JP6581032B2 - ハニカム構造体 - Google Patents
ハニカム構造体 Download PDFInfo
- Publication number
- JP6581032B2 JP6581032B2 JP2016072586A JP2016072586A JP6581032B2 JP 6581032 B2 JP6581032 B2 JP 6581032B2 JP 2016072586 A JP2016072586 A JP 2016072586A JP 2016072586 A JP2016072586 A JP 2016072586A JP 6581032 B2 JP6581032 B2 JP 6581032B2
- Authority
- JP
- Japan
- Prior art keywords
- zeolite
- honeycomb structure
- volume
- inorganic binder
- coarse
- 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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- HNPSIPDUKPIQMN-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical compound O=[Si]=O.O=[Al]O[Al]=O HNPSIPDUKPIQMN-UHFFFAOYSA-N 0.000 claims description 398
- 239000010457 zeolite Substances 0.000 claims description 318
- 229910021536 Zeolite Inorganic materials 0.000 claims description 237
- 239000011148 porous material Substances 0.000 claims description 173
- 239000011230 binding agent Substances 0.000 claims description 119
- 239000002245 particle Substances 0.000 claims description 112
- 238000000034 method Methods 0.000 claims description 46
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims description 44
- VXYADVIJALMOEQ-UHFFFAOYSA-K tris(lactato)aluminium Chemical compound CC(O)C(=O)O[Al](OC(=O)C(C)O)OC(=O)C(C)O VXYADVIJALMOEQ-UHFFFAOYSA-K 0.000 claims description 43
- 239000000463 material Substances 0.000 claims description 39
- 238000005342 ion exchange Methods 0.000 claims description 25
- JPVYNHNXODAKFH-UHFFFAOYSA-N Cu2+ Chemical compound [Cu+2] JPVYNHNXODAKFH-UHFFFAOYSA-N 0.000 claims description 21
- 229910001431 copper ion Inorganic materials 0.000 claims description 21
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims description 18
- 239000011164 primary particle Substances 0.000 claims description 17
- 229910001593 boehmite Inorganic materials 0.000 claims description 15
- FAHBNUUHRFUEAI-UHFFFAOYSA-M hydroxidooxidoaluminium Chemical compound O[Al]=O FAHBNUUHRFUEAI-UHFFFAOYSA-M 0.000 claims description 15
- 239000012784 inorganic fiber Substances 0.000 claims description 15
- 238000004519 manufacturing process Methods 0.000 claims description 13
- 239000000835 fiber Substances 0.000 claims description 12
- 239000000377 silicon dioxide Substances 0.000 claims description 9
- 239000003365 glass fiber Substances 0.000 claims description 3
- MWUXSHHQAYIFBG-UHFFFAOYSA-N Nitric oxide Chemical compound O=[N] MWUXSHHQAYIFBG-UHFFFAOYSA-N 0.000 description 57
- 239000002994 raw material Substances 0.000 description 54
- 238000000746 purification Methods 0.000 description 26
- 238000001878 scanning electron micrograph Methods 0.000 description 23
- 238000009826 distribution Methods 0.000 description 14
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 14
- 239000007789 gas Substances 0.000 description 13
- 238000005192 partition Methods 0.000 description 13
- 238000005259 measurement Methods 0.000 description 11
- QSHDDOUJBYECFT-UHFFFAOYSA-N mercury Chemical compound [Hg] QSHDDOUJBYECFT-UHFFFAOYSA-N 0.000 description 10
- 229910052753 mercury Inorganic materials 0.000 description 10
- 230000000052 comparative effect Effects 0.000 description 9
- 239000003054 catalyst Substances 0.000 description 8
- 238000010304 firing Methods 0.000 description 8
- 230000002093 peripheral effect Effects 0.000 description 8
