CN101585002A - 蜂窝结构体 - Google Patents
蜂窝结构体 Download PDFInfo
- Publication number
- CN101585002A CN101585002A CNA2009101369417A CN200910136941A CN101585002A CN 101585002 A CN101585002 A CN 101585002A CN A2009101369417 A CNA2009101369417 A CN A2009101369417A CN 200910136941 A CN200910136941 A CN 200910136941A CN 101585002 A CN101585002 A CN 101585002A
- Authority
- CN
- China
- Prior art keywords
- honeycomb structured
- structured body
- zeolite
- duct
- cellular unit
- 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.)
- Pending
Links
- 229910021536 Zeolite Inorganic materials 0.000 claims abstract description 52
- 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 52
- 239000010457 zeolite Substances 0.000 claims abstract description 52
- 239000011230 binding agent Substances 0.000 claims abstract description 30
- 210000002421 cell wall Anatomy 0.000 claims abstract description 16
- 230000001413 cellular effect Effects 0.000 claims description 52
- PNEYBMLMFCGWSK-UHFFFAOYSA-N Alumina Chemical compound [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims description 43
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims description 28
- 239000000463 material Substances 0.000 claims description 22
- 239000010954 inorganic particle Substances 0.000 claims description 16
- 239000000377 silicon dioxide Substances 0.000 claims description 14
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 claims description 8
- MCMNRKCIXSYSNV-UHFFFAOYSA-N Zirconium dioxide Chemical compound O=[Zr]=O MCMNRKCIXSYSNV-UHFFFAOYSA-N 0.000 claims description 8
- 239000004113 Sepiolite Substances 0.000 claims description 5
- 229960000892 attapulgite Drugs 0.000 claims description 5
- 238000005342 ion exchange Methods 0.000 claims description 5
- 229910052625 palygorskite Inorganic materials 0.000 claims description 5
- 235000019353 potassium silicate Nutrition 0.000 claims description 5
- 235000019355 sepiolite Nutrition 0.000 claims description 5
- 229910052624 sepiolite Inorganic materials 0.000 claims description 5
- 229910010413 TiO 2 Inorganic materials 0.000 claims description 4
- 229910052802 copper Inorganic materials 0.000 claims description 4
- 239000010949 copper Substances 0.000 claims description 4
- 229910052742 iron Inorganic materials 0.000 claims description 4
- 235000012239 silicon dioxide Nutrition 0.000 claims description 4
- NTHWMYGWWRZVTN-UHFFFAOYSA-N sodium silicate Chemical compound [Na+].[Na+].[O-][Si]([O-])=O NTHWMYGWWRZVTN-UHFFFAOYSA-N 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 3
- NJLLQSBAHIKGKF-UHFFFAOYSA-N dipotassium dioxido(oxo)titanium Chemical compound [K+].[K+].[O-][Ti]([O-])=O NJLLQSBAHIKGKF-UHFFFAOYSA-N 0.000 claims description 3
- 239000012013 faujasite Substances 0.000 claims description 3
- 229910001657 ferrierite group Inorganic materials 0.000 claims description 3
- 239000011521 glass Substances 0.000 claims description 3
- 229910052748 manganese Inorganic materials 0.000 claims description 3
- -1 modenite Substances 0.000 claims description 3
