WO2000044672A1 - Procede de production hydrothermique d'argile anionique a l'aide de boehmite peptisee avec un acide inorganique - Google Patents
Procede de production hydrothermique d'argile anionique a l'aide de boehmite peptisee avec un acide inorganique Download PDFInfo
- Publication number
- WO2000044672A1 WO2000044672A1 PCT/EP2000/000611 EP0000611W WO0044672A1 WO 2000044672 A1 WO2000044672 A1 WO 2000044672A1 EP 0000611 W EP0000611 W EP 0000611W WO 0044672 A1 WO0044672 A1 WO 0044672A1
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- WO
- WIPO (PCT)
- Prior art keywords
- boehmite
- anionic clay
- slurry
- process according
- magnesium
- Prior art date
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Classifications
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01F—COMPOUNDS OF THE METALS BERYLLIUM, MAGNESIUM, ALUMINIUM, CALCIUM, STRONTIUM, BARIUM, RADIUM, THORIUM, OR OF THE RARE-EARTH METALS
- C01F7/00—Compounds of aluminium
- C01F7/02—Aluminium oxide; Aluminium hydroxide; Aluminates
- C01F7/16—Preparation of alkaline-earth metal aluminates or magnesium aluminates; Aluminium oxide or hydroxide therefrom
- C01F7/162—Magnesium aluminates
-
- 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
- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/007—Mixed salts
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01F—COMPOUNDS OF THE METALS BERYLLIUM, MAGNESIUM, ALUMINIUM, CALCIUM, STRONTIUM, BARIUM, RADIUM, THORIUM, OR OF THE RARE-EARTH METALS
- C01F7/00—Compounds of aluminium
- C01F7/78—Compounds containing aluminium and two or more other elements, with the exception of oxygen and hydrogen
- C01F7/784—Layered double hydroxide, e.g. comprising nitrate, sulfate or carbonate ions as intercalating anions
- C01F7/785—Hydrotalcite
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
- C01P2002/00—Crystal-structural characteristics
- C01P2002/20—Two-dimensional structures
- C01P2002/22—Two-dimensional structures layered hydroxide-type, e.g. of the hydrotalcite-type
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
- C01P2002/00—Crystal-structural characteristics
- C01P2002/70—Crystal-structural characteristics defined by measured X-ray, neutron or electron diffraction data
- C01P2002/72—Crystal-structural characteristics defined by measured X-ray, neutron or electron diffraction data by d-values or two theta-values, e.g. as X-ray diagram
Definitions
- This invention involves the preparation of anionic clays and the preparation of Mg-AI solid solutions by heat-treatment of the anionic clay.
- Anionic clays have a crystal structure which consists of positively charged layers built up of specific combinations of metal hydroxides between which there are anions and water molecules.
- Hydrotalcite is an example of a naturally occurring anionic clay, in which carbonate is the predominant anion present.
- Meixnerite is an anionic clay wherein OH " is the predominant anion present.
- the brucite-like main layers are built up of octahedra alternating with interlayers in which water molecules and anions, more particularly carbonate ions, are distributed.
- the interlayers contain anions such as NO 3 -, OH, Cl “ , Br, I “ , SO 4 2” , SiO 3 2 -, CrO 4 2” , BO 3 2 ⁇ MnO, " , HGaO, 2" , HV0 4 2” , CI0 4 ⁇ BO 3 2” , pillaring anions such as V ⁇ Ozs "6 and MO 7 O 24 6" , monocarboxylates such as acetate, dicarboxylates such as oxalate, alkyl sulphonates such as laurylsulphonate.
- anionic clays The preparation of anionic clays has been described in many prior art publications. Recently, two major reviews of anionic clay chemistry were published in which the synthesis methods available for anionic clay synthesis have been summarized, F. Cavani et al "Hydrotalcite-type anionic clays: Preparation, Properties and Applications," Catalysis Today” , 11 (1991) Elsevier Science Publishers B. V. Amsterdam.