- 229910019142 PO4 Inorganic materials 0.000 description 7
- 239000013078 crystal Substances 0.000 description 7
- 230000007423 decrease Effects 0.000 description 7
- 238000001035 drying Methods 0.000 description 7
- 230000000694 effects Effects 0.000 description 7
- 239000000203 mixture Substances 0.000 description 7
- NBIIXXVUZAFLBC-UHFFFAOYSA-K phosphate Chemical compound [O-]P([O-])([O-])=O NBIIXXVUZAFLBC-UHFFFAOYSA-K 0.000 description 7
- 239000010452 phosphate Substances 0.000 description 7
- 238000002156 mixing Methods 0.000 description 6
- 238000001179 sorption measurement Methods 0.000 description 6
- 230000000007 visual effect Effects 0.000 description 6
- 238000004458 analytical method Methods 0.000 description 5
- UNYSKUBLZGJSLV-UHFFFAOYSA-L calcium;1,3,5,2,4,6$l^{2}-trioxadisilaluminane 2,4-dioxide;dihydroxide;hexahydrate Chemical group O.O.O.O.O.O.[OH-].[OH-].[Ca+2].O=[Si]1O[Al]O[Si](=O)O1.O=[Si]1O[Al]O[Si](=O)O1 UNYSKUBLZGJSLV-UHFFFAOYSA-L 0.000 description 5
- 238000010438 heat treatment Methods 0.000 description 5
- 229930195733 hydrocarbon Natural products 0.000 description 5
- 150000002430 hydrocarbons Chemical class 0.000 description 5
- 150000002500 ions Chemical class 0.000 description 5
- 239000000126 substance Substances 0.000 description 5
- 238000012360 testing method Methods 0.000 description 5
- 239000004215 Carbon black (E152) Substances 0.000 description 4
- 238000001354 calcination Methods 0.000 description 4
- 229910052676 chabazite Inorganic materials 0.000 description 4
- 238000010586 diagram Methods 0.000 description 4
- 238000001887 electron backscatter diffraction Methods 0.000 description 4
- 238000001125 extrusion Methods 0.000 description 4
- 239000000243 solution Substances 0.000 description 4
- 238000012935 Averaging Methods 0.000 description 3
- 230000005540 biological transmission Effects 0.000 description 3
- 238000004364 calculation method Methods 0.000 description 3
- 229910052878 cordierite Inorganic materials 0.000 description 3
- 238000003795 desorption Methods 0.000 description 3
- 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 3
- 239000002270 dispersing agent Substances 0.000 description 3
- 238000002003 electron diffraction Methods 0.000 description 3
- 238000009472 formulation Methods 0.000 description 3
- 230000006872 improvement Effects 0.000 description 3
- 238000004898 kneading Methods 0.000 description 3
- 229920000609 methyl cellulose Polymers 0.000 description 3
- 239000001923 methylcellulose Substances 0.000 description 3
- 235000010981 methylcellulose Nutrition 0.000 description 3
- 239000000843 powder Substances 0.000 description 3
- URLKBWYHVLBVBO-UHFFFAOYSA-N Para-Xylene Chemical group CC1=CC=C(C)C=C1 URLKBWYHVLBVBO-UHFFFAOYSA-N 0.000 description 2
- 239000003463 adsorbent Substances 0.000 description 2
- -1 aluminum ion Chemical class 0.000 description 2
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 2
- 229910001423 beryllium ion Inorganic materials 0.000 description 2
- 238000002485 combustion reaction Methods 0.000 description 2
- 238000010276 construction Methods 0.000 description 2
- 230000001186 cumulative effect Effects 0.000 description 2
- 239000012530 fluid Substances 0.000 description 2
- 239000012528 membrane Substances 0.000 description 2