- 229910052759 nickel Inorganic materials 0.000 claims description 3
- 229910010271 silicon carbide Inorganic materials 0.000 claims description 3
- 229910052709 silver Inorganic materials 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
- 229910052720 vanadium Inorganic materials 0.000 claims description 3
- 229910052725 zinc Inorganic materials 0.000 claims description 3
- 210000004027 cell Anatomy 0.000 abstract description 5
- 239000003054 catalyst Substances 0.000 description 22
- 230000000052 comparative effect Effects 0.000 description 19
- 239000002912 waste gas Substances 0.000 description 19
- 239000004202 carbamide Substances 0.000 description 16
- XSQUKJJJFZCRTK-UHFFFAOYSA-N Urea Chemical compound NC(N)=O XSQUKJJJFZCRTK-UHFFFAOYSA-N 0.000 description 15
- 238000011068 loading method Methods 0.000 description 14
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 description 12
- 239000000203 mixture Substances 0.000 description 10
- 239000002002 slurry Substances 0.000 description 9
- 239000007789 gas Substances 0.000 description 8
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 7
- 229910021529 ammonia Inorganic materials 0.000 description 6
- 238000005238 degreasing Methods 0.000 description 6
- 238000000034 method Methods 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
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- 229920000609 methyl cellulose Polymers 0.000 description 5
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- 230000002093 peripheral effect Effects 0.000 description 4
- UHOVQNZJYSORNB-UHFFFAOYSA-N Benzene Chemical compound C1=CC=CC=C1 UHOVQNZJYSORNB-UHFFFAOYSA-N 0.000 description 3
- LYCAIKOWRPUZTN-UHFFFAOYSA-N Ethylene glycol Chemical compound OCCO LYCAIKOWRPUZTN-UHFFFAOYSA-N 0.000 description 3
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 description 3
- 238000006243 chemical reaction Methods 0.000 description 3
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- 239000002994 raw material Substances 0.000 description 3
- 239000005995 Aluminium silicate Substances 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
- 239000004354 Hydroxyethyl cellulose Substances 0.000 description 2
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- 235000012211 aluminium silicate Nutrition 0.000 description 2
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- 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 2
- 238000005516 engineering process Methods 0.000 description 2
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- 235000019447 hydroxyethyl cellulose Nutrition 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
- 239000002609 medium Substances 0.000 description 2
- PXHVJJICTQNCMI-UHFFFAOYSA-N nickel Substances [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 2
- 229910000510 noble metal Inorganic materials 0.000 description 2
- 238000005457 optimization Methods 0.000 description 2
- 230000003647 oxidation Effects 0.000 description 2
- 238000007254 oxidation reaction Methods 0.000 description 2
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- 229920000647 polyepoxide Polymers 0.000 description 2