- European Patent Application 0 536 979 describes a method for introducing pH- dependent anions into the clay.
- the clay is prepared by the addition of a solution of AI(NO 3 ) 3 and Mg(N0 3 ) 2 to a basic solution containing borate anions.
- the product is then filtered, washed repeatedly with water, and dried overnight. Additionally mixtures of Zn/Mg are used.
- the hydrotalcite is made by reacting activated MgO (prepared by activating a magnesium compound such as magnesium carbonate or magnesium hydroxide) with aqueous solutions containing aluminate, carbonate and hydroxyl ions.
- activated MgO prepared by activating a magnesium compound such as magnesium carbonate or magnesium hydroxide
- aqueous solutions containing aluminate, carbonate and hydroxyl ions As an example the solution is made from NaOH, Na 2 C0 3 and Al 2 0 3 .
- the synthesis involves the use of industrial Bayer liquor as the source of Al.
- the resulting products are washed and filtered before drying at 105 °C.
- a catalyst for removing sulphur oxides or nitrogen oxides from a gaseous mixture is made by calcining an anionic clay, said anionic clay having been prepared by co-precipitation of a solution of Mg(N0 3 ) 2 , AI(N0 3 ) 3 and Ce(N0 3 ) 3 .
- the product again is filtered and repeatedly washed with de-ionized water.
- Our invention includes processes for producing anionic clays using novel raw materials and utilizing such raw materials in a simple process which involves reacting mixtures with or without stirring in water at hydrothermal conditions. Such processes can be operated in standard laboratory/industrial equipment. More specifically, there is no need for washing or filtering, and a wide range of ratios of Mg/AI in the reaction product is possible.
- This invention involves the use of boehmite in aqueous suspensions, where at ambient or elevated temperature magnesium sources, for instance MgO or brucite, are added and the reaction mixture results in the direct formation of an anionic clay.
- the powder X-ray diffraction pattern (PXRD) suggests that the product is comparable to anionic clays made by other standard methods.
- the physical and chemical properties of the product are also comparable to those anionic clays made by the other conventional methods.
- the overall process of this invention is very flexible, enabling a wide variety of anionic clay compositions and anionic clay-like materials involving for example carbonate, hydroxide and other anions to be prepared in an economically and environmental-friendly manner.
- the process may be carried out in a one step process either in batch or in continuous mode
- Figure 1 (a) shows a PXRD pattern of commercially available Catapal ®.
- Figure 1(b) shows a PXRD pattern of commercially available P3 ® alumina.
- Figure 1(c) shows a PXRD pattern of commercially available Laroche ® alumina.
- Figure 2. shows a PXRD pattern of a commercially available anionic clay.
- Figure 3 shows a PXRD pattern of a Mg-AI carbonate anionic clay prepared by coprecipitation.
- This invention involves the preparation of anionic clays.
- it describes a process for the preparation of an anionic clay by reacting a slurry comprising boehmite which has been peptized with an inorganic acid and a magnesium source.
- Said magnesium source may be composed of a solution of a magnesium salt, a solid magnesium-bearing compound or a mixture of the two.
- Reaction between the Mg source and boehmite results in the direct formation of an anionic clay. Said reaction takes place at hydrothermal conditions.
- the reaction is preferably carried out under autogeneous conditions.
- carbonate, hydroxyl, or other anions or mixtures thereof either provided within the reaction medium for example as a soluble salt or absorbed during the synthesis from the atmosphere, are incorporated into the interlayer region as the necessary charge-balancing anion.
- Anionic clays prepared by this method exhibit the well known properties and characteristics (e.g. chemical analysis, powder X-ray diffraction pattern, FTIR, thermal decomposition characteristics, surface area, pore volume, and pore size distribution) usually associated with anionic clays prepared by the customary and previously disclosed methods.
