
- 239000011777 magnesium Substances 0.000 claims description 2
- 229910052712 strontium Inorganic materials 0.000 claims description 2
- OYPRJOBELJOOCE-UHFFFAOYSA-N Calcium Chemical compound [Ca] OYPRJOBELJOOCE-UHFFFAOYSA-N 0.000 claims 1
- FYYHWMGAXLPEAU-UHFFFAOYSA-N Magnesium Chemical compound [Mg] FYYHWMGAXLPEAU-UHFFFAOYSA-N 0.000 claims 1
- 239000011575 calcium Substances 0.000 claims 1
- CIOAGBVUUVVLOB-UHFFFAOYSA-N strontium atom Chemical compound [Sr] CIOAGBVUUVVLOB-UHFFFAOYSA-N 0.000 claims 1
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 description 18
- 229910052717 sulfur Inorganic materials 0.000 description 18
- 239000011593 sulfur Substances 0.000 description 18
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical group [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 description 16
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 10
- 229910052760 oxygen Inorganic materials 0.000 description 10
- 239000001301 oxygen Substances 0.000 description 10
- KDLHZDBZIXYQEI-UHFFFAOYSA-N palladium Substances [Pd] KDLHZDBZIXYQEI-UHFFFAOYSA-N 0.000 description 10
- 230000008929 regeneration Effects 0.000 description 10
- 238000011069 regeneration method Methods 0.000 description 10
- 239000000758 substrate Substances 0.000 description 10
- 229910052697 platinum Inorganic materials 0.000 description 9
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 description 8
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 8
- RAHZWNYVWXNFOC-UHFFFAOYSA-N Sulphur dioxide Chemical compound O=S=O RAHZWNYVWXNFOC-UHFFFAOYSA-N 0.000 description 8
- 229910052763 palladium Inorganic materials 0.000 description 7
- 239000010948 rhodium Substances 0.000 description 7
- QVQLCTNNEUAWMS-UHFFFAOYSA-N barium oxide Chemical compound [Ba]=O QVQLCTNNEUAWMS-UHFFFAOYSA-N 0.000 description 6
- 238000006243 chemical reaction Methods 0.000 description 6
- 239000000203 mixture Substances 0.000 description 6
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 5
- 229910002091 carbon monoxide Inorganic materials 0.000 description 5
- 229930195733 hydrocarbon Natural products 0.000 description 5
- 150000002430 hydrocarbons Chemical class 0.000 description 5
- 229910052703 rhodium Inorganic materials 0.000 description 5
- 238000012360 testing method Methods 0.000 description 5
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 description 4
- 229910002651 NO3 Inorganic materials 0.000 description 4
- NHNBFGGVMKEFGY-UHFFFAOYSA-N Nitrate Chemical compound [O-][N+]([O-])=O NHNBFGGVMKEFGY-UHFFFAOYSA-N 0.000 description 4
- 229910000287 alkaline earth metal oxide Inorganic materials 0.000 description 4
- 229910021529 ammonia Inorganic materials 0.000 description 4
- 239000000919 ceramic Substances 0.000 description 4
- 238000002474 experimental method Methods 0.000 description 4
- FZLIPJUXYLNCLC-UHFFFAOYSA-N lanthanum atom Chemical compound [La] FZLIPJUXYLNCLC-UHFFFAOYSA-N 0.000 description 4
- CPLXHLVBOLITMK-UHFFFAOYSA-N magnesium oxide Inorganic materials [Mg]=O CPLXHLVBOLITMK-UHFFFAOYSA-N 0.000 description 4
- 229910052751 metal Inorganic materials 0.000 description 4