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- 229920002451 polyvinyl alcohol Polymers 0.000 description 2
- 239000011148 porous material Substances 0.000 description 2
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- 230000008023 solidification Effects 0.000 description 2
- 238000009955 starching Methods 0.000 description 2
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 2
- KXGFMDJXCMQABM-UHFFFAOYSA-N 2-methoxy-6-methylphenol Chemical compound [CH]OC1=CC=CC([CH])=C1O KXGFMDJXCMQABM-UHFFFAOYSA-N 0.000 description 1
- 239000004925 Acrylic resin Substances 0.000 description 1
- 229920000178 Acrylic resin Polymers 0.000 description 1
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 1
- 239000004215 Carbon black (E152) Substances 0.000 description 1
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 1
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 1
- 239000004375 Dextrin Substances 0.000 description 1
- 229920001353 Dextrin Polymers 0.000 description 1
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 1
- 239000002253 acid Substances 0.000 description 1
- 125000001931 aliphatic group Chemical group 0.000 description 1
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 1
- OSGAYBCDTDRGGQ-UHFFFAOYSA-L calcium sulfate Chemical compound [Ca+2].[O-]S([O-])(=O)=O OSGAYBCDTDRGGQ-UHFFFAOYSA-L 0.000 description 1
- 229910002091 carbon monoxide Inorganic materials 0.000 description 1
- 239000000919 ceramic Substances 0.000 description 1
- CETPSERCERDGAM-UHFFFAOYSA-N ceric oxide Chemical compound O=[Ce]=O CETPSERCERDGAM-UHFFFAOYSA-N 0.000 description 1
- 229910000422 cerium(IV) oxide Inorganic materials 0.000 description 1
- 239000003638 chemical reducing agent Substances 0.000 description 1
- 238000002485 combustion reaction Methods 0.000 description 1
- 239000000470 constituent Substances 0.000 description 1
- 238000010276 construction Methods 0.000 description 1
- 230000006837 decompression Effects 0.000 description 1
- 230000007423 decrease Effects 0.000 description 1
- 238000001514 detection method Methods 0.000 description 1
- 235000019425 dextrin Nutrition 0.000 description 1
- 229910003460 diamond Inorganic materials 0.000 description 1
- 239000010432 diamond Substances 0.000 description 1
- 239000002283 diesel fuel Substances 0.000 description 1
- 235000014113 dietary fatty acids Nutrition 0.000 description 1
- 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 description 1
- 239000002612 dispersion medium Substances 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
- 238000004108 freeze drying Methods 0.000 description 1
- 239000010439 graphite Substances 0.000 description 1
- 229910002804 graphite Inorganic materials 0.000 description 1
- 229930195733 hydrocarbon Natural products 0.000 description 1
- 150000002430 hydrocarbons Chemical class 0.000 description 1
- 239000000314 lubricant Substances 0.000 description 1
- 238000003754 machining Methods 0.000 description 1
- 238000005259 measurement Methods 0.000 description 1
