JP7433416B2 - 燃焼エンジンの排気ガスからのアンモニア及び窒素酸化物の排出量低減のための触媒 - Google Patents
燃焼エンジンの排気ガスからのアンモニア及び窒素酸化物の排出量低減のための触媒 Download PDFInfo
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- JP7433416B2 JP7433416B2 JP2022511059A JP2022511059A JP7433416B2 JP 7433416 B2 JP7433416 B2 JP 7433416B2 JP 2022511059 A JP2022511059 A JP 2022511059A JP 2022511059 A JP2022511059 A JP 2022511059A JP 7433416 B2 JP7433416 B2 JP 7433416B2
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- catalyst
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- platinum
- oxide
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- 239000003054 catalyst Substances 0.000 title claims description 75
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 title claims description 58
- 229910021529 ammonia Inorganic materials 0.000 title claims description 28
- MWUXSHHQAYIFBG-UHFFFAOYSA-N Nitric oxide Chemical compound O=[N] MWUXSHHQAYIFBG-UHFFFAOYSA-N 0.000 title claims description 21
- 239000007789 gas Substances 0.000 title claims description 12
- 238000002485 combustion reaction Methods 0.000 title description 3
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 claims description 83
- 239000000463 material Substances 0.000 claims description 44
- 239000010457 zeolite Substances 0.000 claims description 39
- 229910052697 platinum Inorganic materials 0.000 claims description 38
- HNPSIPDUKPIQMN-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical compound O=[Si]=O.O=[Al]O[Al]=O HNPSIPDUKPIQMN-UHFFFAOYSA-N 0.000 claims description 35
- 239000000758 substrate Substances 0.000 claims description 35
- 239000010949 copper Substances 0.000 claims description 33
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 claims description 31
- 229910021536 Zeolite Inorganic materials 0.000 claims description 29
- KDLHZDBZIXYQEI-UHFFFAOYSA-N Palladium Chemical compound [Pd] KDLHZDBZIXYQEI-UHFFFAOYSA-N 0.000 claims description 24
- 229910052802 copper Inorganic materials 0.000 claims description 21
- OGIDPMRJRNCKJF-UHFFFAOYSA-N titanium oxide Inorganic materials [Ti]=O OGIDPMRJRNCKJF-UHFFFAOYSA-N 0.000 claims description 21
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 claims description 20
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims description 20
- 239000002245 particle Substances 0.000 claims description 16
- 229910052763 palladium Inorganic materials 0.000 claims description 10
- TWNQGVIAIRXVLR-UHFFFAOYSA-N oxo(oxoalumanyloxy)alumane Chemical compound O=[Al]O[Al]=O TWNQGVIAIRXVLR-UHFFFAOYSA-N 0.000 claims description 9
- 229910052814 silicon oxide Inorganic materials 0.000 claims description 8
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims description 7
- 239000000377 silicon dioxide Substances 0.000 claims description 6
- 239000002243 precursor Substances 0.000 claims description 5
- RVTZCBVAJQQJTK-UHFFFAOYSA-N oxygen(2-);zirconium(4+) Chemical compound [O-2].[O-2].[Zr+4] RVTZCBVAJQQJTK-UHFFFAOYSA-N 0.000 claims description 3
- 229910001928 zirconium oxide Inorganic materials 0.000 claims description 3