- 239000002184 metal Substances 0.000 description 4
- 229910052757 nitrogen Inorganic materials 0.000 description 4
- 229910000510 noble metal Inorganic materials 0.000 description 4
- TWNQGVIAIRXVLR-UHFFFAOYSA-N oxo(oxoalumanyloxy)alumane Chemical compound O=[Al]O[Al]=O TWNQGVIAIRXVLR-UHFFFAOYSA-N 0.000 description 4
- XTQHKBHJIVJGKJ-UHFFFAOYSA-N sulfur monoxide Chemical compound S=O XTQHKBHJIVJGKJ-UHFFFAOYSA-N 0.000 description 4
- 229910052815 sulfur oxide Inorganic materials 0.000 description 4
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 4
- 229910001868 water Inorganic materials 0.000 description 4
- RWSOTUBLDIXVET-UHFFFAOYSA-N Dihydrogen sulfide Chemical compound S RWSOTUBLDIXVET-UHFFFAOYSA-N 0.000 description 3
- 230000015572 biosynthetic process Effects 0.000 description 3
- 150000004649 carbonic acid derivatives Chemical class 0.000 description 3
- 150000001875 compounds Chemical class 0.000 description 3
- 230000007423 decrease Effects 0.000 description 3
- 238000011161 development Methods 0.000 description 3
- 230000018109 developmental process Effects 0.000 description 3
- 239000003344 environmental pollutant Substances 0.000 description 3
- 238000010438 heat treatment Methods 0.000 description 3
- 229910000037 hydrogen sulfide Inorganic materials 0.000 description 3
- 150000004679 hydroxides Chemical class 0.000 description 3
- 239000000395 magnesium oxide Substances 0.000 description 3
- 231100000719 pollutant Toxicity 0.000 description 3
- 229910052761 rare earth metal Inorganic materials 0.000 description 3
- QAOWNCQODCNURD-UHFFFAOYSA-L Sulfate Chemical compound [O-]S([O-])(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-L 0.000 description 2
- 229910052783 alkali metal Inorganic materials 0.000 description 2
- 150000001340 alkali metals Chemical class 0.000 description 2
- 229910002092 carbon dioxide Inorganic materials 0.000 description 2
- 239000001569 carbon dioxide Substances 0.000 description 2
- 239000003638 chemical reducing agent Substances 0.000 description 2
- 239000011248 coating agent Substances 0.000 description 2
- 238000000576 coating method Methods 0.000 description 2
- 230000001419 dependent effect Effects 0.000 description 2
- 208000028659 discharge Diseases 0.000 description 2
- 229910052746 lanthanum Inorganic materials 0.000 description 2
- MRELNEQAGSRDBK-UHFFFAOYSA-N lanthanum oxide Inorganic materials [O-2].[O-2].[O-2].[La+3].[La+3] MRELNEQAGSRDBK-UHFFFAOYSA-N 0.000 description 2
- AXZKOIWUVFPNLO-UHFFFAOYSA-N magnesium;oxygen(2-) Chemical compound [O-2].[Mg+2] AXZKOIWUVFPNLO-UHFFFAOYSA-N 0.000 description 2
- 229910044991 metal oxide Inorganic materials 0.000 description 2
- 150000004706 metal oxides Chemical group 0.000 description 2
- VUZPPFZMUPKLLV-UHFFFAOYSA-N methane;hydrate Chemical compound C.O VUZPPFZMUPKLLV-UHFFFAOYSA-N 0.000 description 2
- 150000002823 nitrates Chemical class 0.000 description 2
- MMKQUGHLEMYQSG-UHFFFAOYSA-N oxygen(2-);praseodymium(3+) Chemical compound [O-2].[O-2].[O-2].[Pr+3].[Pr+3] MMKQUGHLEMYQSG-UHFFFAOYSA-N 0.000 description 2