- 239000003595 mist Substances 0.000 description 1
- 229910052863 mullite Inorganic materials 0.000 description 1
- 239000003960 organic solvent Substances 0.000 description 1
- 239000005022 packaging material Substances 0.000 description 1
- 239000004014 plasticizer Substances 0.000 description 1
- 238000002360 preparation method Methods 0.000 description 1
- 238000012545 processing Methods 0.000 description 1
- RMAQACBXLXPBSY-UHFFFAOYSA-N silicic acid Chemical compound O[Si](O)(O)O RMAQACBXLXPBSY-UHFFFAOYSA-N 0.000 description 1
- 238000004513 sizing Methods 0.000 description 1
- 239000000344 soap Substances 0.000 description 1
- 238000005728 strengthening Methods 0.000 description 1
- 150000005846 sugar alcohols Polymers 0.000 description 1
- 238000012360 testing method Methods 0.000 description 1
- WTHDKMILWLGDKL-UHFFFAOYSA-N urea;hydrate Chemical compound O.NC(N)=O WTHDKMILWLGDKL-UHFFFAOYSA-N 0.000 description 1
- 150000003672 ureas Chemical class 0.000 description 1
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- B01J29/69—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of the ferrierite type, e.g. types ZSM-21, ZSM-35 or ZSM-38, as exemplified by patent documents US4046859, US4016245 and US4046859, respectively containing arsenic, antimony, bismuth, vanadium, niobium, tantalum, polonium, chromium, molybdenum, tungsten, manganese, technetium or rhenium
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Abstract
本发明的目的在于提供一种针对具有各种全长及直径的蜂窝结构体也能得到适当的NOx净化性能的蜂窝结构体。该蜂窝结构体由蜂窝单元构成,该蜂窝单元包含沸石和无机粘结剂且沿着长度方向从第一端面延伸至第二端面的多个孔道被孔道壁隔开,所述蜂窝结构体的特征在于,所述孔道的垂直于长度方向的截面实质上为正方形状,所述蜂窝单元的开口率为50~65%,当将所述蜂窝结构体的体积设定为V升、所述孔道的孔道宽度设定为wc厘米、所述孔道的长度方向的长度设定为Lc厘米时,式12.5V+50<Lc/wc<12.5V+200成立。
Description
技术领域
本发明涉及一种处理废气的蜂窝结构体。
背景技术
关于汽车废气的净化,已经开发了很多技术,但由于交通量也在增加,因此还很难说已经采取了充分的对付废气的方法。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。以往,通过控制发动机的燃烧系统来谋求减少NOx,但仅此不能完全对付废气。作为对应于这种课题的柴油NOx净化系统,已经提出了一种将氨作为还原剂来使用的NOx还原系统(被称作SCR(选择性催化还原)系统)。作为应用于这种系统的催化剂担载体,众所周知的有蜂窝结构体。
该蜂窝结构体例如具有沿着长度方向从该蜂窝结构体的一侧端面延伸至另一侧端面的多个孔道(贯通孔),这些孔道被担载有催化剂的孔道壁相互隔开。因此,当废气流通到这种蜂窝结构体中时,通过担载在孔道壁上的催化剂来净化包含在废气中的NOx,从而可以处理废气。
通常,这种蜂窝结构体的孔道壁由堇青石(cordierite)构成,在该孔道壁上担载例如沸石(使用铁或铜等进行了离子交换的物质)作为催化剂。另外,还提出了一种在孔道壁上使用沸石而形成蜂窝结构体的发明(例如,专利文献1:日本特开昭61-171539号公报)
当将蜂窝结构体用作催化剂担载体时,其应用对象很广泛,例如从诸如卡车等大型车辆涉及到普通轿车。因此,蜂窝结构体中存在各种形状(尤其,全长及直径)。
另外,孔道的尺寸规格(尤其是孔道的宽度、孔道的全长)对蜂窝结构体的NOx净化性能带来很大影响。因此,针对具有各种形状的各蜂窝结构体,应该将孔道的尺寸规格(尤其是孔道的宽度、孔道的全长)设定为最佳的值。但是,如果要对需求量少的特殊形状的蜂窝结构体也要求孔道的尺寸规格的最佳值、且基于该值而制作蜂窝结构体,则会导致效率低且成本上升。因此,实际上,蜂窝结构体的孔道的尺寸规格在很多情况下根据经验来确定,不能说对所有形状的蜂窝结构体的孔道的尺寸规格都进行了最佳化设计。并且,对于这种孔道的尺寸规格没有被最佳化的蜂窝结构体而言,当这种蜂窝结构体被用作催化剂担载体时,经常出现得不到充分的NOx净化性能的情况。
发明内容
本发明是为了解决这种问题而提出的,其目的在于提供一种蜂窝结构体,该蜂窝结构体在具有各种全长及直径时都能得到合适的NOx净化性能。
本发明所提供的蜂窝结构体,其由蜂窝单元构成,该蜂窝单元包含沸石和无机粘结剂且沿着长度方向从第一端面延伸至第二端面的多个孔道被孔道壁隔开,所述蜂窝结构体的特征在于,所述孔道的垂直于长度方向的截面实质上为正方形状,所述蜂窝单元的开口率为50~65%,当将所述蜂窝结构体的体积设定为V(升)、所述孔道的孔道宽度设定为wc(cm)、所述孔道的长度方向的长度设定为Lc(cm)时,12.5V+50<Lc/wc<12.5V+200成立。
在本发明中,包含在所述蜂窝单元中的沸石可以为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型沸石或L型沸石。
并且,包含在所述蜂窝单元中的沸石中,二氧化硅相对于氧化铝的重量比可以在30~50的范围内。
并且,包含在所述蜂窝单元中的沸石可以使用Fe、Cu、Ni、Co、Zn、Mn、Ti、Ag或V进行离子交换。
