CN101585000B - 蜂窝结构体 - Google Patents
蜂窝结构体 Download PDFInfo
- Publication number
- CN101585000B CN101585000B CN200910136939XA CN200910136939A CN101585000B CN 101585000 B CN101585000 B CN 101585000B CN 200910136939X A CN200910136939X A CN 200910136939XA CN 200910136939 A CN200910136939 A CN 200910136939A CN 101585000 B CN101585000 B CN 101585000B
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- CN
- China
- Prior art keywords
- structured body
- honeycomb structured
- cellular unit
- zeolite
- body according
- 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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- 239000010457 zeolite Substances 0.000 claims abstract description 93
- 229910021536 Zeolite Inorganic materials 0.000 claims abstract description 89
- HNPSIPDUKPIQMN-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical compound O=[Si]=O.O=[Al]O[Al]=O HNPSIPDUKPIQMN-UHFFFAOYSA-N 0.000 claims abstract description 89
- 239000011148 porous material Substances 0.000 claims abstract description 47
- 239000011230 binding agent Substances 0.000 claims abstract description 39
- 230000001413 cellular effect Effects 0.000 claims description 159
- 239000000463 material Substances 0.000 claims description 65
- PNEYBMLMFCGWSK-UHFFFAOYSA-N Alumina Chemical compound [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims description 35
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims description 27
- 239000000835 fiber Substances 0.000 claims description 26
- 239000002245 particle Substances 0.000 claims description 22
- 238000000034 method Methods 0.000 claims description 17
- MCMNRKCIXSYSNV-UHFFFAOYSA-N Zirconium dioxide Chemical compound O=[Zr]=O MCMNRKCIXSYSNV-UHFFFAOYSA-N 0.000 claims description 14
- 239000000377 silicon dioxide Substances 0.000 claims description 11
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 claims description 10
- 238000005342 ion exchange Methods 0.000 claims description 9
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 claims description 6
- 229960000892 attapulgite Drugs 0.000 claims description 6
- 229910052625 palygorskite Inorganic materials 0.000 claims description 6
- 229910052624 sepiolite Inorganic materials 0.000 claims description 6
- 235000019355 sepiolite Nutrition 0.000 claims description 6
- 239000000499 gel Substances 0.000 claims description 5
- 239000004113 Sepiolite Substances 0.000 claims description 4
- OJMOMXZKOWKUTA-UHFFFAOYSA-N aluminum;borate Chemical compound [Al+3].[O-]B([O-])[O-] OJMOMXZKOWKUTA-UHFFFAOYSA-N 0.000 claims description 4
- KZHJGOXRZJKJNY-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical compound O=[Si]=O.O=[Si]=O.O=[Al]O[Al]=O.O=[Al]O[Al]=O.O=[Al]O[Al]=O KZHJGOXRZJKJNY-UHFFFAOYSA-N 0.000 claims description 4
- 239000012013 faujasite Substances 0.000 claims description 4
- 229910001657 ferrierite group Inorganic materials 0.000 claims description 4
- 239000003365 glass fiber Substances 0.000 claims description 4
- 239000008187 granular material Substances 0.000 claims description 4
- 229910052863 mullite Inorganic materials 0.000 claims description 4
- 235000019353 potassium silicate Nutrition 0.000 claims description 4
- 229910052802 copper Inorganic materials 0.000 claims description 3
- OQRWAMBQGTYSRD-UHFFFAOYSA-N dipotassium;oxygen(2-);titanium(4+) Chemical compound [O-2].[O-2].[O-2].[O-2].[O-2].[O-2].[O-2].[O-2].[O-2].[K+].[K+].[Ti+4].[Ti+4].[Ti+4].[Ti+4] OQRWAMBQGTYSRD-UHFFFAOYSA-N 0.000 claims description 3