- 229910000420 cerium oxide Inorganic materials 0.000 claims description 2
- BMMGVYCKOGBVEV-UHFFFAOYSA-N oxo(oxoceriooxy)cerium Chemical compound [Ce]=O.O=[Ce]=O BMMGVYCKOGBVEV-UHFFFAOYSA-N 0.000 claims description 2
- GQPLMRYTRLFLPF-UHFFFAOYSA-N Nitrous Oxide Chemical compound [O-][N+]#N GQPLMRYTRLFLPF-UHFFFAOYSA-N 0.000 description 22
- 239000011148 porous material Substances 0.000 description 16
- 235000013842 nitrous oxide Nutrition 0.000 description 11
- 230000003647 oxidation Effects 0.000 description 9
- 238000007254 oxidation reaction Methods 0.000 description 9
- 238000006243 chemical reaction Methods 0.000 description 8
- 238000000576 coating method Methods 0.000 description 8
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 6
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 6
- 239000011248 coating agent Substances 0.000 description 6
- QPLDLSVMHZLSFG-UHFFFAOYSA-N Copper oxide Chemical compound [Cu]=O QPLDLSVMHZLSFG-UHFFFAOYSA-N 0.000 description 5
- 229910052760 oxygen Inorganic materials 0.000 description 5
- 239000000843 powder Substances 0.000 description 5
- 230000015572 biosynthetic process Effects 0.000 description 4
- 239000011149 active material Substances 0.000 description 3
- 239000007864 aqueous solution Substances 0.000 description 3
- 239000002657 fibrous material Substances 0.000 description 3
- 229910052742 iron Inorganic materials 0.000 description 3
- 238000002844 melting Methods 0.000 description 3
- 239000002808 molecular sieve Substances 0.000 description 3
- 229910052757 nitrogen Inorganic materials 0.000 description 3
- 229910000510 noble metal Inorganic materials 0.000 description 3
- URGAHOPLAPQHLN-UHFFFAOYSA-N sodium aluminosilicate Chemical compound [Na+].[Al+3].[O-][Si]([O-])=O.[O-][Si]([O-])=O URGAHOPLAPQHLN-UHFFFAOYSA-N 0.000 description 3
- 239000000126 substance Substances 0.000 description 3
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 3
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 2
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 description 2
- XSQUKJJJFZCRTK-UHFFFAOYSA-N Urea Chemical compound NC(N)=O XSQUKJJJFZCRTK-UHFFFAOYSA-N 0.000 description 2
- 238000002441 X-ray diffraction Methods 0.000 description 2
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 2
- 239000011230 binding agent Substances 0.000 description 2
- 239000004202 carbamide Substances 0.000 description 2
- 229910002091 carbon monoxide Inorganic materials 0.000 description 2
- 230000000052 comparative effect Effects 0.000 description 2
- 150000001875 compounds Chemical class 0.000 description 2
- 238000000151 deposition Methods 0.000 description 2
- 238000002474 experimental method Methods 0.000 description 2
- 239000000835 fiber Substances 0.000 description 2
- 229930195733 hydrocarbon Natural products 0.000 description 2
- 150000002430 hydrocarbons Chemical class 0.000 description 2
- 238000011068 loading method Methods 0.000 description 2
- 238000004519 manufacturing process Methods 0.000 description 2