并且,所述蜂窝单元还可以包含沸石以外的无机颗粒。
并且,所述沸石以外的无机颗粒可以为从氧化铝、二氧化钛、二氧化硅和氧化锆中选择的至少一种物质。
并且,包含在所述蜂窝单元中的无机粘结剂可以包含从氧化铝溶胶、二氧化硅溶胶、二氧化钛溶胶、水玻璃、海泡石和绿坡缕石的组中选择的至少一种材料。
并且,所述蜂窝单元还可以包含无机纤维。
包含在所述蜂窝单元中的所述无机纤维可以是从氧化铝、二氧化硅、碳化硅、硅铝、玻璃、钛酸钾和硼酸铝的组中选择的至少一种物质。
并且,本发明的蜂窝结构体可以通过粘结层接合多个所述蜂窝单元而构成。
根据本发明可以提供一种蜂窝结构体,该蜂窝结构体可以针对具有各种全长及直径的蜂窝结构体能得到合适的NOx净化性能。
附图说明
图1为表示本发明的蜂窝结构体的一个例子的立体图。
图2为表示构成图1所示的蜂窝结构体的蜂窝单元的一个例子的立体图。
图3为表示本发明的蜂窝结构体的另一个例子的立体图。
图4为表示用于评价蜂窝结构体的NOx净化性能的装置结构的框图。
图5为在蜂窝结构体的体积(V)和孔道的全长(Lc)与孔道宽度(wc)之比(Lc/wc)的关系中,能得到良好的NOx净化性能的范围的图。
主要符号说明:
100为蜂窝结构体,110为第一端面,115为第二端面,120为外周涂覆层,121、122为孔道,123、124为孔道壁,130为蜂窝单元,150为粘结层,200为另一个蜂窝结构体,400为NOx净化性能的评价试验装置,405为柴油发动机,410为柴油氧化催化剂系统,415为柴油微粒过滤器,420为尿素SCR系统,425为尿素罐,430为催化剂担载体部。
具体实施方式
下面参照附图说明本发明的特征。
图1中示出根据本发明的蜂窝结构体。并且,图2中示出作为图1所示的蜂窝结构体的基本单位的蜂窝单元的一个例子。
如图1所示,本发明的蜂窝结构体100具有两个端面110、115。并且,在蜂窝结构体100的除了两个端面以外的外周面上形成外周涂覆层120。
蜂窝结构体100是例如通过粘结层150接合多个(在图1的例子中,纵向和横向各设置4列,共16个)图2中示出的柱状的陶瓷制蜂窝单元130之后,按照预定的形状(在图1的例子中为圆柱状)对外周侧进行切削加工而构成的。
如图2所示,蜂窝单元130具有沿着该蜂窝单元的长度方向从一端延伸至另一端且在两个端面开口的多个孔道(贯通孔)121、以及隔开该孔道的孔道壁123。孔道121的垂直于长度方向(Z方向)的截面实际上形成为正方形,一边的长度(下面简称“孔道宽度”)为wc。并且,孔道121的全长(也是蜂窝单元130的全长)为Lc。在此,蜂窝单元130包含有助于NOx净化的沸石。因此,当本发明的蜂窝结构体被用作NOx净化用的催化剂担载体时,孔道壁上不一定要设置贵金属催化剂。但是,孔道壁上可以进一步设置贵金属催化剂。
构成为这种结构的蜂窝结构体100,例如可以作为具有尿素罐的尿素SCR系统的催化剂担载体而使用。当废气流通到该尿素SCR系统中时,收容在尿素罐中的尿素与废气中的水发生反应而生成氨。
CO(NH2)2+H2O→2NH3+CO2 式(1)
当该氨与包含NOx的废气一起从蜂窝结构体100的一侧端面(例如,端面110)流入到各孔道中时,通过包含在孔道壁中的沸石的催化剂作用,该混合气体之间发生如下反应。
4NH3+4NO+O2→4N2+6H2O 式(2-1)
8NH3+6NO2→7N2+12H2O 式(2-2)
2NH3+NO+NO2→2N2+3H2O 式(2-3)
然后,从蜂窝结构体100的另一侧端面(例如端面115)排出净化后的废气。如此,通过将废气流通到蜂窝结构体100内,可以处理废气中的NOx。这里,给出了对尿素水进行水解而供应NH3的方法,但也可以通过其它方法来供应NH3。
当将蜂窝结构体用作NOx净化用的催化剂担载体时,可以认为其应用对象很广泛,例如从诸如卡车等大型车辆涉及到普通轿车。因此,蜂窝结构体中存在各种形状(尤其,全长L及直径D(参照图1和图3))。
另外,孔道的尺寸规格(尤其是孔道的宽度wc、孔道的全长Lc(参照图2))对蜂窝结构体的NOx净化性能带来很大影响。因此,针对具有各种形状的各蜂窝结构体,应该将孔道的尺寸规格(尤其是孔道的宽度、孔道的全长)设定为最佳的值。但是,如果要对需求量少的特殊形状的蜂窝结构体也要求孔道的尺寸规格的最佳值、且基于该值而制作蜂窝结构体,则会导致效率低且成本上升。因此,实际上,蜂窝结构体的孔道的尺寸规格在很多情况下根据经验来确定,不能说对所有形状的蜂窝结构体的孔道的尺寸规格都进行了最佳化设计。并且,对于这种孔道的尺寸规格没有被最佳化的蜂窝结构体而言,当这种蜂窝结构体被用作催化剂担载体时,经常出现得不到充分的NOx净化性能的情况。
本申请的发明人针对这种问题反复进行了研究,研究结果发现了下面的情况,从而提出了本发明。
(1)在通常的情况下,通过使用蜂窝结构体的体积V,蜂窝结构体的形状、尤其是外径D及其全长L被定义为一个参数,
(2)对于具有正方形截面的孔道的尺寸规格而言,可以将孔道的全长Lc与孔道宽度wc之比即值Lc/wc定义为参数,以及
(3)通过将值Lc/wc设定在相对于蜂窝结构体的体积V的某一个范围内,可以得到能呈现出良好的NOx净化性能的蜂窝结构体。
即,如果将蜂窝结构体100的体积设定为V(升),将各孔道121的孔道宽度设定为wc(cm),将孔道的全长设定为Lc(cm)时,本发明的特征在于将孔道的尺寸规格设定为满足下述关系式:
12.5V+50<Lc/wc<12.5V+200 式(3)
据此,即使蜂窝结构体的体积V发生变化,也能得到最佳的NOx净化性能,即在具有各种全长及直径的蜂窝结构体中,可以总得到最佳的NOx净化性能。
在此,对蜂窝结构体的体积V的范围没有进行特殊限定,体积V最好在1L(升)≤V≤15L(升)的范围内。并且,孔道宽度wc最好在0.5cm≤wc≤2.0cm的范围内。如果孔道宽度未满0.5cm,则蜂窝结构体的压力损失变大,如果孔道宽度wc超过2.0cm,则几何表面积变小,因此NOx与沸石中的氨不能充分接触,导致NOx净化性能下降。并且,蜂窝单元130的开口率最好在50~65%的范围内。
下面,对本发明的蜂窝结构体的构成进行详细说明。
构成蜂窝结构体100的蜂窝单元130除了沸石之外还包含无机粘结剂。并且,蜂窝单元130还可以包含沸石以外的无机颗粒及/或无机纤维。
沸石可以为例如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型沸石或L型沸石。或者,沸石可以为使用Fe、Cu、Ni、Co、Zn、Mn、Ti、Ag或V进行了离子交换的物质。
并且,沸石中的二氧化硅相对于氧化铝的重量比最好在30~50的范围内。
作为无机粘结剂,可以使用无机溶胶或粘土系粘结剂等,作为无机溶胶的具体例子,例如有氧化铝溶胶(alumina sol)、二氧化硅溶胶(silica sol)、二氧化钛溶胶(titania sol)、水玻璃(liquid glass)等。并且,作为粘土系粘结剂,例如有白土(terra alba)、高岭土(kaolin)、蒙脱土(montmonrillonite)、海泡石(sepiolite)、绿坡缕石(attapulgite)等复链结构型粘土(multiple chain structure clay)等。这些可以单独使用或并用两种以上。