- 229910003447 praseodymium oxide Inorganic materials 0.000 description 2
- 150000002910 rare earth metals Chemical class 0.000 description 2
- MHOVAHRLVXNVSD-UHFFFAOYSA-N rhodium atom Chemical compound [Rh] MHOVAHRLVXNVSD-UHFFFAOYSA-N 0.000 description 2
- 150000003464 sulfur compounds Chemical class 0.000 description 2
- 238000003786 synthesis reaction Methods 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
- 229910018072 Al 2 O 3 Inorganic materials 0.000 description 1
- 239000004215 Carbon black (E152) Substances 0.000 description 1
- 238000005033 Fourier transform infrared spectroscopy Methods 0.000 description 1
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 1
- 230000032683 aging Effects 0.000 description 1
- SNAAJJQQZSMGQD-UHFFFAOYSA-N aluminum magnesium Chemical compound [Mg].[Al] SNAAJJQQZSMGQD-UHFFFAOYSA-N 0.000 description 1
- 239000002585 base Substances 0.000 description 1
- 150000007514 bases Chemical class 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 230000033228 biological regulation Effects 0.000 description 1
- 238000010531 catalytic reduction reaction Methods 0.000 description 1
- 239000012141 concentrate Substances 0.000 description 1
- 238000001816 cooling Methods 0.000 description 1
- 230000002950 deficient Effects 0.000 description 1
- 230000008021 deposition Effects 0.000 description 1
- TXKMVPPZCYKFAC-UHFFFAOYSA-N disulfur monoxide Inorganic materials O=S=S TXKMVPPZCYKFAC-UHFFFAOYSA-N 0.000 description 1
- 238000011156 evaluation Methods 0.000 description 1
- 238000000605 extraction Methods 0.000 description 1
- 230000002349 favourable effect Effects 0.000 description 1
- 238000011049 filling Methods 0.000 description 1
- 239000000796 flavoring agent Substances 0.000 description 1
- 239000000295 fuel oil Substances 0.000 description 1
- 239000001257 hydrogen Substances 0.000 description 1
- 229910052739 hydrogen Inorganic materials 0.000 description 1
- 238000002347 injection Methods 0.000 description 1
- 239000007924 injection Substances 0.000 description 1
- 238000005259 measurement Methods 0.000 description 1
- 239000010705 motor oil Substances 0.000 description 1
- JCXJVPUVTGWSNB-UHFFFAOYSA-N nitrogen dioxide Inorganic materials O=[N]=O JCXJVPUVTGWSNB-UHFFFAOYSA-N 0.000 description 1
- 150000002898 organic sulfur compounds Chemical class 0.000 description 1
- 231100000572 poisoning Toxicity 0.000 description 1
- 230000000607 poisoning effect Effects 0.000 description 1
- 239000011148 porous material Substances 0.000 description 1
- 238000006722 reduction reaction Methods 0.000 description 1
- 230000001172 regenerating effect Effects 0.000 description 1
- 238000011160 research Methods 0.000 description 1
- 239000000523 sample Substances 0.000 description 1
- 229910052596 spinel Inorganic materials 0.000 description 1
- 239000011029 spinel Substances 0.000 description 1
- 239000007921 spray Substances 0.000 description 1
- IATRAKWUXMZMIY-UHFFFAOYSA-N strontium oxide Chemical class [O-2].[Sr+2] IATRAKWUXMZMIY-UHFFFAOYSA-N 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 150000003467 sulfuric acid derivatives Chemical class 0.000 description 1