- 229910021645 metal ion Inorganic materials 0.000 description 2
- 239000001301 oxygen Substances 0.000 description 2
- 229910052760 oxygen Inorganic materials 0.000 description 2
- 230000000704 physical effect Effects 0.000 description 2
- 238000000790 scattering method Methods 0.000 description 2
- 238000000926 separation method Methods 0.000 description 2
- JNYAEWCLZODPBN-JGWLITMVSA-N (2r,3r,4s)-2-[(1r)-1,2-dihydroxyethyl]oxolane-3,4-diol Chemical compound OC[C@@H](O)[C@H]1OC[C@H](O)[C@H]1O JNYAEWCLZODPBN-JGWLITMVSA-N 0.000 description 1
- LNAZSHAWQACDHT-XIYTZBAFSA-N (2r,3r,4s,5r,6s)-4,5-dimethoxy-2-(methoxymethyl)-3-[(2s,3r,4s,5r,6r)-3,4,5-trimethoxy-6-(methoxymethyl)oxan-2-yl]oxy-6-[(2r,3r,4s,5r,6r)-4,5,6-trimethoxy-2-(methoxymethyl)oxan-3-yl]oxyoxane Chemical compound CO[C@@H]1[C@@H](OC)[C@H](OC)[C@@H](COC)O[C@H]1O[C@H]1[C@H](OC)[C@@H](OC)[C@H](O[C@H]2[C@@H]([C@@H](OC)[C@H](OC)O[C@@H]2COC)OC)O[C@@H]1COC LNAZSHAWQACDHT-XIYTZBAFSA-N 0.000 description 1
- SMZOUWXMTYCWNB-UHFFFAOYSA-N 2-(2-methoxy-5-methylphenyl)ethanamine Chemical compound COC1=CC=C(C)C=C1CCN SMZOUWXMTYCWNB-UHFFFAOYSA-N 0.000 description 1
- NIXOWILDQLNWCW-UHFFFAOYSA-N 2-Propenoic acid Natural products OC(=O)C=C NIXOWILDQLNWCW-UHFFFAOYSA-N 0.000 description 1
- 241000269350 Anura Species 0.000 description 1
- 229920002134 Carboxymethyl cellulose Polymers 0.000 description 1
- 239000001856 Ethyl cellulose Substances 0.000 description 1
- 229920000663 Hydroxyethyl cellulose Polymers 0.000 description 1
- 239000004354 Hydroxyethyl cellulose Substances 0.000 description 1
- BPQQTUXANYXVAA-UHFFFAOYSA-N Orthosilicate Chemical compound [O-][Si]([O-])([O-])[O-] BPQQTUXANYXVAA-UHFFFAOYSA-N 0.000 description 1
- 239000004372 Polyvinyl alcohol Substances 0.000 description 1
- 238000005411 Van der Waals force Methods 0.000 description 1
- 239000002253 acid Substances 0.000 description 1
- 238000004220 aggregation Methods 0.000 description 1
- 230000002776 aggregation Effects 0.000 description 1
- 229910052782 aluminium Inorganic materials 0.000 description 1
- 239000007864 aqueous solution Substances 0.000 description 1
- 230000002902 bimodal effect Effects 0.000 description 1
- 239000001768 carboxy methyl cellulose Substances 0.000 description 1
- 235000010948 carboxy methyl cellulose Nutrition 0.000 description 1
- 239000008112 carboxymethyl-cellulose Substances 0.000 description 1
- 239000000969 carrier Substances 0.000 description 1
- 230000003197 catalytic effect Effects 0.000 description 1
- 238000013329 compounding Methods 0.000 description 1
- 150000001875 compounds Chemical class 0.000 description 1
- 229910000365 copper sulfate Inorganic materials 0.000 description 1
- XTVVROIMIGLXTD-UHFFFAOYSA-N copper(II) nitrate Chemical compound [Cu+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O XTVVROIMIGLXTD-UHFFFAOYSA-N 0.000 description 1
- ARUVKPQLZAKDPS-UHFFFAOYSA-L copper(II) sulfate Chemical compound [Cu+2].[O-][S+2]([O-])([O-])[O-] ARUVKPQLZAKDPS-UHFFFAOYSA-L 0.000 description 1
- OPQARKPSCNTWTJ-UHFFFAOYSA-L copper(ii) acetate Chemical compound [Cu+2].CC([O-])=O.CC([O-])=O OPQARKPSCNTWTJ-UHFFFAOYSA-L 0.000 description 1
- 230000003247 decreasing effect Effects 0.000 description 1
- 238000005238 degreasing Methods 0.000 description 1
- 230000006866 deterioration Effects 0.000 description 1