其中,最好使用由氧化铝溶胶、二氧化硅溶胶、二氧化钛溶胶、水玻璃、海泡石和绿坡缕石组成的组中选择的至少一种。
作为沸石以外的无机颗粒,最好使用氧化铝、二氧化硅、氧化锆、二氧化钛、二氧化铈、莫来石等构成的颗粒。这些颗粒可以单独使用或并用两种以上。其中,优选使用氧化铝、氧化锆。
当在蜂窝单元中加入无机纤维时,作为无机纤维的材料,最好使用氧化铝、二氧化硅、碳化硅、硅铝、玻璃、钛酸钾或硼酸铝等。这些可以单独使用,也可以并用两种以上。在上述材料中,最好使用氧化铝。在此,无机纤维中包含晶须(whisker)。
就包含在蜂窝单元中的无机颗粒(沸石及除沸石以外的无机颗粒)的含量而言,下限最好为30重量%,优选为40重量%,最优选为50重量%。另外,上限最好为90重量%,优选为80重量%,最优选为75重量%。如果无机颗粒(沸石及除沸石以外的无机颗粒)的含量未满30重量%,则有助于净化废气的沸石的量相对减少。另外,如果超过90重量%,则蜂窝单元的强度可能降低。
并且,沸石中的二氧化硅相对于氧化铝的重量比最好在30~50的范围内。
无机粘结剂以固体成分计最好包含5重量%以上,优选包含10重量%以上,最优选包含15重量%以上。另外,无机粘结剂的含量以固体成分计最好包含50重量%以下,优选包含40重量%以下,最优选包含35重量%以下。如果无机粘结剂的量以固体成分计未满5重量%,则所制造的蜂窝单元的强度可能会降低。另外,如果无机粘结剂的量以固体成分计超过50重量%,则原料组合物的成型性可能下降。
当蜂窝单元中包含无机纤维时,无机纤维的总量的下限最好为3重量%,优选为5重量%,最优选为8重量%。另外,上限最好为50重量%,优选为40重量%,最优选为30重量%。如果无机纤维的含量未满3重量%,则无机纤维对蜂窝单元的强度的增加所起的作用减少,如果无机纤维的含量超过50重量%,则有助于净化废气的沸石的量相对减少。
蜂窝单元130的孔道密度最好在15.5~186个/cm2(100~1200cpsi)的范围内,优选在46.5~170个/cm2(300~1100cpsi)的范围内,最优选在62.0~155个/cm2(400~1000cpsi)的范围内。
对蜂窝单元130的孔道壁123的厚度并没有特殊限制,从强度方面考虑下限最好为0.1mm,从净化性能的观点考虑上限最好为0.4mm。
蜂窝结构体100的粘结层150以粘结层用浆作为原料而形成。对粘结层用浆并没有特殊限制,例如,可以使用无机颗粒和无机粘结剂的混合物、无机粘结剂和无机纤维的混合物、无机颗粒和无机粘结剂以及无机纤维的混合物等。并且,也可以在这些混合物中再加入有机粘结剂。
作为无机颗粒、无机粘结剂及无机纤维可以使用与构成上述蜂窝单元的材料相同的材料。对有机粘结剂并没有特殊限制,例如可以为从聚乙烯醇(polyvinyl alcohol)、甲基纤维素(methylcellulose)、乙基纤维素(ethylcellulose)以及羧甲基纤维素(carboxymethylcellulose)等中选择的一种以上物质。在有机粘结剂中,最好使用羧甲基纤维素。
粘结层的厚度最好在0.3~2.0mm的范围内。这是因为,如果粘结层的厚度未满0.3mm,则可能得不到足够的接合强度。另外,如果粘结层的厚度超过2.0mm,则压力损失可能增加。在此,所接合的蜂窝单元的数量可以根据蜂窝结构体大小来适当地确定。
蜂窝结构体100的外周涂覆层120使用与形成上述粘结材料层的材料相同的、包含无机颗粒、无机粘结剂及无机纤维并进一步包含有机粘结剂的浆作为原料而形成。外周涂覆层120可以使用与粘结层150相同或不同的材料,但最好使用相同的材料。这是由于使用相同的材料时,外周涂覆层难以发生剥离或裂开。可以根据需要在作为原料的浆中添加造孔剂,该造孔剂可以为氧化物系陶瓷成分的微小中空球体即空心球(balloon)、球状丙烯酸树脂颗粒或石墨等。外周涂覆层的最终厚度最好在0.1mm~2.0mm的范围内。
在此,上面的内容以如图1所示的通过粘结层150接合多个蜂窝单元130而构成的蜂窝结构体为例子进行了说明。
图3中示出本发明的蜂窝结构体的另一个构成例。在此,蜂窝结构体200除了由一个蜂窝单元构成之外,与蜂窝结构体100具有相同的结构,该蜂窝结构体200的蜂窝单元的多个孔道122被孔道壁124隔开且沿长度方向并列设置。需要说明的是,在图3的例子中,在蜂窝结构体200的外周面上设置了外周涂覆层120,但该外周涂覆层可以设置,也可以不设置。
(蜂窝结构体的制作方法)
下面说明本发明的蜂窝结构体的制造方法。需要说明的是,这里,以上述图1所示的由多个蜂窝单元构成的蜂窝结构体100的制造方法为例子进行说明。
首先,使用原料浆进行挤压成型等而制造蜂窝单元成型体,该原料浆中作为主成分而包含含有沸石的无机颗粒和无机粘结剂,根据需要还可以添加无机纤维。
在该原料浆中,除了上述材料之外,还可以根据成型性适当地添加有机粘结剂、分散介质(dispersion media)以及成型助剂。对有机粘结剂并没有特殊限制,例如可以是从甲基纤维素(methylcellulose)、羧甲基纤维素(carboxymethylcellulose)、羟乙基纤维素(hydroxyethylcellulose)、聚乙二醇(polyethyleneglycol)、酚醛树脂(phenolic resin)和环氧树脂(epoxy resin)等中选择的一种以上有机粘结剂。在无机颗粒、无机粘结剂及无机纤维的总量为100重量份时,有机粘结剂的混合量最好为1~10重量份。
对分散介质并没有特殊限制,例如可以是水、有机溶剂(苯等)、醇(甲醇等)等。对成型助剂并没有特殊限制,例如可以是乙二醇、糊精、脂肪酸、脂肪酸皂及多元醇等。
对原料浆并没有特殊限制,最好被混合和混炼,例如可以使用搅拌机(mixer)或磨碎机(attritor)等进行混合,也可以使用捏合机等进行充分混炼。对原料浆的成型方法并没有特殊限制,例如最好通过挤压成型等,将原料浆成型为具有孔道的形状。
然后,最好对所得到的成型体进行干燥。对用于干燥的干燥装置并没有特殊限制,可以是微波干燥装置、热风干燥装置、高频烘干装置、减压干燥装置、真空干燥装置及冷冻干燥装置等。并且,所得到的成型体最好进行脱脂。对脱脂条件并没有特殊限制,根据成型体中所包含的有机物种类和量来适当地进行选择,但最好为约400℃、2小时。并且,对所得到的成型体最好进行烧成。对烧成条件并没有特殊限制,但最好在600~1200℃烧成2小时左右,优选在600~1000℃烧成2小时左右。这是由于当烧成温度未满600℃时,不能进行烧结,蜂窝单元的强度会降低;当烧成温度超过1200℃时,导致过度烧结,沸石的反应位减少。
然后,在由上述工序得到的蜂窝单元的侧面以均匀的厚度涂布将成为粘结层的粘结层用浆,然后通过该粘结层用浆,在蜂窝单元上依次层叠其它蜂窝单元。通过重复该工序,制造预定大小(例如,纵向和横向各设置四个蜂窝单元)的蜂窝结构体。
然后,加热该蜂窝结构体,对粘结层用浆进行干燥固化,以此形成粘结层并固定各蜂窝单元。
然后,使用金刚石切割器等将蜂窝结构体切割成例如圆柱形状,以此制作所需外周形状的蜂窝结构体。
然后,在蜂窝结构体的外周面(侧面)上涂布涂覆层用浆之后,对该涂覆层用浆进行干燥固化而形成外周涂覆层。