- 229910052742 iron Inorganic materials 0.000 claims description 3
- 239000006193 liquid solution Substances 0.000 claims description 3
- 229910052748 manganese Inorganic materials 0.000 claims description 3
- 229910052759 nickel Inorganic materials 0.000 claims description 3
- 239000000741 silica gel Substances 0.000 claims description 3
- 229910002027 silica gel Inorganic materials 0.000 claims description 3
- HBMJWWWQQXIZIP-UHFFFAOYSA-N silicon carbide Chemical compound [Si+]#[C-] HBMJWWWQQXIZIP-UHFFFAOYSA-N 0.000 claims description 3
- 229910010271 silicon carbide Inorganic materials 0.000 claims description 3
- 235000012239 silicon dioxide Nutrition 0.000 claims description 3
- 229910052709 silver Inorganic materials 0.000 claims description 3
- NTHWMYGWWRZVTN-UHFFFAOYSA-N sodium silicate Chemical compound [Na+].[Na+].[O-][Si]([O-])=O NTHWMYGWWRZVTN-UHFFFAOYSA-N 0.000 claims description 3
- 239000010936 titanium Substances 0.000 claims description 3
- 229910052719 titanium Inorganic materials 0.000 claims description 3
- 239000004408 titanium dioxide Substances 0.000 claims description 3
- 229910052725 zinc Inorganic materials 0.000 claims description 3
- 229910000420 cerium oxide Inorganic materials 0.000 claims description 2
- -1 modenite Substances 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
- 238000012545 processing Methods 0.000 claims description 2
- 210000002421 cell wall Anatomy 0.000 abstract 2
- 210000004027 cell Anatomy 0.000 abstract 1
- 239000003054 catalyst Substances 0.000 description 20
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- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 description 6
- LYCAIKOWRPUZTN-UHFFFAOYSA-N Ethylene glycol Chemical compound OCCO LYCAIKOWRPUZTN-UHFFFAOYSA-N 0.000 description 6
- YXFVVABEGXRONW-UHFFFAOYSA-N Toluene Chemical compound CC1=CC=CC=C1 YXFVVABEGXRONW-UHFFFAOYSA-N 0.000 description 6
- 229920000609 methyl cellulose Polymers 0.000 description 6
- 239000001923 methylcellulose Substances 0.000 description 6
- 229920002134 Carboxymethyl cellulose Polymers 0.000 description 5
- 239000001768 carboxy methyl cellulose Substances 0.000 description 5
- 235000010948 carboxy methyl cellulose Nutrition 0.000 description 5
- 239000008112 carboxymethyl-cellulose Substances 0.000 description 5
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- 125000002887 hydroxy group Chemical group [H]O* 0.000 description 5
- 238000000465 moulding Methods 0.000 description 5
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- CETPSERCERDGAM-UHFFFAOYSA-N ceric oxide Chemical compound O=[Ce]=O CETPSERCERDGAM-UHFFFAOYSA-N 0.000 description 4
- 229910000422 cerium(IV) oxide Inorganic materials 0.000 description 4
- 238000006243 chemical reaction Methods 0.000 description 4
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- FAHBNUUHRFUEAI-UHFFFAOYSA-M hydroxidooxidoaluminium Chemical compound O[Al]=O FAHBNUUHRFUEAI-UHFFFAOYSA-M 0.000 description 3
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- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 3
- 239000005995 Aluminium silicate Substances 0.000 description 2
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- 229920001353 Dextrin Polymers 0.000 description 2
- 239000001856 Ethyl cellulose Substances 0.000 description 2