- 238000011161 development Methods 0.000 description 1
- GUJOJGAPFQRJSV-UHFFFAOYSA-N dialuminum;dioxosilane;oxygen(2-);hydrate Chemical compound O.[O-2].[O-2].[O-2].[Al+3].[Al+3].O=[Si]=O.O=[Si]=O.O=[Si]=O.O=[Si]=O GUJOJGAPFQRJSV-UHFFFAOYSA-N 0.000 description 1
- 238000007604 dielectric heating drying Methods 0.000 description 1
- 235000014113 dietary fatty acids Nutrition 0.000 description 1
- 239000006185 dispersion Substances 0.000 description 1
- 229920001249 ethyl cellulose Polymers 0.000 description 1
- 235000019325 ethyl cellulose Nutrition 0.000 description 1
- 238000002474 experimental method Methods 0.000 description 1
- 239000000194 fatty acid Substances 0.000 description 1
- 229930195729 fatty acid Natural products 0.000 description 1
- 150000004665 fatty acids Chemical class 0.000 description 1
- 238000007602 hot air drying Methods 0.000 description 1
- 235000019447 hydroxyethyl cellulose Nutrition 0.000 description 1
- 239000001866 hydroxypropyl methyl cellulose Substances 0.000 description 1
- 229920003088 hydroxypropyl methyl cellulose Polymers 0.000 description 1
- 235000010979 hydroxypropyl methyl cellulose Nutrition 0.000 description 1
- UFVKGYZPFZQRLF-UHFFFAOYSA-N hydroxypropyl methyl cellulose Chemical compound OC1C(O)C(OC)OC(CO)C1OC1C(O)C(O)C(OC2C(C(O)C(OC3C(C(O)C(O)C(CO)O3)O)C(CO)O2)O)C(CO)O1 UFVKGYZPFZQRLF-UHFFFAOYSA-N 0.000 description 1
- 238000007654 immersion Methods 0.000 description 1
- 238000009616 inductively coupled plasma Methods 0.000 description 1
- 229910052751 metal Inorganic materials 0.000 description 1
- 239000002184 metal Substances 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 229910052901 montmorillonite Inorganic materials 0.000 description 1
- 238000000465 moulding Methods 0.000 description 1
- 230000001590 oxidative effect Effects 0.000 description 1
- 238000005498 polishing Methods 0.000 description 1
- 229920002451 polyvinyl alcohol Polymers 0.000 description 1
- 235000019422 polyvinyl alcohol Nutrition 0.000 description 1
- 238000002360 preparation method Methods 0.000 description 1
- 230000008569 process Effects 0.000 description 1
- 230000009467 reduction Effects 0.000 description 1
- 229920006395 saturated elastomer Polymers 0.000 description 1
- 239000011163 secondary particle Substances 0.000 description 1
- RMAQACBXLXPBSY-UHFFFAOYSA-N silicic acid Chemical compound O[Si](O)(O)O RMAQACBXLXPBSY-UHFFFAOYSA-N 0.000 description 1
- 239000011973 solid acid Substances 0.000 description 1
- 150000005846 sugar alcohols Polymers 0.000 description 1
- 239000011800 void material Substances 0.000 description 1
- 150000003738 xylenes Chemical class 0.000 description 1
Classifications
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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
- B01J29/00—Catalysts comprising molecular sieves
- B01J29/82—Phosphates
- B01J29/84—Aluminophosphates containing other elements, e.g. metals, boron
- B01J29/85—Silicoaluminophosphates [SAPO compounds]
-
- 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
- B01D53/02—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 by adsorption, e.g. preparative gas chromatography
- B01D53/04—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 by adsorption, e.g. preparative gas chromatography with stationary adsorbents
- B01D53/0407—Constructional details of adsorbing systems