- 230000008018 melting Effects 0.000 description 2
- 229910044991 metal oxide Inorganic materials 0.000 description 2
- 150000004706 metal oxides Chemical class 0.000 description 2
- 239000001301 oxygen Substances 0.000 description 2
- 229910052710 silicon Inorganic materials 0.000 description 2
- 239000010703 silicon Substances 0.000 description 2
- 229910000505 Al2TiO5 Inorganic materials 0.000 description 1
- 241000269350 Anura Species 0.000 description 1
- 239000005751 Copper oxide Substances 0.000 description 1
- 229910021193 La 2 O 3 Inorganic materials 0.000 description 1
- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 description 1
- 230000010718 Oxidation Activity Effects 0.000 description 1
- 229910004283 SiO 4 Inorganic materials 0.000 description 1
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 description 1
- AZDRQVAHHNSJOQ-UHFFFAOYSA-N alumane Chemical group [AlH3] AZDRQVAHHNSJOQ-UHFFFAOYSA-N 0.000 description 1
- BVCZEBOGSOYJJT-UHFFFAOYSA-N ammonium carbamate Chemical compound [NH4+].NC([O-])=O BVCZEBOGSOYJJT-UHFFFAOYSA-N 0.000 description 1
- VZTDIZULWFCMLS-UHFFFAOYSA-N ammonium formate Chemical compound [NH4+].[O-]C=O VZTDIZULWFCMLS-UHFFFAOYSA-N 0.000 description 1
- 238000001354 calcination Methods 0.000 description 1
- KXDHJXZQYSOELW-UHFFFAOYSA-N carbonic acid monoamide Natural products NC(O)=O KXDHJXZQYSOELW-UHFFFAOYSA-N 0.000 description 1
- 230000003197 catalytic effect Effects 0.000 description 1
- 238000006555 catalytic reaction Methods 0.000 description 1
- 239000000919 ceramic Substances 0.000 description 1
- 239000003638 chemical reducing agent Substances 0.000 description 1
- 239000000470 constituent Substances 0.000 description 1
- -1 copper cations Chemical class 0.000 description 1
- 229910000431 copper oxide Inorganic materials 0.000 description 1
- 229910052878 cordierite Inorganic materials 0.000 description 1
- JSKIRARMQDRGJZ-UHFFFAOYSA-N dimagnesium dioxido-bis[(1-oxido-3-oxo-2,4,6,8,9-pentaoxa-1,3-disila-5,7-dialuminabicyclo[3.3.1]nonan-7-yl)oxy]silane Chemical compound [Mg++].[Mg++].[O-][Si]([O-])(O[Al]1O[Al]2O[Si](=O)O[Si]([O-])(O1)O2)O[Al]1O[Al]2O[Si](=O)O[Si]([O-])(O1)O2 JSKIRARMQDRGJZ-UHFFFAOYSA-N 0.000 description 1
- 238000003618 dip coating Methods 0.000 description 1
- 238000001035 drying Methods 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 239000000446 fuel Substances 0.000 description 1
- 239000003365 glass fiber Substances 0.000 description 1
- 238000010438 heat treatment Methods 0.000 description 1
- 238000010030 laminating Methods 0.000 description 1
- 229910052746 lanthanum Inorganic materials 0.000 description 1
- FZLIPJUXYLNCLC-UHFFFAOYSA-N lanthanum atom Chemical compound [La] FZLIPJUXYLNCLC-UHFFFAOYSA-N 0.000 description 1
- 238000013507 mapping Methods 0.000 description 1
- 238000000034 method Methods 0.000 description 1
- 229910017604 nitric acid Inorganic materials 0.000 description 1
- 229910000069 nitrogen hydride Inorganic materials 0.000 description 1
- 229960001730 nitrous oxide Drugs 0.000 description 1