- ZZSNKZQZMQGXPY-UHFFFAOYSA-N Ethyl cellulose Chemical compound CCOCC1OC(OC)C(OCC)C(OCC)C1OC1C(O)C(O)C(OC)C(CO)O1 ZZSNKZQZMQGXPY-UHFFFAOYSA-N 0.000 description 2
- 229920000663 Hydroxyethyl cellulose Polymers 0.000 description 2
- KDLHZDBZIXYQEI-UHFFFAOYSA-N Palladium Chemical compound [Pd] KDLHZDBZIXYQEI-UHFFFAOYSA-N 0.000 description 2
- 239000004793 Polystyrene Substances 0.000 description 2
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- 150000001341 alkaline earth metal compounds Chemical class 0.000 description 2
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- 235000019425 dextrin Nutrition 0.000 description 2
- 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 2
- 235000014113 dietary fatty acids Nutrition 0.000 description 2
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- 150000004665 fatty acids Chemical class 0.000 description 2
- 229910010272 inorganic material Inorganic materials 0.000 description 2
- NLYAJNPCOHFWQQ-UHFFFAOYSA-N kaolin Chemical compound O.O.O=[Al]O[Si](=O)O[Si](=O)O[Al]=O NLYAJNPCOHFWQQ-UHFFFAOYSA-N 0.000 description 2
- 229910052901 montmorillonite Inorganic materials 0.000 description 2
- 229910000510 noble metal Inorganic materials 0.000 description 2
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- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 description 2
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- 239000000344 soap Substances 0.000 description 2
- 150000005846 sugar alcohols Polymers 0.000 description 2
- SMZOUWXMTYCWNB-UHFFFAOYSA-N 2-(2-methoxy-5-methylphenyl)ethanamine Chemical compound COC1=CC=C(C)C=C1CCN SMZOUWXMTYCWNB-UHFFFAOYSA-N 0.000 description 1
- PAWQVTBBRAZDMG-UHFFFAOYSA-N 2-(3-bromo-2-fluorophenyl)acetic acid Chemical compound OC(=O)CC1=CC=CC(Br)=C1F PAWQVTBBRAZDMG-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
- 125000003903 2-propenyl group Chemical group [H]C([*])([H])C([H])=C([H])[H] 0.000 description 1
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- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 1
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- DGAQECJNVWCQMB-PUAWFVPOSA-M Ilexoside XXIX Chemical compound C[C@@H]1CC[C@@]2(CC[C@@]3(C(=CC[C@H]4[C@]3(CC[C@@H]5[C@@]4(CC[C@@H](C5(C)C)OS(=O)(=O)[O-])C)C)[C@@H]2[C@]1(C)O)C)C(=O)O[C@H]6[C@@H]([C@H]([C@@H]([C@H](O6)CO)O)O)O.[Na+] DGAQECJNVWCQMB-PUAWFVPOSA-M 0.000 description 1
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 description 1
- 239000002202 Polyethylene glycol Substances 0.000 description 1
- ZLMJMSJWJFRBEC-UHFFFAOYSA-N Potassium Chemical compound [K] ZLMJMSJWJFRBEC-UHFFFAOYSA-N 0.000 description 1
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 description 1
- 239000000853 adhesive Substances 0.000 description 1
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- 229910052784 alkaline earth metal Inorganic materials 0.000 description 1
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- 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
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- NJLLQSBAHIKGKF-UHFFFAOYSA-N dipotassium dioxido(oxo)titanium Chemical compound [K+].[K+].[O-][Ti]([O-])=O NJLLQSBAHIKGKF-UHFFFAOYSA-N 0.000 description 1
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- ZQPPMHVWECSIRJ-KTKRTIGZSA-N oleic acid group Chemical group C(CCCCCCC\C=C/CCCCCCCC)(=O)O ZQPPMHVWECSIRJ-KTKRTIGZSA-N 0.000 description 1
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- 229910052703 rhodium Inorganic materials 0.000 description 1