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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
- B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
- B01D53/86—Catalytic processes
- B01D53/8621—Removing nitrogen compounds
- B01D53/8625—Nitrogen oxides
- B01D53/8628—Processes characterised by a specific catalyst
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- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
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- 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
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- 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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- 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
- B01J21/00—Catalysts comprising the elements, oxides, or hydroxides of magnesium, boron, aluminium, carbon, silicon, titanium, zirconium, or hafnium
- B01J21/12—Silica and alumina
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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
- B01J29/00—Catalysts comprising molecular sieves
- B01J29/04—Catalysts comprising molecular sieves having base-exchange properties, e.g. crystalline zeolites
- B01J29/06—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof
- B01J29/08—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of the faujasite type, e.g. type X or Y
- B01J29/084—Y-type faujasite
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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
- B01J29/00—Catalysts comprising molecular sieves
- B01J29/04—Catalysts comprising molecular sieves having base-exchange properties, e.g. crystalline zeolites
- B01J29/06—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof
- B01J29/08—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of the faujasite type, e.g. type X or Y
- B01J29/10—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of the faujasite type, e.g. type X or Y containing iron group metals, noble metals or copper
- B01J29/14—Iron group metals or copper
- B01J29/146—Y-type faujasite
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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
- B01J29/00—Catalysts comprising molecular sieves
- B01J29/04—Catalysts comprising molecular sieves having base-exchange properties, e.g. crystalline zeolites
- B01J29/06—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof
- B01J29/40—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of the pentasil type, e.g. types ZSM-5, ZSM-8 or ZSM-11, as exemplified by patent documents US3702886, GB1334243 and US3709979, respectively
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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
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- B01J29/04—Catalysts comprising molecular sieves having base-exchange properties, e.g. crystalline zeolites
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- B01J29/40—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of the pentasil type, e.g. types ZSM-5, ZSM-8 or ZSM-11, as exemplified by patent documents US3702886, GB1334243 and US3709979, respectively
- B01J29/42—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of the pentasil type, e.g. types ZSM-5, ZSM-8 or ZSM-11, as exemplified by patent documents US3702886, GB1334243 and US3709979, respectively containing iron group metals, noble metals or copper