- 125000004430 oxygen atom Chemical group O* 0.000 description 1
- 150000003058 platinum compounds Chemical class 0.000 description 1
- 230000001376 precipitating effect Effects 0.000 description 1
- AABBHSMFGKYLKE-SNAWJCMRSA-N propan-2-yl (e)-but-2-enoate Chemical compound C\C=C\C(=O)OC(C)C AABBHSMFGKYLKE-SNAWJCMRSA-N 0.000 description 1
- 238000000746 purification Methods 0.000 description 1
- 230000001105 regulatory effect Effects 0.000 description 1
- HBMJWWWQQXIZIP-UHFFFAOYSA-N silicon carbide Chemical compound [Si+]#[C-] HBMJWWWQQXIZIP-UHFFFAOYSA-N 0.000 description 1
- 229910010271 silicon carbide Inorganic materials 0.000 description 1
- 235000012239 silicon dioxide Nutrition 0.000 description 1
- 239000000243 solution Substances 0.000 description 1
- 239000004071 soot Substances 0.000 description 1
- 241000894007 species Species 0.000 description 1
- CBXCPBUEXACCNR-UHFFFAOYSA-N tetraethylammonium Chemical compound CC[N+](CC)(CC)CC CBXCPBUEXACCNR-UHFFFAOYSA-N 0.000 description 1
- 229910052719 titanium Inorganic materials 0.000 description 1
- 239000010936 titanium Substances 0.000 description 1
- 239000004408 titanium dioxide Substances 0.000 description 1
- 231100000331 toxic Toxicity 0.000 description 1
- 230000002588 toxic effect Effects 0.000 description 1
- WFKWXMTUELFFGS-UHFFFAOYSA-N tungsten Chemical compound [W] WFKWXMTUELFFGS-UHFFFAOYSA-N 0.000 description 1
- 229910052721 tungsten Inorganic materials 0.000 description 1
- 239000010937 tungsten Substances 0.000 description 1
- 229910052720 vanadium Inorganic materials 0.000 description 1
- GPPXJZIENCGNKB-UHFFFAOYSA-N vanadium Chemical compound [V]#[V] GPPXJZIENCGNKB-UHFFFAOYSA-N 0.000 description 1
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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
- B01J2229/00—Aspects of molecular sieve catalysts not covered by B01J29/00
- B01J2229/30—After treatment, characterised by the means used
- B01J2229/42—Addition of matrix or binder particles
-
- 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
- Y02C—CAPTURE, STORAGE, SEQUESTRATION OR DISPOSAL OF GREENHOUSE GASES [GHG]
- Y02C20/00—Capture or disposal of greenhouse gases
- Y02C20/10—Capture or disposal of greenhouse gases of nitrous oxide (N2O)
-
- 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
- Y02T—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO TRANSPORTATION
- Y02T10/00—Road transport of goods or passengers
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- Y02T10/12—Improving ICE efficiencies
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- General Chemical & Material Sciences (AREA)
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Description
・第1端面「a」と第2端面「b」の間に延びる長さLを有する担体基材と、
・担体基材上に配置された異なる構成物質ゾーンA及びBを含む触媒に関し、ここで、
物質ゾーンAはパラジウムを含まない白金又はPt:Pdの重量比が≧1である白金とパラジウムを含み、かつ、
物質ゾーンBは0.355以上のCu/Al比を有する銅含有ゼオライトを含む、触媒に関する。
a)希硝酸を添加して、白金を、テトラエチルアンモニウムヘキサヒドロキソプラチネート(EP 3 210 989(B1))の水溶液から、5重量%のシリカで安定化された酸化チタン粉末上に沈殿させて、酸化チタン粉末に基づいて3重量%の濃度のPtを有する材料を得る。続いて、このようにして調製した粉末を濾別し、乾燥させて、空気雰囲気中、800℃で2時間固定する。