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- MHOVAHRLVXNVSD-UHFFFAOYSA-N rhodium atom Chemical compound [Rh] MHOVAHRLVXNVSD-UHFFFAOYSA-N 0.000 description 1
- RMAQACBXLXPBSY-UHFFFAOYSA-N silicic acid Chemical compound O[Si](O)(O)O RMAQACBXLXPBSY-UHFFFAOYSA-N 0.000 description 1
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Classifications
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Abstract
本发明提供一种小型、轻量的蜂窝结构体,其具有即使作为汽车的废气净化催化剂而安装在车辆上也能发挥功能的强度,并可以高效地发挥净化性能。所述蜂窝结构体具有包含沸石和无机粘结剂的蜂窝单元,该蜂窝单元具有沿长方向从一个端面延伸至另一个端面的多个孔格被孔格壁分隔而形成的形状,所述蜂窝结构体的特征在于:所述蜂窝单元的单位表观体积的沸石含量为230g/L以上;如果所述孔格壁的厚度为X(单位:mm)、所述孔格壁表面的由显微镜观察到的平均气孔直径为Y(单位:μm),则满足X+0.07≤Y≤X+0.27和0.15≤X≤0.35。
Description
技术领域
本发明涉及一种蜂窝结构体。
背景技术
关于汽车废气的净化,已经开发了很多技术,但是,由于交通量也在增加,所以还很难说已经采取了完善的废气应对方法。无论在日本国内还是在世界范围内,都在进一步加强对汽车废气的控制。其中,对于柴油废气中的NOX的控制要求正在变得非常严格。目前为止,是通过控制发动机的燃烧系统来谋求减少NOX的,但是,仅使用该方法并不能百分之百地减少NOX。作为应对该问题的柴油NOX净化系统,已经提出了一种将氨用作还原剂还原NOX的NOX还原系统(被称为SCR(选择性催化还原)系统)。
作为应用于该系统中的催化剂载体,众所周知的有蜂窝结构体。专利文献1(国际公开第2005/063653号小册子)中公开的蜂窝结构体是由蜂窝单元构成的,该蜂窝单元是通过将γ-氧化铝(γ-alumina)、二氧化铈(ceria)、氧化锆(zirconia)、沸石(zeolite)等与无机纤维和无机粘结剂进行混合,形成蜂窝形状后进行烧成制得的。
专利文献2(日本特许第2675321号公报)中公开了一种NOX净化方法,该方法使用蜂窝(型)催化剂通过氨来还原柴油发动机废气中的NOX,在该蜂窝(型)催化剂中,孔格(cell,也称“贯穿孔”、“孔道”或“格子”)贯穿孔的等效直径为1.5~5mm,孔格壁的厚度为0.3~0.9mm,特定细孔范围内的细孔容积占整个细孔容积的40%以上。这种蜂窝(型)催化剂被认为具有充分的强度和良好的NOX净化性能。
在如专利文献1中公开的蜂窝结构体中,当使用沸石为主原料通过成型、烧成来制作蜂窝单元时,如果特别地增加沸石的含量,就有可能不能充分地保持蜂窝单元的强度。所以,由该蜂窝单元制成的蜂窝结构体在SCR系统中存在着这样的问题,即:有时不能维持其作为汽车废气用NOX净化催化剂的功能。
在如专利文献2中公开的蜂窝催化剂中,通过将蜂窝的孔格壁的厚度设为0.3mm以上来保持其强度。但是,如果加厚孔格壁,废气就很难充分地浸入孔格壁的内部,在废气的净化反应中,反应仅在孔格壁表面进行,这样,就不能有效地利用整个孔格壁。因此,针对同样的汽车废气,如果想得到期望的净化性能,为了增加可被有效利用的催化剂空间,有必要增加蜂窝催化剂的体积,这样,就存在着如何将其应用至要求轻量化、小型化的汽车废气用NOX净化催化剂上的问题。
发明内容
本发明是鉴于上述问题而提出的,其目的在于,提供一种小型、轻量的蜂窝结构体,其具有即使作为汽车的废气净化催化剂而安装在车辆上也能发挥功能的强度,并可以高效地发挥净化性能。
用于解决本发明的课题的技术手段如下所述。
本发明是具有蜂窝单元的蜂窝结构体,该蜂窝单元包含沸石和无机粘结剂,该蜂窝单元具有沿长度方向从一个端面延伸至另一个端面的多个孔格被孔格壁分隔而形成的形状,所述蜂窝结构体的特征在于,所述蜂窝单元的单位表观体积的沸石含量为230g/L以上,如果所述孔格壁的厚度为X(单位:mm)、所述孔格壁表面的由显微镜观察到的平均气孔直径为Y(单位:μm),则满足下列公式(1)和公式(2)。
公式(1):X+0.07≤Y≤X+0.27
公式(2):0.15≤X≤0.35
较好的本发明是,其特征在于所述蜂窝单元的单位表观体积的沸石含量为270g/L以下的所述蜂窝结构体。
较好的本发明是,其特征在于所述孔格壁的孔隙率为25~40%的所述蜂窝结构体。
较好的本发明是,其特征在于所述蜂窝单元的开口率为50~60%的所述蜂窝结构体。
较好的本发明是,其特征在于所述沸石至少包含β型沸石、Y型沸石、镁碱沸石、ZSM-5型沸石、丝光沸石、八面沸石、A型沸石以及L型沸石中的任意一种的所述蜂窝结构体。
较好的本发明是,其特征在于所述沸石中的二氧化硅与氧化铝的摩尔比(硅铝之比)为30~50的所述蜂窝结构体。
较好的本发明是,其特征在于所述沸石是至少用Fe、Cu、Ni、Co、Zn、Mn、Ti、Ag以及V中的任意一种进行了离子交换的所述蜂窝结构体。
较好的本发明是,其特征在于所述蜂窝单元至少包含氧化铝颗粒、二氧化钛颗粒、二氧化硅颗粒、氧化锆颗粒、氧化铈颗粒、莫来石颗粒以及这些颗粒的前驱体中任意一种的所述蜂窝结构体。
较好的本发明是,其特征在于所述无机粘结剂至少包含氧化铝胶体溶液、二氧化硅胶体溶液、二氧化钛胶体溶液、水玻璃、海泡石胶体溶液以及绿坡缕石胶体溶液中任意一种的所述蜂窝结构体。
较好的本发明是,其特征在于所述蜂窝单元包含无机纤维的所述蜂窝结构体。
较好的本发明是,其特征在于所述无机纤维至少包含氧化铝纤维、二氧化硅纤维、碳化硅纤维、硅铝纤维、玻璃纤维、钛酸钾纤维以及硼酸铝纤维中的任意一种的所述蜂窝结构体。
较好的本发明是,其特征在于多个所述蜂窝单元是通过粘结材料结合在一起的所述蜂窝结构体。
根据本发明,其效果在于,可以提供一种小型、轻量的蜂窝结构体,其具有即使作为汽车废气的净化催化剂而安装在车辆上也能发挥功能的强度,并可以高效地发挥净化性能。
附图说明
图1(a)是本发明的蜂窝结构体的立体图,具体是由多个蜂窝单元构成的蜂窝结构体的立体图。
图1(b)是本发明的蜂窝结构体的立体图,具体是由一个蜂窝单元构成的蜂窝结构体的立体图。
图2是构成图1(a)的蜂窝结构体的蜂窝单元的立体图。
图3是实施例和比较例的蜂窝单元的孔格壁厚度与气孔直径之间的关系图。
主要符号说明:
1蜂窝结构体
2蜂窝单元
3孔格
4孔格壁
5粘结材料
6被覆材料层
具体实施方式
以下参考附图说明本发明的最佳实施方式。
本发明的蜂窝结构体具有蜂窝单元,该蜂窝单元包含沸石和无机粘结剂,该蜂窝单元具有沿长度方向从一个端面延伸至另一个端面的多个孔格被孔格壁分隔而形成的形状,所述蜂窝结构体的特征在于,所述蜂窝单元的单位表观体积的沸石含量为230g/L以上,如果所述孔格壁的厚度为X(单位:mm)、所述孔格壁表面的由显微镜观察到的平均气孔直径为Y(单位:μm),则满足下列公式(1)和公式(2)。
公式(1):X+0.07≤Y≤X+0.27
公式(2):0.15≤X≤0.35
本发明的蜂窝结构体具有一个或多个蜂窝单元,该蜂窝单元是具有沿长度方向从一个端面延伸至另一个端面的多个孔格被孔格壁分隔而形成的形状的烧成体。本发明的蜂窝结构体的一个例子如图1(a)所示。图1(a)所示的蜂窝结构体1的多个蜂窝单元2通过粘结材料5来结合。每个蜂窝单元2的孔格3沿蜂窝单元的长度方向平行排列。需要注意的是,为了保持强度,蜂窝结构体1的侧面(与孔格3的贯穿孔平行的面)最好由被覆材料层6覆盖。如图2的立体图所示,构成蜂窝结构体1的蜂窝单元2具有沿长度方向延伸的多个孔格3、以及、用于分隔各孔格3的孔格壁4。