- 230000008685 targeting Effects 0.000 description 1
- 239000002341 toxic gas Substances 0.000 description 1
- 230000001960 triggered effect Effects 0.000 description 1
- 238000011144 upstream manufacturing Methods 0.000 description 1
Classifications
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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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Abstract
Description
λ<1(例えば0.9)は「空気不足」:濃い混合ガス又は濃すぎる混合ガスを意味する。
λ>1(例えば1.1)は「空気過剰」:リーン又は薄い混合ガスを意味する。
述部:λ=1.1は、化学量論的な反応に必要とされる量より10%多い空気が燃焼に関与していることを意味する。同時にこれは空気過剰である。
−リーンモードでの運転が少なくとも5〜10分;
−A/F=0.995〜1.0(±0.005以内の振れ幅)、少なくとも10〜20分;
−リーンモードでの運転が少なくとも2〜5分;
−A/F=0.995〜1.0(±0.005以内の振れ幅)、少なくとも10〜30分;
触媒2を作成するために、ハチの巣状のセラミック基板を、17g/Lの酸化バリウム、15g/Lの酸化マグネシウムとともに、ランタン安定化酸化アルミニウムで担持されたPt、Pd、及びRhと116g/Lの酸化セリウムを含む第1のウォッシュコート層Aにより被覆した。Pt及びPdの量は、50g/cft(1.766g/L)、5g/cft(0.177g/L)であり、ウォッシュコート層の合計量は、セラミック基板の体積に対して181g/Lであった。追加のウォッシュコート層Bを、第1のウォッシュコート層に塗布した。追加のウォッシュコート層Bは、同様に、ランタン安定化酸化アルミニウムに担持されたRhとともに、Pt及びPdを含んでいた。このウォッシュコート層内のPt、Pd、及びRhの量は、それぞれ50g/cft(1.766g/L)、5g/cft(0.177g/L)、及び5g/cft(0.177g/L)であった。ウォッシュコート層Bは、層Bのウォッシュコートの量181g/Lに対し、93g/L酸化セリウムを更に含んでいた。
試験は、ハイダイナミックエンジン試験台で実施する。エンジンは、スプレーガイド方式、成層燃焼プロセスの直接噴射式ガソリンエンジンである。高濃度の含硫黄燃料(硫黄200ppm)を使用して、それぞれの硫黄の規定量が、一定のエンジン動作点と適度な触媒温度(250〜350℃)において、触媒に適用する(SOx法)。
試験は、合成により作られた排気ガスを用いて、動的合成排気ガス装置で実施する。実験において、加熱された触媒1又は触媒2を、7.5℃/分の速度で冷却する。冷却中、特定の時間範囲内において吸蔵と再生(抽出)を交互に行う。本件で定数と定められているNOx濃度は、500ppmである。それぞれの場合の評価は、リーン/リッチサイクルで行い、転換率を触媒温度の関数として、NOx初期濃度の500ppmに対して示す。
試験は、ハイダイナミック合成ガス装置で実施する。ここでは、自動車の排出プロファイル(排出、温度、質量流量、車両の触媒体積等)が、1:5〜1:50という特定の値で合成ガス装置に運ばれ(適用され)、両方の触媒(1と2)で転換挙動を試験した。合成ガス装置と車両との間の様々な相互比較で、それぞれ対応するスケールにおいてその転換挙動が良く相関することが判明した。
Claims (9)
- 主にリーンバーン燃焼エンジンの排気ガス浄化に使用されるNOx吸蔵触媒の標的化脱硫方法の使用であって、前記NOx吸蔵触媒は、セリウムを含む酸化窒素吸蔵触媒とアルカリ土類金属を含む吸蔵触媒の重量比が10:1〜20:1であるセリウム及びアルカリ土類金属を含む酸化窒素吸蔵触媒を含み、
0.98≦λ≦1.0のA/F範囲で、平均温度≧500℃で脱硫される、NOx吸蔵触媒の標的化脱硫方法の使用。 - 前記NOx吸蔵触媒が、酸化セリウム、セリウム−ジルコニウム混合酸化物、希土類の添加された酸化セリウム、及びそれらの組み合わせを含む群から選択されるセリウムを含む酸化窒素吸蔵触媒を含む、請求項1に記載の使用。
- 前記NOx吸蔵触媒が、アルカリ土類金属を含む酸化窒素吸蔵材料を含み、前記材料中の前記アルカリ土類金属がバリウム、カルシウム、ストロンチウム、及びマグネシウムからなる群から選択される、請求項1及び/又は2に記載の使用。
- 前記脱硫中の温度が500℃〜800℃であることを特徴とする、請求項1〜3の一つ以上に記載の使用。
- 前記脱硫中に調整された空燃比は、0.5〜20Hzの周波数を用いて変調されることを特徴とする、請求項1〜4の一つ以上に記載の使用。
- 前記脱硫中における変調が、前記調整された空燃比(λ)の振れ幅±0.05以内で実施されることを特徴とする、請求項5に記載の使用。
- 前記酸化窒素吸蔵触媒の脱硫での前記排気ガスは、温度を前記脱硫温度まで上昇させるために、前記エンジンを用いて追加的に濃縮されないことを特徴とする、請求項1〜6の一つ以上に記載の使用。
- 前記脱硫が、通常の運転状態で実施され、前記リーンバーンガソリンエンジンが、請求項1に記載の範囲内で運転されることを特徴とする、請求項7に記載の使用。
- 前記エンジンの少なくとも4つの運転段階が交互に交代し、リーン段階の後に脱硫段階(λ=0.995〜1.0(振れ幅±0.005以内))が行われ、個々の前記運転段階が5〜30分の範囲で継続することを特徴とする、請求項1〜6の一つ以上に記載の使用。
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DE102016101761A1 (de) * | 2016-02-02 | 2017-08-03 | Umicore Ag & Co. Kg | Katalysator zur Reduktion von Stickoxiden |
WO2017144426A1 (de) * | 2016-02-22 | 2017-08-31 | Umicore Ag & Co. Kg | Katalysator zur reduktion von stickoxiden |
DE102016203225A1 (de) * | 2016-02-29 | 2017-08-31 | Robert Bosch Gmbh | Verfahren zum Betreiben eines Abgasnachbehandlungssystems eines Kraftfahrzeugs |
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