- B01J29/46—Iron group metals or copper
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
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- B01J29/04—Catalysts comprising molecular sieves having base-exchange properties, e.g. crystalline zeolites
- B01J29/06—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof
- B01J29/70—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of types characterised by their specific structure not provided for in groups B01J29/08 - B01J29/65
- B01J29/7007—Zeolite Beta
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
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- B01J29/00—Catalysts comprising molecular sieves
- B01J29/04—Catalysts comprising molecular sieves having base-exchange properties, e.g. crystalline zeolites
- B01J29/06—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof
- B01J29/70—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of types characterised by their specific structure not provided for in groups B01J29/08 - B01J29/65
- B01J29/7015—CHA-type, e.g. Chabazite, LZ-218
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
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- B01J29/00—Catalysts comprising molecular sieves
- B01J29/04—Catalysts comprising molecular sieves having base-exchange properties, e.g. crystalline zeolites
- B01J29/06—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof
- B01J29/70—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of types characterised by their specific structure not provided for in groups B01J29/08 - B01J29/65
- B01J29/72—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of types characterised by their specific structure not provided for in groups B01J29/08 - B01J29/65 containing iron group metals, noble metals or copper
- B01J29/76—Iron group metals or copper
- B01J29/7615—Zeolite Beta
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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
- B01J29/00—Catalysts comprising molecular sieves
- B01J29/04—Catalysts comprising molecular sieves having base-exchange properties, e.g. crystalline zeolites
- B01J29/06—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof
- B01J29/70—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of types characterised by their specific structure not provided for in groups B01J29/08 - B01J29/65
- B01J29/72—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of types characterised by their specific structure not provided for in groups B01J29/08 - B01J29/65 containing iron group metals, noble metals or copper
- B01J29/76—Iron group metals or copper
- B01J29/763—CHA-type, e.g. Chabazite, LZ-218
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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
- B01J29/00—Catalysts comprising molecular sieves
- B01J29/04—Catalysts comprising molecular sieves having base-exchange properties, e.g. crystalline zeolites
- B01J29/06—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof
- B01J29/80—Mixtures of different zeolites
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- B—PERFORMING OPERATIONS; TRANSPORTING
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Description