在本发明的蜂窝结构体中,蜂窝单元的单位表观体积的沸石含量较好为230~270g/L,最好为245~270g/L。如果蜂窝单元的单位表观体积的沸石含量未满230g/L,则NOX的净化性能降低。另外,如果蜂窝单元的单位表观体积的沸石含量超过270g/L,则不能保持蜂窝单元的强度,甚至不能保持蜂窝结构体的强度。
本发明的发明人就蜂窝单元的单位表观体积的沸石含量、蜂窝单元孔格壁的厚度以及蜂窝单元孔格壁表面的气孔直径对蜂窝结构体的基本单位(即蜂窝单元)的强度和催化剂性能的影响进行了研究。由研究结果可知,为了提高蜂窝单元的强度,可以降低沸石的含量,可以将孔格壁致密化,还可以加厚孔格壁。但是,为了提高净化性能,需要增加沸石的含量。另外,为了得到小型、轻量的蜂窝单元,需要使孔格壁变薄,以使不仅孔格壁表面而且整个孔格壁都能被高效地利用,还需要增大气孔直径,以使废气容易地浸入孔格壁。本发明的发明人对上述参数之间的关系进行了定量研究,发现了满足下述条件表达式的蜂窝结构体适合被用作柴油废气中的NOX净化用车载催化剂。
本发明的蜂窝结构体中的蜂窝单元的特征在于,当孔格壁的厚度为X(单位:mm),孔格壁表面的由显微镜观察到的平均气孔直径为Y(单位:μm)时,满足下列公式(1)和公式(2):
公式(1):X+0.07≤Y≤X+0.27
公式(2):0.15≤X≤0.35
上述平均气孔直径是指蜂窝单元孔格壁表面的由显微镜观察到的气孔直径的平均值。
从定性角度来看,增大蜂窝单元孔格壁表面的平均气孔直径Y,则废气容易浸入,可以提高催化剂的利用效率;减小蜂窝单元孔格壁表面的平均气孔直径Y,可以提高蜂窝结构体的强度。所以,通过对蜂窝单元的强度和NOX净化率进行定量研究可知,需要满足上述公式(1)。如果蜂窝单元孔格壁表面的平均气孔直径Y超过公式(1)中的上限,则NOX的净化率降低。这可以被认为是,如果过分增大蜂窝单元孔格壁表面的平均气孔直径Y,则从维持蜂窝单元强度的观点来看,需要减少气孔的数量,所以废气很难浸入孔格壁内部,导致NOX的净化率降低。另外,如果蜂窝单元孔格壁表面的平均气孔直径Y未达到公式(1)中的下限,则NOX的净化率也降低。这可以被认为是,如果过分地减小蜂窝单元孔格壁表面的平均气孔直径Y,则因为废气不能从气孔中充分地浸入,所以导致NOX的净化率降低。
蜂窝单元孔格壁表面的平均气孔直径Y可以采用如下方法求得,即:使用反射型电子显微镜(SEM)或光学显微镜观察孔格壁表面,通过图像处理技术取得一定范围内(例如,边长为5mm的正方形范围)的图像中的气孔,计算平均气孔直径。
这里,测量气孔直径的气孔以直径为大约0.05μm以上的、被称为所谓的“大孔”的气孔为对象。这样,就可以使用放大倍率为500~5000倍的显微镜来观察。显微镜的倍率较好为1000~3000倍,特别地,最好使用2000倍的反射型电子显微镜(SEM)进行观察,求得平均气孔直径Y。
蜂窝单元孔格壁的厚度X较好为0.15~0.35mm,最好为0.15~0.27mm。如果孔格壁的厚度X未满0.15mm,有可能不能保持蜂窝单元的强度。另外,如果孔格壁的壁厚超过0.35mm,废气有时很难浸入孔格壁内部,导致NOX的净化性能降低。所以,当作为车载蜂窝催化剂使用时,需要增加蜂窝结构体的体积,增加量相当于净化性能的降低量。
需要注意的是,如果蜂窝单元孔格壁的厚度X在0.15~0.35mm范围内比较薄,因为废气浸入的距离较短,所以可以稍微减小平均气孔直径Y。另外,如果孔格壁的壁厚X在0.15~0.35mm范围内比较厚,因为可以容易地保持蜂窝单元的强度,所以即使稍微增加平均气孔直径,也没有必要减少气孔数量。这样,就可以提高NOX的净化性能,即:可知本发明的蜂窝结构体中的蜂窝单元位于图3所示的、右侧较高的平行四边形所围成的范围内时,可以得到充分的强度和良好的NOX净化性能。
以下对本发明的蜂窝结构体进行详细说明。
(蜂窝单元)
本发明的蜂窝结构体的蜂窝单元如图2所示,是具有多个平行贯穿孔(即孔格3)的所谓的蜂窝结构。对蜂窝单元的每个孔格3的截面形状并没有特别的限定。图2所示孔格3具有正方形截面形状,但是,孔格3的截面形状可以为近似三角形、近似六边形、近似圆形、或者近似四边形与近似八边形的组合等。
蜂窝单元孔格壁的孔隙率最好为25~40%。如上所述,尽管可以稍微增加平均气孔直径,但是如果极端地减少气孔的数量,废气也很难浸入孔格壁深处。由定量研究可知,如果孔隙率未满25%,则废气很难充分浸入孔格壁的深处,NOX的净化率可能变低;另外,如果孔隙率超过40%,则孔格壁的强度可能降低。
在与蜂窝单元孔格的长度方向(与贯穿孔平行的方向)垂直的截面(多个孔格呈现开口的面)上,开口部的面积比率(即开口率)最好为50~65%。
从不增加用于净化的废气压力损失的方面来看,蜂窝单元的开口率最好为50%以上;从确保发挥净化作用的孔格壁数量的方面来看,蜂窝单元的开口率最好为65%以下。
蜂窝单元可以包含沸石和无机粘结剂,还可以包含沸石以外的无机颗粒和无机纤维。
(沸石)
在本发明的蜂窝单元的沸石中,沸石颗粒由无机粘结剂来结合。沸石例如可以为β型沸石(β~type zeolite)、Y型沸石(Y-typezeolite)、镁碱沸石(ferrierite)、ZSM-5型沸石(ZSM-5-typezeolite)、丝光沸石(modernite)、八面沸石(faujasite)、A型沸石(zeolite A)以及L型沸石(zeolite L)等。可以使用这些沸石中的一种或多种。
沸石中的二氧化硅(silica)与氧化铝(alumina)的摩尔比(硅铝的比)最好为30~50。
另外,最好还包含对上述沸石进行了离子交换的离子交换沸石。可以使用事先进行了离子交换的离子交换沸石来形成蜂窝单元,也可以在形成蜂窝单元后再对沸石进行离子交换。离子交换沸石最好使用例如用Fe、Cu、Ni、Co、Zn、Mn、Ti、Ag以及V中的至少一种金属进行了离子交换的沸石。这些离子交换沸石可以使用一种金属,也可以使用多种金属。
蜂窝单元的单位表观体积的沸石含量最好为230~270g/L。从另一方面来看,蜂窝单元中的沸石含有率(成分比例)最好为60~80质量%。因为沸石是用来净化NOX的,所以蜂窝单元中的沸石含量越多越好。但是,如果只增加沸石含量,必须减少其他构成物质(例如,无机纤维或无机粘结剂)的含量,因此,蜂窝单元的强度就会降低。另外,如果为了增加沸石含量,而过分地减小开口率,则在NOX净化反应中,有时废气的流动阻力就会变得过大。
沸石包含二次颗粒,沸石的二次颗粒的平均颗粒直径最好为0.5~10μm。需要注意的是,二次颗粒的平均直径可以通过使用沸石颗粒来测量,该沸石颗粒是通过烧成制成蜂窝单元之前的、形成了二次颗粒的颗粒状的原料。
(无机粘结剂)
在蜂窝单元中,无机粘结剂中的水分等被蒸发,仅留下固体成分。当言及蜂窝单元中的无机粘结剂时,是指该无机粘结剂中的固体成分。原料阶段的无机粘结剂例如可以是无机胶体溶液(inorganic sol)或粘土系粘结剂(clay based binder)等。其中,无机胶体溶液可以是例如氧化铝胶体溶液(alumina sol)、二氧化硅胶体溶液(silica sol)、二氧化钛胶体溶液(titania sol)、海泡石胶体溶液(meerschaum sol)、绿坡缕石胶体溶液(attapulgite sol)以及水玻璃(liquid glass)等;粘土系粘结剂可以是例如白土(white clay)、高岭土(kaolin)、蒙脱石(montmorillonite)、多链结构型粘土(multiple chain type clay)(海泡石(meerschaum)、绿坡缕石(attapulgite))等。这些无机胶体溶液或粘土系粘结剂可以使用一种,也可以将2种以上混合使用。蜂窝单元中的无机粘结剂以固体成分计的含量较好为5~30质量%,最好为10~20质量%。无机粘结剂以固体成分计的含量如果不在5~30质量%的范围内,则形成蜂窝单元时的成型性就会下降。
(无机纤维)