b)次いで、a)に従って得られた粉末を水中でスラリー化し、白金を含有しない酸化チタンを加えて、所望の0.14重量%のPt(総酸化チタン粉末に基づく)担持量に調整する。このようにして得られたウォッシュコートを使用して、400cpsiのセル密度及び110μmの壁厚を有する市販のセラミック製フロースルー基材をその全長にわたって従来の方法でコーティングする。次いで、コーティングした基材を110℃で乾燥させ、600℃で6時間焼成する。触媒のウォッシュコート担持量は25g/Lであり、触媒の白金担持量は0.0353g/Lである。
c)構造タイプCHA(SAR=13)のゼオライトに、銅含有ゼオライトの重量に基づいてCuOとして計算される7重量%の量で銅を担持させる。Cu/Al比は0.42である。このようにして得られたゼオライトをバインダー材料を含有する水中に分散させてウォッシュコートを得る。
d)c)に従って得られたウォッシュコートを、b)に従って得られたコーティングされた基材上にその全長にわたって上層としてコーティングする。ウォッシュコートの担持量は100g/Lである。次いで、コーティングされた基材を110℃で乾燥させ、600℃で6時間焼成する。
ステップc)に従って得られたゼオライトに5.5重量%の量の銅を担持させること以外は実施例1を繰り返す。Cu/Al比は0.325である。
a)触媒K1及びVK1を、10%のH2O及び10%のO2を含む雰囲気中、750℃で16時間エージングした。
b)供給ガス中にNH3、O2及びH2を含むライトダウン-ライトアップ実験においてライトアップ期を検討し、ここで、温度は5K/分で100℃から600℃まで上昇させる。触媒VK1と比較して、本発明の触媒K1は改善されたNH3転化率を示し、20%少ない平均N2O形成、30%少ない最大N2O濃度及び5%小さいNO選択性を示した。また結果を図1に示し、灰色のグラフは触媒K1に、及び黒色のグラフは触媒VK1に対応する。
c)供給ガス中にNH3、NO、O2及びH2Oを含むマッピング試験において、反応器出口におけるNH3の濃度が20ppmとなるときに得られるNOx転化率及びN2O形成を測定した。
Claims (16)
- 排気ガスからのアンモニア及び窒素酸化物の排出量を低減するための触媒であって、
第1端面「a」と第2端面「b」の間に延びる長さLを有する担体基材と、
前記担体基材上に配置された異なる構成物質ゾーンA及びBを含み、ここで、
物質ゾーンAがパラジウムを含まない白金又はPt:Pdの重量比が≧1である白金とパラジウムを含み、かつ、
物質ゾーンBが0.4~2のCu/Alモル比を有する銅含有ゼオライトを含み、
物質ゾーンAが白金粒子の形態の白金を含み、前記白金粒子が50~200nmの平均直径を有する、触媒。 - 物質ゾーンAが白金を含みパラジウムを含まないことを特徴とする、請求項1に記載の触媒。
- 前記白金粒子が80~120nmの平均直径を有することを特徴とする、請求項1又は2に記載の触媒。
- 物質ゾーンAの白金又は白金とパラジウムが1つ以上の担体酸化物上に担持されていることを特徴とする、請求項1~3のいずれか一項に記載の触媒。
- 前記担体酸化物が、酸化アルミニウム、ドープされた酸化アルミニウム、酸化ケイ素、酸化チタン、ドープされた酸化チタン、酸化セリウム、酸化ジルコニウム、及びそれらの1つ以上の混合酸化物からなる群から選択されることを特徴とする、請求項4に記載の触媒。
- 前記白金粒子が酸化チタン上に担持されていることを特徴とする、請求項1~5のいずれか一項に記載の触媒。
- 酸化チタンが酸化ケイ素でドープされていることを特徴とする、請求項6に記載の触媒。
- 酸化チタンが、前記ドープされた酸化チタンの重量に基づいて、1~10重量%の酸化ケイ素でドープされていることを特徴とする、請求項7に記載の触媒。
- 物質ゾーンBの前記ゼオライトが構造タイプABW、AEI、AFX、BEA、CHA、DDR、ERI、ESV、FAU、FER、KFI、LEV、LTA、MER MFI、MWW、SOD、又はSTTに属することを特徴とする、請求項1~8のいずれか一項に記載の触媒。
- 物質ゾーンBの前記ゼオライトが構造タイプCHAに属することを特徴とする、請求項1~9のいずれか一項に記載の触媒。
- 物質ゾーンBの前記ゼオライトが2~100のSAR(シリカ対アルミナ比)値を有することを特徴とする、請求項1~10のいずれか一項に記載の触媒。
- 物質ゾーンBの前記銅含有ゼオライトが0.4~0.45のCu/Alモル比を有することを特徴とする、請求項1~11のいずれか一項に記載の触媒。
- 物質ゾーンA及びBの両方が前記担体基材の長さLの100%にわたって延びることを特徴とする、請求項1~12のいずれか一項に記載の触媒。
- 物質ゾーンAが前記担体基材上にコーティングされて下層を形成し、物質ゾーンBが物質ゾーンA上にコーティングされて上層を形成することを特徴とする、請求項13に記載の触媒。
- 物質ゾーンAが前記担体基材の長さLの20~60%にコーティングされ、物質ゾーンBが前記担体基材の長さLの100%にわたってコーティングされることを特徴とする、請求項1~12のいずれか一項に記載の触媒。
- 順に、アンモニア又はアンモニア前駆体を供給するための第1装置と、第1のSCR触媒と、その端面「a」が前記第1のSCR触媒の方向を向くように配置された請求項1~15のいずれか一項に記載の触媒と、を含む、触媒装置。
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EP19192426.5A EP3782726A1 (en) | 2019-08-20 | 2019-08-20 | Catalyst for the abatement of ammonia and nitrogen oxide emissions from the exhaust gases of combustion engines |
EP19192426.5 | 2019-08-20 | ||
PCT/EP2019/073966 WO2021032308A1 (en) | 2019-08-20 | 2019-09-09 | Catalyst for the abatement of ammonia and nitrogen oxide emissions from the exhaust gases of combustion engines |
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KR20220050170A (ko) | 2022-04-22 |
CN114269471A (zh) | 2022-04-01 |
EP3782726A1 (en) | 2021-02-24 |
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