[9] 前記[1]〜[8]のいずれかに記載のハニカム構造体の製造方法であって、前記ゼオライト材料が、前記ゼオライト材料の総体積中に、前記無機結合材を3体積%以上含み、前記無機結合材が、塩基性乳酸アルミニウム由来のアルミナを、前記ゼオライト材料の総体積に対して1体積%以上含む、ハニカム構造体の製造方法。
[10] 前記無機結合材が、塩基性乳酸アルミニウム由来のアルミナと、ベーマイト由来のアルミナと、を含み、前記ベーマイト由来のアルミナの体積A2に対する、前記塩基性乳酸アルミニウム由来のアルミナの体積A1の比率であるA1/A2の値が、0.6以上である、前記[9]に記載のハニカム構造体の製造方法。
図1〜図3に示すように、本発明のハニカム構造体の一の実施形態は、粗粒ゼオライト、微粒ゼオライト、及び無機結合材を少なくとも含有するゼオライト材料から構成されたハニカム構造部4を含む、ハニカム構造体100である。ハニカム構造部4は、第一の端面11から第二の端面12まで延びる流体の流路となる複数のセル2を区画形成する隔壁1を有するものである。本実施形態のハニカム構造体100は、例えば、上述したゼオライト粒子と無機結合材とを少なくとも含有するゼオライト原料を押出成形して形成されたハニカム構造体100であることが好ましい。
式(1):無機結合材の体積の比率={(無機結合材の体積)/(ゼオライト粒子全体の体積+無機結合材の体積+その他の成分の体積)}
式(2):気孔率=細孔容量/(細孔容量+1/ハニカム構造部の真密度)×100
次に、本発明のハニカム構造体の製造方法について説明する。
粗粒ゼオライトとして、銅イオンで4.1質量%イオン交換された、平均粒子径が3.9μmのSAPO−34を用意した。また、微粒ゼオライトとして、銅イオンで6.3質量%イオン交換された、平均粒子径が0.4μmのβ型ゼオライトを用意した。表1に、実施例1に使用した粗粒ゼオライト及び微粒ゼオライトの種類及び平均粒子径を示す。表1の「ゼオライトの欄」の、「Cu−SAPO−34」は、銅イオンでイオン交換されたSAPO−34であることを意味する。また、表1の「ゼオライトの欄」の、「Cu−β」は、銅イオンでイオン交換されたβ型ゼオライトであることを意味する。各ゼオライトの平均粒子径は、それぞれのゼオライトの粒子を含有する粉末の粒子径分布におけるメジアン径(d50)であり、JIS R1629に準拠したレーザー回折散乱法にて測定した。
(2)ゼオライト材料全体の体積に対する、塩基性乳酸アルミニウム由来のアルミナの体積の比率(体積%)。
(3)ゼオライト材料全体の体積に対する、無機結合材の体積の比率(体積%)。
(4)ベーマイト由来のアルミナの体積A2に対する、塩基性乳酸アルミニウム由来のアルミナの体積A1の比率(A1/A2)。
(5)細孔径が0.02〜0.15μmの細孔容積比率(%)。
(6)細孔径0.02μm以下の細孔容積比率(%)。
(7)細孔径0.15μm以上の細孔容積比率(%)。
(8)細孔径0.52μm以上の細孔容積比率(%)。
(9)気孔率(%)。
(10)圧縮強度(MPa)。
式(3):気孔率=細孔容量/(細孔容量+1/ハニカム構造部の真密度)×100
表2に示すように、ゼオライト原料の配合処方を変更した以外は、実施例1と同様の方法で、ハニカム構造体を製造した。なお、実施例2〜8において、乳酸アルミニウムについては、乳酸アルミニウムの質量の2倍の質量の水に溶解して用いた。
粗粒ゼオライトとして、銅イオンで5.0質量%イオン交換された、平均粒子径が4.4μmのチャバサイトを用いた以外は実施例3と同様の配合と方法で、ハニカム構造体を製造した。
微粒ゼオライトとして銅イオンで5.0質量%イオン交換された、平均粒子径が0.6μmのチャバサイトを用いた以外は実施例9と同様の配合と方法で、ハニカム構造体を製造した。
表3に示すように、ゼオライト原料の配合処方を変更した以外は、実施例1と同様の方法で、ハニカム構造体を製造した。なお、比較例1、3及び5〜7においては、無機結合材として、アルミナゾルを用いた。アルミナゾルは、日産化学社製のアルミナゾル「AS520(商品名)」を用いた。
表4に示すように、実施例1〜10のハニカム構造体は、細孔径が0.02〜0.15μmの細孔容積比率が、42体積%以下であり、圧縮強度(MPa)が高いものであった。また、実施例1〜10のハニカム構造体は、ゼオライト材料中に粗粒ゼオライトとしてのチャバサイト型ゼオライトを含むものであるため、NOx浄化性能に優れたものであった。実施例1〜10のハニカム構造体は、無機結合材の凝集性が向上し、圧縮強度が向上したものと考えられる。また、図8に示すSEM画像においては、ゼオライト材料中のゼオライト粒子の輪郭が比較的に明瞭に確認することができた。即ち、このようなゼオライト材料は、ゼオライト材料中の無機結合材の凝集性が高く、無機結合材によって比較的緻密なネック部が形成され、その圧縮強度が高いものになっていると考えられる。
Claims (10)
- 平均粒子径が大きな粗粒ゼオライト、前記粗粒ゼオライトよりも平均粒子径が小さな微粒ゼオライト及び、無機結合材を少なくとも含有するゼオライト材料から構成されたハニカム構造部を含み、
前記粗粒ゼオライトは、一次粒子の平均粒子径が2μm以上、6μm以下のチャバサイト型ゼオライトであり、
前記微粒ゼオライトは、一次粒子の平均粒子径が0.02μm以上、2μm未満のものであり、
前記ハニカム構造部を構成する前記ゼオライト材料は、細孔径が0.02〜0.15μmの細孔の容積が、全細孔の容積に対して42%以下である、ハニカム構造体。 - 前記ゼオライト材料は、細孔径が0.02μm未満の細孔の容積が、全細孔の容積に対して8〜20%のものである、請求項1に記載のハニカム構造体。
- 前記ゼオライト材料は、細孔径が0.15μmを超える細孔の容積が、全細孔の容積の40〜60%で、且つ、細孔径が0.52μm以上の細孔の容積が、全細孔の容積の5%以下のものである、請求項1又は2に記載のハニカム構造体。
- 前記粗粒ゼオライト及び前記微粒ゼオライトが、イオン交換部位に銅イオンを含むものである、請求項1〜3のいずれか一項に記載のハニカム構造体。
- 前記粗粒ゼオライトが、チャバサイト、SAPO−34、及びSSZ−13のうち少なくとも一種のゼオライトである、請求項1〜4のいずれか一項に記載のハニカム構造体。
- 前記微粒ゼオライトが、β型ゼオライト、Y型ゼオライト、ZSM−5型ゼオライト、及びチャバサイト型ゼオライトのうち少なくとも一種のゼオライトである、請求項1〜5のいずれか一項に記載のハニカム構造体。
- 前記ゼオライト材料が、アルミナ繊維、シリカアルミナ繊維、及びガラス繊維のうちの少なくとも一種の無機繊維を含む、請求項1〜6のいずれか一項に記載のハニカム構造体。
- 前記ゼオライト材料が、前記ゼオライト材料の総体積中に、前記無機繊維を3〜8体積%含む、請求項7に記載のハニカム構造体。
- 請求項1〜8のいずれか一項に記載のハニカム構造体の製造方法であって、
前記ゼオライト材料が、前記ゼオライト材料の総体積中に、前記無機結合材を3体積%以上含み、
前記無機結合材が、塩基性乳酸アルミニウム由来のアルミナを、前記ゼオライト材料の総体積に対して1体積%以上含む、ハニカム構造体の製造方法。 - 前記無機結合材が、塩基性乳酸アルミニウム由来のアルミナと、ベーマイト由来のアルミナと、を含み、
前記ベーマイト由来のアルミナの体積A2に対する、前記塩基性乳酸アルミニウム由来のアルミナの体積A1の比率であるA1/A2の値が、0.6以上である、請求項9に記載のハニカム構造体の製造方法。
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