在本发明的蜂窝结构体中,蜂窝单元中还可以包含无机纤维。对蜂窝单元中包含的无机纤维没有特别的限定,可以是氧化铝纤维(alumina fiber)、二氧化硅纤维(silica fiber)、碳化硅纤维(silicon fiber)、硅铝纤维(silica-alumina fiber)、玻璃纤维(glassfiber)、钛酸钾纤维(potassium titanate fiber)以及硼酸铝纤维(aluminum borate fiber)中选出的一种或两种以上的无机纤维。这些无机纤维可以在原料阶段与沸石或无机粘结剂混合,然后通过成型、烧成制得蜂窝单元。无机纤维用于提高蜂窝单元的强度。需要注意的是,无机纤维既可以使用长纤维,也可以使用诸如晶须(whisker)的短纤维。
无机纤维是具有较大长径比(纤维长度/纤维直径)的无机材料,其对提高弯曲强度特别有效。无机纤维的长径比较好为2~1000,更好为5~800,最好为10~500。如果无机纤维的长径比小于2,则对提高蜂窝单元强度所起的作用很小;如果超过1000,对蜂窝单元进行成型时,成型模具内容易发生网眼堵塞等,导致成型性下降。另外,通过挤压成型对蜂窝单元进行成型时,有时无机纤维折断,长度出现不均,导致蜂窝单元强度下降。这里,如果无机纤维的长径比分布不均,则取其平均值。
蜂窝单元中包含的无机纤维的含量较好为3~50质量%,更好为3~30质量%,最好为5~20质量%。如果无机纤维的含量未满3质量%,则对提高蜂窝单元所起的作用很小;如果超过50质量%,则因为相对地减少了用于净化NOX的沸石含量,所以蜂窝结构体的NOX净化性能下降。
(无机颗粒)
在本发明的蜂窝结构体中,蜂窝单元还可以包含沸石颗粒以外的无机颗粒。沸石颗粒以外的无机颗粒具有提高蜂窝单元强度的功能。在本发明的蜂窝结构体中,对蜂窝单元中含有的沸石颗粒以外的无机颗粒并无特别限定,可以是例如氧化铝(alumina)、二氧化硅(silica)、氧化锆(zirconia)、二氧化钛(titania)、二氧化铈(ceria)、莫来石(mullite)以及它们的前驱体,最好是氧化铝或氧化锆,另外,γ氧化铝(γ-alumina)或软水铝石(boehmite,也称“勃姆石”)也比较适合。需要说明的是,这些沸石颗粒以外的无机颗粒可以包含一种或二种以上。
本发明的蜂窝结构体的无机颗粒在烧成前的原料无机颗粒阶段存在着氢氧基(hydroxyl group,也称“羟基”),与工业上使用的大多数无机化合物颗粒相同,本发明的蜂窝结构体的蜂窝单元中的、烧成前的原料沸石颗粒以外的无机颗粒和原料沸石颗粒中都存在着氢氧基。这些氢氧基在对蜂窝单元进行烧成时引起脱水缩合反应,具有强化颗粒间结合的作用。特别地,烧成时的脱水缩合反应可以牢固地结合以氧化铝为首的原料无机颗粒。
在本发明的蜂窝结构体的蜂窝单元中,作为原料来使用的除沸石颗粒以外的无机颗粒的二次颗粒的平均颗粒直径最好为小于或等于沸石的二次颗粒的平均颗粒直径。特别地,沸石颗粒以外的无机颗粒的平均颗粒直径最好为沸石颗粒的平均颗粒直径的1/10~1/1。这样,通过平均颗粒直径小的无机颗粒的结合力就可以提高蜂窝单元的强度。
蜂窝单元内含有的沸石颗粒以外的无机颗粒含量较好为3~30质量%,最好为5~20质量%。如果蜂窝单元中含有的沸石颗粒以外的无机颗粒含量未满3质量%,则对提高强度所起的作用很小。如果蜂窝单元中含有的无机颗粒含量超过30质量%,因为相对地减少了用于NOX净化的沸石含量,所以会导致NOX的净化性能降低。
(催化剂成分)
本发明的蜂窝结构体的蜂窝单元的孔格壁还担载催化剂成分。对催化剂成分并无特别限定,可以是例如从贵金属(nobel metal)、碱金属化合物(alkali metal compound)、碱土金属化合物(alkali earthmetal compound)等。贵金属可以是例如从铂、钯、铑中选出的一种或二种以上;碱金属化合物可以是例如从钾、钠等中选出的一种或二种以上的化合物;碱土金属化合物可以是例如钡等的化合物。
(蜂窝单元的制作)
对上述本发明的蜂窝结构体的蜂窝单元制造方法的一个例子进行说明。首先,制作含有主成分为上述沸石和无机粘结剂的原料浆,通过挤压成型等将其形成为蜂窝单元成型体。原料浆中除了上述沸石和无机粘结剂外,还可以适当地添加无机纤维、无机颗粒、有机粘结剂、造孔剂、分散介质以及成型助剂等。有机粘结剂并无特别的限定,但是,可以是例如从甲基纤维素(methylcellulose)、羧甲基纤维素(carboxymethyl cellulose)、羟乙基纤维素(hydroxylethylcellulose)、聚乙二醇(polyethyleneglycole)、酚醛树脂(phenolresin)以及环氧树脂(epoxy resin)等中选出的一种或二种以上的有机粘结剂。整个原料的固体成分合计为100质量份时,有机粘结剂的混合量最好为其中的1~10质量份。造孔剂可以使用丙烯酸系列树脂(acrylic acid based resin)、聚烯烃系列树脂(polyolefin basedresin)、聚苯乙烯系列树脂(polystyrene based resin)、聚酯系列树脂(polyester based resin)等的树脂粉末。有机粘结剂或造孔剂对挤压成型性、蜂窝单元的平均气孔直径Y或孔隙率的调整至关重要,可以对应于期望的平均气孔直径Y或孔隙率来调整造孔剂的大小和含量。对分散介质并无特别限定,可以是例如水、有机溶剂(甲苯(toluene)等)以及醇(甲醇(methanol)等)等。对成型助剂并无特别限定,可以是例如乙二醇(ethylene glycol)、糊精(dextrin)、脂肪酸皂(fatty acid soap)以及多元醇(polyalcohol)等。
原料浆并无特别限定,最好进行混合和混炼,例如,可以使用搅拌机或磨碎机等来混合,也可以使用捏合机等来进行充分的混炼。对原料浆的成型方法并无特别限定,例如,最好通过挤压成型等将其成型为具有预定孔格密度或开口率的形状。
其次,对得到的蜂窝单元成型体进行干燥。对用来进行干燥的干燥机并无特别限定,可以是微波干燥机、热风干燥机、高频干燥机、减压干燥机、真空干燥机以及冷冻干燥机等。最好对干燥后的成型体进行脱脂。对脱脂条件并无特别限定,可以根据成型体中含有的有机物的种类或含量进行适当的选择,最好在400℃下进行大约2小时的脱脂。然后,对干燥、脱脂后的蜂窝单元成型体进行烧成。对烧成条件并无特别限定,较好为在600~1200℃下进行大约2小时的烧成,最好为在600~1000℃下进行大约2小时的烧成。如果烧成温度未满600℃,则有时不能进行烧结,蜂窝单元的强度就不能提高。如果烧成温度超过1200℃,则有时会破坏沸石结晶,或者导致过度烧结,而不能制成具有适当孔隙率的多孔质蜂窝单元。
(蜂窝结构体)
本发明的蜂窝结构体具有一个或多个蜂窝单元。在具有多个蜂窝单元的蜂窝结构体中,每个蜂窝单元中的孔格的贯穿孔被垒积配置成朝向相同的方向。本发明的蜂窝结构体的例子示于图1(a)、图1(b)的立体图中。在图1(a)所示蜂窝结构体1中,多个蜂窝单元2通过粘结材料5结合配置。在每个蜂窝单元2中,孔格3平行排列。图1(b)所示的蜂窝结构体1是由一个蜂窝单元2构成的例子。这样,蜂窝结构体1即可以由一个蜂窝单元2构成,也可以由多个蜂窝单元2构成。需要注意的是,蜂窝结构体1的侧面(与孔格的长度方向平行的面,也简称为侧面,下同。)由于需要保持强度,最好覆盖被覆材料层6。
在图1(a)、图1(b)所示的蜂窝结构体中,截面为圆形,但是,在本发明的蜂窝结构体中,截面也可以为正方形、长方形、六边形或扇形等。蜂窝结构体的截面可以根据使用情况来决定,但在长度方向上最好保持相同的截面。另外,对蜂窝结构体的外周面可以进行切削加工,也可以不进行切削加工。
(蜂窝结构体的制作)
首先,对如图1(a)所示的、由多个蜂窝单元构成的蜂窝结构体的制造方法进行说明。在由上述方法得到的蜂窝单元侧面涂敷粘结剂,按顺序进行结合。对结合的蜂窝单元的接合体进行干燥固化,制成预定大小的蜂窝单元接合体。对蜂窝单元接合体的侧面进行切削加工,形成期望的形状。