然后,通过粘结层接合多个蜂窝单元之后(当设有外周涂覆层时,在形成外周涂覆层之后),对该蜂窝结构体进行脱脂。当粘结层用浆和外周涂覆层用浆中包含有机粘结剂时,通过该处理可以脱脂而除去这些有机粘结剂。脱脂条件可以根据所包含的有机物种类和量来适当地进行选择,在通常的情况下为700℃、2小时左右。
根据上述工序,可以制作图1中所示的蜂窝结构体。
[实施例]
下面,通过实施例来详细说明本发明。
[实施例1]
首先,在2250重量份的Fe沸石颗粒(平均粒径2μm)、550重量份的氧化铝颗粒(平均粒径2μm)、2600重量份的氧化铝溶胶(固体成分30重量%)、780重量份的氧化铝纤维(平均纤维长度100μm、平均纤维直径6μm)、410重量份的甲基纤维素中添加增塑剂及润滑剂(UNILUB)进行混合、混炼而得到混合组合物。Fe沸石颗粒是沸石的相对于沸石重量为3重量%的部分被Fe离子交换而成的物质。然后,通过挤压成形机对该混合组合物进行挤压成型,得到蜂窝单元成型体。
然后,使用微波干燥装置及热风干燥装置对这些成型体进行充分干燥,并在400℃保持2小时进行脱脂。然后,在700℃保持2小时进行烧成,由此制作蜂窝结构体(外径102mm×全长120mm,体积1L(升))(图3中示出的形状的蜂窝结构体)。蜂窝结构体的开口率为60%。并且,蜂窝结构体的孔道宽度wc为0.69mm,孔道壁的厚度为0.2mm,孔道密度为124个/cm2。
(实施例2~13)
根据与实施例1相同的工序制作了实施例2~13的蜂窝结构体。这些蜂窝结构体与实施例1的蜂窝结构体相比,改变了全长L、外径D、体积V、孔道宽度wc。但是,其它的参数值与实施例1相同。
表1中综合地示出了实施例1~13的各蜂窝结构体的全长L、外径D、体积V、孔道宽度wc及孔道的全长Lc与孔道宽度wc之比(Lc/wc)的值。在此,在表1中,由于孔道的全长Lc与蜂窝结构体的全长L相同,因此进行了省略。在表1中,A1及A2栏中分别示出了使用各蜂窝结构体的体积V并由A1=(12.5V+50)及A2=(12.5V+200)这两个式子求出的值。A1相当于上述式(3)的不等式左边的值,A2相当于上述式(3)的不等式右边的值。
[表1]
全长Lmm | 外径Dmm | 体积VL | 孔道宽度wcmm | 值Lc/wc- | A1- | A2- | NOx净化率% | |
实施例1 | 120 | 102 | 1.0 | 0.69 | 174 | 62 | 212 | 90 |
实施例2 | 120 | 102 | 1.0 | 1.05 | 114 | 62 | 212 | 96 |
实施例3 | 75 | 203 | 2.4 | 0.69 | 109 | 80 | 230 | 98 |
实施例4 | 75 | 203 | 2.4 | 0.88 | 85 | 80 | 230 | 85 |
实施例5 | 150 | 144 | 2.4 | 0.69 | 217 | 80 | 230 | 88 |
实施例6 | 150 | 144 | 2.4 | 0.88 | 170 | 80 | 230 | 98 |
实施例7 | 150 | 144 | 2.4 | 1.05 | 143 | 80 | 230 | 99 |
实施例8 | 170 | 133 | 2.4 | 0.88 | 193 | 80 | 230 | 93 |
实施例9 | 170 | 133 | 2.4 | 1.05 | 162 | 80 | 230 | 98 |
实施例10 | 220 | 241 | 10.0 | 0.69 | 319 | 175 | 325 | 90 |
实施例11 | 220 | 241 | 10.0 | 1.05 | 210 | 175 | 325 | 96 |
实施例12 | 250 | 275 | 15.0 | 0.69 | 362 | 238 | 388 | 92 |
实施例13 | 265 | 270 | 15.0 | 1.05 | 252 | 238 | 388 | 94 |
比较例1 | 50 | 157 | 1.0 | 1.05 | 48 | 62 | 212 | 78 |
比较例2 | 150 | 90 | 1.0 | 0.69 | 217 | 62 | 212 | 79 |
比较例3 | 120 | 102 | 1.0 | 0.53 | 226 | 62 | 212 | 74 |
比较例4 | 75 | 203 | 2.4 | 1.05 | 71 | 80 | 230 | 78 |
比较例5 | 150 | 144 | 2.4 | 0.53 | 283 | 80 | 230 | 68 |
比较例6 | 170 | 133 | 2.4 | 0.69 | 246 | 80 | 230 | 75 |
比较例7 | 160 | 280 | 10.0 | 1.05 | 152 | 175 | 325 | 78 |
比较例8 | 220 | 241 | 10.0 | 0.53 | 415 | 175 | 325 | 70 |
比较例9 | 235 | 235 | 10.0 | 0.69 | 341 | 175 | 325 | 77 |
比较例10 | 230 | 287 | 15.0 | 1.05 | 219 | 238 | 388 | 76 |
比较例11 | 280 | 259 | 15.0 | 0.69 | 406 | 238 | 388 | 76 |
(比较例1~11)
根据与实施例1相同的工序制作了比较例1~11的蜂窝结构体。这些蜂窝结构体与实施例1的蜂窝结构体相比,改变了全长L、外径D、体积V、孔道宽度wc。但是,其它的参数值与实施例1相同。
表1中综合地示出了比较例1~11的各蜂窝结构体的各形状参数及上述A1和A2的值。从表1中可知,实施例1~13的蜂窝结构体的Lc/wc的值在A1~A2的范围内。另外,比较例1~11的蜂窝结构体的Lc/wc的值处于A1~A2的范围之外。
(NOx净化性能的评价)
使用上述的各蜂窝结构体进行了NOx净化性能的评价。
图4中示出NOx净化性能的评价试验装置的框图。该装置400由柴油发动机405、柴油氧化催化剂系统(DOC)410、柴油微粒过滤器(DPF)415和尿素SCR系统420以图中的顺序串联连接而构成。尿素SCR系统420由尿素罐425和催化剂担载体部430构成。催化剂担载体部430中设置上述实施例及比较例中的蜂窝结构体中的一种。
在该装置400中,从发动机405排出的废气最初被导入到DOC410。在DOC410中,废气中的一氧化碳及烃系气体被氧化。然后,从DOC410排出的气体被导入到DPF415,废气中的微粒(PM)在这里被清除。然后,从DPF415排出的气体被导入到尿素SCR系统420中。在尿素SCR系统420中,由尿素罐425向废气供应尿素,根据上述式(1)的反应而生成氨。含有该氨的废气接着被导入到催化剂担载体部430,在这里如上述式(2-1)、(2-2)、(2-3)所示,NOx被处理。然后,NOx得到处理的废气被排到系统外部。
在此,通过在图4中的A点和B点,即在尿素罐425和催化剂担载体部430之间以及尿素SCR系统420的出口侧的两个地方测定废气中的NO浓度,从而可以评价设置在催化剂担载体部430中的蜂窝结构体的NOx净化性能。