对粘结材料并无特别限定,可以使用例如在无机粘结剂内混入无机颗粒的粘结材料、在无机粘结剂内混入无机纤维的粘结材料、或者、在无机粘结剂内混入无机颗粒和无机纤维的粘结材料。另外,也可以在这些粘结材料中添加有机粘结剂。对有机粘结剂并无特别限定,可以是例如聚乙烯醇(polyvinyl alcohol)、甲基纤维素(methylcellulose)、乙基纤维素(ethylcellulose)以及羧甲基纤维素(carboxymethyl cellulose)等中选出的一种或二种以上的有机粘结剂。
接合多个蜂窝单元的粘结材料层的厚度最好为0.5~2.0mm。接合的蜂窝单元的数量可以按照蜂窝结构体的大小来适当地确定。另外,由粘结材料接合蜂窝单元得到的蜂窝接合体可以按照蜂窝结构体的形状进行适当的切削和研磨等。
在蜂窝结构体的贯穿孔不开口的外周面(侧面)上涂敷被覆材,然后进行干燥固化,形成被覆材料层。这样,就可以保护蜂窝结构体的外表面,并可以提高强度。对被覆材并无特别限定,可以由与粘结材料相同的材料构成,也可以由与粘结材料不同的材料构成。另外,被覆材的混合比可以与粘结材料相同,也可以不同。对被覆材料层的厚度并无特别的限定,最好为0.1~2.0mm。需要注意的是,可以形成被覆材料层,也可以不形成被覆材料层。
由粘结材料接合多个蜂窝单元后,最好进行加热处理。设置了被覆材料层时,在形成粘结材料层和被覆材料层之后,最好进行脱脂。在粘结材料层或被覆材料层内含有有机粘结剂时,通过脱脂,可以去除其中的有机粘结剂。脱脂条件可以根据含有的有机物的种类和含量进行适当的确定,最好为大约在700℃下进行2小时左右的脱脂。
作为蜂窝结构体的一个例子的蜂窝结构体1的概念图示于图1(a)中,该蜂窝结构体1的外形为圆柱形,并接合了多个长方体的蜂窝单元2,蜂窝单元2的与贯穿孔的长度方向垂直的截面为正方形。在这个蜂窝结构体1中,通过粘结剂5结合了多个蜂窝单元2,在将外周面部切削成圆柱状后,由被覆材形成被覆材料层6。需要注意的是,将蜂窝单元2制成截面为扇形、以及、截面为正方形,并将这些蜂窝单元2结合,形成预定形状的蜂窝结构体时,也可以省略切削和研磨工序。
其次,对如图1(b)所示的、由一个蜂窝单元构成的蜂窝结构体的制造方法进行说明。图1(b)的蜂窝结构体除了是由一个蜂窝单元构成之外,可以采用与图1(a)同样的方法来制得。与上述由多个蜂窝单元构成的蜂窝结构体的制造方法中叙述的相同,根据实际要求,通过切削和研磨等将蜂窝单元做成圆柱形,并与上述方法同样地,通过在其外周部涂敷粘结材料形成被覆材料层,然后进行脱脂。这样,就可以制成如图1(b)所示的、由一个蜂窝单元构成的蜂窝结构体。
[实施例]
以下对在各种条件下制成的蜂窝结构体的实施例进行说明,但是,本发明并不限定于这些实施例。
(实施例1)
(蜂窝单元的制作)
首先,添加并混合2250质量份的Fe沸石颗粒(3质量%的Fe离子交换β型沸石、二氧化硅/二氧化铝之比为40、比表面积为110m2/g、平均颗粒直径为2μm(平均颗粒直径是二次颗粒的平均颗粒直径,下同))、980质量份的氧化铝纤维(平均纤维直径为6μm、平均纤维长度为100μm)、2600质量份的氧化铝胶体溶液(固体浓度为20质量%)、410质量份的有机粘结剂(甲基纤维素(methylcellulose))、200质量份的造孔剂(丙烯树脂粉末(acrylic resin poeder))(平均颗粒直径为0.75μm);然后,添加少量增塑剂、表面活性剂和润滑剂,一边加水调整粘度一边进行混合和混炼,得到用于成型的混合组合物。接下来,用挤压成型机对该混合组合物进行挤压成型,得到生蜂窝成型体。
使用微波干燥机和热风干燥机对得到的生蜂窝成型体进行充分干燥,并在400℃下进行2小时的脱脂。之后,在700℃下保持2小时进行烧成,制成蜂窝单元,该蜂窝单元为方柱形状(截面为35mm×35mm;长度为150mm)、壁厚为0.15mm、孔格密度为160个/cm2、平均气孔直径为0.25μm、单位表观体积的沸石含量为250g/L、孔隙率为35%、开口率为60%、孔格形状为四边形(正方形)。需要注意的是,Fe离子交换型沸石使用的是将沸石颗粒浸渍在硝酸铁铵(ferric nitrateammonium)溶液进行Fe离子交换后得到的离子交换型沸石。离子交换量使用ICPS~8100(岛津制作所制)通过IPC发光分析法来求得。
蜂窝单元的孔格厚度(孔格壁厚X)通过使用长度测量显微镜来测量,并求得10个测量样品的平均值。由显微镜观察得到的蜂窝单元孔格壁表面的气孔直径的平均值(平均气孔直径Y)是通过将蜂窝单元的孔格壁表面部分切割成边长为5mm的正方形,然后填入透明树脂,进行研磨,并将其作为测量样品得到的。对该测量样品进行SEM观察(2000倍),并将由SEM观察得到的图像输入计算机进行二值化处理,从二值化图像中求得平均气孔直径。
表1中列出了该蜂窝单元制作中使用的造孔剂的颗粒直径以及蜂窝单元的壁厚X、孔格密度、平均气孔直径Y、公式(1)中的Y值的上限和下限等。
表1
(蜂窝结构体的制作)
在制成的蜂窝单元的侧面涂敷粘结材料浆以形成厚度为1mm的粘结材料层,在120℃下进行干燥固化,制成蜂窝接合体,该蜂窝接合体是将蜂窝单元按4排、4列接合的大致长方体的结构。粘结材料浆是通过将29质量%的氧化铝颗粒(平均颗粒直径为2μm)、7质量%的氧化铝纤维(平均纤维直径为6μm、平均纤维长度为100μm)、34质量%的氧化铝胶体溶液(固体浓度为20质量%)、5质量%的羧甲基纤维素以及25质量%的水混合制成的。使用金刚石切割器对制成的蜂窝接合体的侧壁进行切割,使其变成为圆柱形状,在变成了圆柱形状的侧壁部分的外表面上涂敷厚度为0.5mm的上述粘结材料浆作为被覆材(与粘结材料相同),制成与图1(a)所示蜂窝结构体相同形状的圆柱形状蜂窝接合体。在120℃下对该圆柱形状蜂窝接合体进行干燥固化后,并在700℃下保持2小时对粘结材料层和被覆材进行脱脂,制成圆柱形状(直径144mm×长度150mm)的蜂窝结构体。
(实施例2~8、比较例1~7)
除了对造孔剂的颗粒直径以及挤压成型机的成型模具形状进行了变化外,采用与实施例1同样的方法制作实施例2~8和比较例1~7的蜂窝单元和蜂窝结构体。表1中列出了实施例2~8和比较例1~7的各例中制成的蜂窝单元的壁厚、孔格密度、平均气孔直径、公式(1)中的Y值的上限和下限。
(蜂窝结构体的NOX净化率的评价)
对实施例1~8和比较例1~7制成的蜂窝结构体的NOX净化率进行测量。
从实施例和比较例的各蜂窝单元体中切割出直径为30mm、长度为50mm的圆柱形状蜂窝体作为评价样品。在700℃下对得到的评价样品加热48小时,进行模拟老化处理后,将其保持在300℃,然后将表2所示成分的汽车废气的模拟气体加热至300℃,将其以35000hr~1的SV(空间速度)导入,并将通过评价样品之前和之后的模拟气体中的NO成分的减少率(%)作为NOX净化率(%)。表1中列出了实施例1~8、比较例1~7的评价样品的NOX净化率(%)测量结果。
表2
模拟气体 | 成分 |
N2 | 余量 |
CO2 | 5体积% |
O2 | 14体积% |
NO | 350ppm |
NH3 | 350ppm |
H2O | 5体积% |
SV(空间速度) | 35000/小时 |
由表1所示结果可知,实施例1~8所示蜂窝单元的评价样品的NOX净化率高达85%以上,而比较例1~7所示蜂窝单元的评价样品的NOX净化率却未满80%。需要注意的是,实施例1~8和比较例1~7的孔格壁的厚度X与蜂窝单元的平均气孔直径Y之间的关系示于图3所示的关系图内。在图3的关系图中,横轴表示蜂窝单元的孔格壁厚度X(mm),纵轴表示蜂窝单元的平均气孔直径Y(μm),实施例用○来表示,比较例用△来表示,○和△的编号分别代表实施例和比较例的编号。另外可知,实施例1~8在本发明的条件表达式(1)和(2)的范围内,而比较例1~7在其范围之外。
因此可知,实施例1~8所示的蜂窝单元适合用于对汽车废气进行净化处理。
本发明并不局限于上述具体实施例,只要不脱离权利要求书的范围,亦可采用其他变化形式代替,但那些变化形式仍属于本发明所涉及的范围。
工业实用性
本发明的蜂窝结构体的NOX净化率高,所以可作为小型、轻量化的汽车废气净化用催化剂来使用。特别适合作为使用沸石的SCR系统(例如使用氨的柴油废气净化系统)的NOX还原催化剂。
Claims (12)
1.一种蜂窝结构体,其具有包含沸石和无机粘结剂的蜂窝单元,该蜂窝单元形成为沿长度方向从一个端面延伸至另一个端面的多个孔格被孔格壁分隔而形成的形状,所述蜂窝结构体的特征在于,
所述蜂窝单元的单位表观体积的沸石含量为230g/L以上,
如果所述孔格壁的厚度为X毫米、所述孔格壁表面的由显微镜观察到的平均气孔直径为Y微米,则满足X+0.07≤Y≤X+0.27和0.15≤X≤0.35,
所述蜂窝单元的所述孔格壁表面的平均气孔直径Y采用如下方法求得:使用反射型电子显微镜SEM或光学显微镜观察所述孔格壁表面,通过图像处理技术取得一定范围内的图像中的气孔,计算平均气孔直径。
2.根据权利要求1所述的蜂窝结构体,其特征在于,
所述蜂窝单元的单位表观体积的沸石含量为270g/L以下。
3.根据权利要求1或2所述的蜂窝结构体,其特征在于,
所述孔格壁的气孔率为25%~40%。
4.根据权利要求1所述的蜂窝结构体,其特征在于,
所述蜂窝单元的开口率为50~60%。
5.根据权利要求1所述的蜂窝结构体,其特征在于,
所述沸石至少包含β型沸石、Y型沸石、镁碱沸石、ZSM-5型沸石、丝光沸石、八面沸石、A型沸石以及L型沸石中的任意一种。
6.根据权利要求1所述的蜂窝结构体,其特征在于,
所述沸石中的二氧化硅与氧化铝的摩尔比为30~50。
7.根据权利要求1所述的蜂窝结构体,其特征在于,
所述沸石至少用Fe、Cu、Ni、Co、Zn、Mn、Ti、Ag以及V中的任意一种进行了离子交换。
8.根据权利要求1所述的蜂窝结构体,其特征在于,
所述蜂窝单元至少包含氧化铝颗粒、二氧化钛颗粒、二氧化硅颗粒、氧化锆颗粒、二氧化铈颗粒、莫来石颗粒以及这些颗粒的前驱体中的任意一种。
9.根据权利要求1所述的蜂窝结构体,其特征在于,
所述无机粘结剂至少包含氧化铝胶体溶液、二氧化硅胶体溶液、二氧化钛胶体溶液、水玻璃、海泡石胶体溶液以及绿坡缕石胶体溶液中的任意一种。
10.根据权利要求1所述的蜂窝结构体,其特征在于,
所述蜂窝单元包含无机纤维。
11.根据权利要求10所述的蜂窝结构体,其特征在于,
所述无机纤维至少包含氧化铝纤维、二氧化硅纤维、碳化硅纤维、硅铝纤维、玻璃纤维、钛酸钾纤维以及硼酸铝纤维中的任意一种。
12.根据权利要求1所述的蜂窝结构体,其特征在于,
多个所述蜂窝单元通过粘结材料结合在一起。
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EP (1) | EP2130597B8 (zh) |
KR (1) | KR101102294B1 (zh) |
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WO2012131916A1 (ja) * | 2011-03-29 | 2012-10-04 | イビデン株式会社 | ハニカム構造体およびハニカム構造体の製造方法 |
SI3365394T1 (sl) | 2015-10-21 | 2020-10-30 | Tronox Llc | Oplaščenja, ki znižujejo NOx in postopki za zniževanje NOx s pomočjo njih |
JP6581926B2 (ja) * | 2016-03-07 | 2019-09-25 | 日本碍子株式会社 | ハニカム構造体 |
USD837356S1 (en) * | 2016-09-15 | 2019-01-01 | Ngk Insulators, Ltd. | Catalyst carrier for exhaust gas purification |
CN108993613A (zh) * | 2018-08-15 | 2018-12-14 | 山东鑫澳节能环保科技有限公司 | 一种复合陶瓷纤维结构及其制备方法和应用 |
JP6940787B2 (ja) | 2019-07-31 | 2021-09-29 | 株式会社デンソー | 排ガス浄化フィルタ |
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JP2675321B2 (ja) | 1987-01-27 | 1997-11-12 | 株式会社日本触媒 | ディーゼルエンジン排ガス中の窒素酸化物除去方法 |
MXPA02006446A (es) * | 1999-12-28 | 2002-11-29 | Corning Inc | Composiciones de soporte de catalizador de zeolita/alumina y metodos para elaborarlas. |
DE60023743T2 (de) * | 1999-12-29 | 2006-07-27 | Corning Incorporated | Katalysator mit hoher widerstandskraft und grosser oberfläche, katalysatorträger oder adsorberverbindungen |
JP2004024026A (ja) * | 2002-06-21 | 2004-01-29 | National Food Research Institute | キトサン加水分解活性に関与する機能性を有するポリペプチド、該ポリペプチドをコードする遺伝子、該遺伝子を含むベクター及び該ベクターを導入した形質転換体 |
JP2004202426A (ja) * | 2002-12-26 | 2004-07-22 | Toyota Motor Corp | 排ガス浄化用触媒 |
JP4815108B2 (ja) | 2003-12-26 | 2011-11-16 | イビデン株式会社 | ハニカム構造体 |
CN100534617C (zh) * | 2005-06-24 | 2009-09-02 | 揖斐电株式会社 | 蜂窝结构体 |
KR100725435B1 (ko) | 2005-12-30 | 2007-06-07 | 이비덴 가부시키가이샤 | 허니컴 구조체 |
JP2007296514A (ja) * | 2006-04-07 | 2007-11-15 | Ngk Insulators Ltd | 触媒体とその製造方法 |
DE102006020158B4 (de) * | 2006-05-02 | 2009-04-09 | Argillon Gmbh | Extrudierter Vollkatalysator sowie Verfahren zu seiner Herstellung |
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EP2130597B8 (en) | 2015-03-18 |
CN101585000A (zh) | 2009-11-25 |
KR20090121203A (ko) | 2009-11-25 |
KR101102294B1 (ko) | 2012-01-03 |
EP2130597A2 (en) | 2009-12-09 |
EP2130597A3 (en) | 2010-02-24 |
US8221867B2 (en) | 2012-07-17 |
US20090291256A1 (en) | 2009-11-26 |
EP2130597B1 (en) | 2014-09-17 |
WO2009141877A1 (ja) | 2009-11-26 |
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