试验从起动发动机405开始一直持续到B点的NO浓度几乎不变为止。测定NO浓度时使用了HORIBA制的装置(MEXA-7100D)。该装置的NO检测限度为0.1ppm。根据设置在催化剂担载体部430中的蜂窝结构体的体积,对发动机405的转速及扭矩进行如下设定:
(1)当蜂窝结构体的体积V为1.0L(升)时,发动机转速为1000rpm,扭矩为100N·m,
(2)当蜂窝结构体的体积V为2.4L(升)时,发动机转速为1500rpm,扭矩为150N·m,
(3)当蜂窝结构体的体积V为10.0L(升)时,发动机的转速为3500rpm,扭矩为270N·m,
(4)当蜂窝结构体的体积V为15.0L(升)时,发动机的转速为4500rpm,扭矩为300N·m。
在此,发动机的容积总共为1.6L(升)。
根据所得到的测定结果计算出NOx净化率N。这里,NOx净化率N根据下式进行计算。
N(%)={(在A点的气体中的NO浓度-在B点的气体中的NO浓度)/(在A点的气体中的NO浓度)}×100 式(4)
将结果表示在表1的右栏中。并且,图5中示出了各实施例及比较例的蜂窝结构体的蜂窝结构体体积V和孔道全长Lc与孔道宽度wc之比(Lc/wc)的关系。在图5中,直线L1表示上述A1即A1=(12.5V+50)的关系。并且,直线L2表示上述A2即A2=(12.5V+200)的关系。因此,直线L1和L2之间的范围相当于满足上述式(3)的关系的区域。在图5中,用○表示实施例,用●表示比较例。
根据表1的结果可知,实施例1~13的蜂窝结构体与比较例1~11的蜂窝结构体相比,具有高的NOx净化性能。并且,从图5的曲线结果可知,当蜂窝结构体的体积V和值Lc/wc的关系在直线L1和L2之间的范围内时,蜂窝结构体呈现出良好的NOx净化性能。
Claims (10)
1、一种蜂窝结构体,其由蜂窝单元构成,该蜂窝单元包含沸石和无机粘结剂,在该蜂窝单元中,沿着长度方向从第一端面延伸至第二端面的多个孔道被孔道壁隔开,所述蜂窝结构体的特征在于,
所述孔道的垂直于长度方向的截面实质上为正方形状,
所述蜂窝单元的开口率为50%~65%,
当将所述蜂窝结构体的体积设定为V升、所述孔道的孔道宽度设定为wc厘米、所述孔道的长度方向的长度设定为Lc厘米时,下式成立
12.5V+50<Lc/wc<12.5V+200。
2、根据权利要求1所述的蜂窝结构体,其特征在于,所述沸石为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型沸石或L型沸石。
3、根据权利要求1或2所述的蜂窝结构体,其特征在于,在所述沸石中,二氧化硅相对于氧化铝的重量比在30重量%~50重量%的范围内。
4、根据权利要求1或2所述的蜂窝结构体,其特征在于,所述沸石使用Fe、Cu、Ni、Co、Zn、Mn、Ti、Ag或V进行了离子交换。
5、根据权利要求1或2所述的蜂窝结构体,其特征在于,所述蜂窝单元还包含沸石以外的无机颗粒。
6、根据权利要求5所述的蜂窝结构体,其特征在于,所述沸石以外的无机颗粒为从氧化铝、二氧化钛、二氧化硅和氧化锆中选择的至少一种物质。
7、根据权利要求1或2所述的蜂窝结构体,其特征在于,所述无机粘结剂包含从氧化铝溶胶、二氧化硅溶胶、二氧化钛溶胶、水玻璃、海泡石和绿坡缕石的组中选择的至少一种物质。
8、根据权利要求1或2所述的蜂窝结构体,其特征在于,所述蜂窝单元还包含无机纤维。
9、根据权利要求8所述的蜂窝结构体,其特征在于,所述无机纤维是从氧化铝、二氧化硅、碳化硅、硅铝、玻璃、钛酸钾和硼酸铝的组中选择的至少一种物质。
10、根据权利要求1或2所述的蜂窝结构体,其特征在于,所述蜂窝结构体是通过粘结层将多个所述蜂窝单元接合起来而构成的。
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JP2019058875A (ja) * | 2017-09-27 | 2019-04-18 | イビデン株式会社 | ハニカム触媒 |
JP6698602B2 (ja) * | 2017-09-27 | 2020-05-27 | イビデン株式会社 | 排ガス浄化用ハニカム触媒 |
JP2019058876A (ja) | 2017-09-27 | 2019-04-18 | イビデン株式会社 | ハニカム触媒 |
JP6684257B2 (ja) * | 2017-09-27 | 2020-04-22 | イビデン株式会社 | 排ガス浄化用ハニカム触媒 |
WO2019195406A1 (en) | 2018-04-04 | 2019-10-10 | Unifrax | Llc | Activated porous fibers and products including same |
WO2020121607A1 (ja) * | 2018-12-10 | 2020-06-18 | 日本碍子株式会社 | 還元剤噴射装置、排ガス処理装置及び排ガス処理方法 |
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ATE130831T1 (de) * | 1991-01-07 | 1995-12-15 | Takeda Chemical Industries Ltd | Verfahren zur formgebung und zum brennen von zeolith-pulver. |
CN100441287C (zh) | 2002-04-18 | 2008-12-10 | 触媒化成工业株式会社 | 蜂窝状废气处理催化剂用二氧化钛粉末及废气处理催化剂 |
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WO2006070540A1 (ja) * | 2004-12-27 | 2006-07-06 | Ibiden Co., Ltd. | セラミックハニカム構造体 |
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WO2007074507A1 (ja) * | 2005-12-26 | 2007-07-05 | Ibiden Co., Ltd. | 粉末の混合方法、攪拌機、及び、ハニカム構造体の製造方法 |
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US11213781B2 (en) | 2017-01-31 | 2022-01-04 | Corning Incorporated | Pattern-plugged honeycomb bodies, particulate filters, and extrusion dies therefor |
CN110475599B (zh) * | 2017-01-31 | 2022-01-25 | 康宁股份有限公司 | 图案堵塞的蜂窝体、微粒过滤器及用于其的挤出模头 |
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