- anionic clays Upon being heated, anionic clays generally form Mg-AI solid solutions, and at higher temperatures, spinels.
- an adsorbent for instance a SO x adsorbent for catalytic cracking reactions
- the anionic clay according to the invention is usually heated during preparation and is thus in the Mg-AI solid solution form.
- the catalyst or adsorbent is converted from an anionic clay into Mg-AI solid solutions .
- the present invention is also directed to a process wherein an anionic clay prepared by the reaction according to the invention, is heat-treated at a temperature between 300 and 1200 °C to form a Mg-AI-containing solid solution and/or spinel.
- the anionic clay according to the invention has a layered structure corresponding to the general formula
- X may be CO 3 2 ⁇ , OH " or any other anion normally present in the interlayers of anionic clays. It is more preferred that m/n should have a value of 2 to 4, more particularly a value close to 3.
- the product can be spray dried directly to form microspheres or can be extruded to form shaped bodies.
- the present invention includes the use of boehmite.
- boehmites and pseudoboehmites such as Catapal ®, Condea P3 ®, P200 ®, Laroche ® etcetera).
- the boehmite is peptized with inorganic acids. These types of acids are not expensive and the use of inorganic acids renders the process cost-effective. Suitable inorganic acids are nitric acid, Hydrochloric acid, sulfuric acid, sulfurous acid.sulfonic acid, phosphoric acid, phosphonic acid, phosphinic acid.
- boehmites and pseudoboehmites.
- other aluminium sources such as oxides and hydroxides of aluminium, (e.g. sols, aluminium trihydrate, and its thermally treated forms, flash calcined aluminium trihydrate), aluminium salts such as aluminium nitrate, aluminium chloride, aluminium chlorohydrate and sodium aluminate.
- Said other aluminium sources may be soluble or insoluble in water.
- Said different aluminium sources may be combined in any sequence in a slurry before and/or after the Mg source is added.
- Mg-bearing sources which may be used include MgO, Mg(OH) 2 , magnesium acetate, magnesium formate, magnesium hydroxy acetate, magnesium carbonate, magnesium bicarbonate, magnesium nitrate, magnesium chloride, dolomite, sepiolite.
- Preferred Mg sources are MgO, Mg(HO) 2 , and MgCO 3 , because they are cheap, readily available and reactive in the reaction of the present invention. Both solid Mg sources as soluble Mg salts are suitable. Also combinations of Mg sources may be used. Conditions
- Said aqueous suspension may be obtained by either combining slurries of the starting materials or adding magnesium source to a slurry of boehmite or vice versa.
- the acid to peptize the boehmite may be added prior to combining the Mg source with the boehmite or the acid may be added to the combined mg source -boehmite slurry
- the hydrothermal treatment can be conducted in an autoclave at temperatures above 100 °C and increased pressures. This is particularly advantageous, because it this is faster and a higher conversion is obtained compared to a conventional thermal treatement at atmospheric pressure. Further, larger crystals are obtained when using hydrothermal treatment. There is no need to wash or filter the product, as unwanted ions (e.g.
- the process is conducted in a two-step process, e.g. a slurry of boehmite and Mg source is treated thermally at a mild temperature, followed by a hydrothermal treatment.
- a preformed anionic clay may be added to the reaction mixture.
- Said preformed clay may be recycled anionic clay from the reaction mixture or anionic clay made separately by the process according to the invention or any other process.
- this process can be carried out in a continuous mode by mixing of a first slurry comprising boehmite and a second slurry comprising magnesium source passing the mixed slurry through a reactor vessel which can operate under hydrothermal/autogeneous conditions.
- Said first and/or second slurry may be subjected to a treatment prior to mixing the slurries.
- inorganic acids and bases for example for control of the pH, may be added to the slurry before or during reaction or to the individual reactants before combining them in the slurry.
- the anionic clay prepared by the process according to the invention may be subjected to ion exchange.
- ion exchange the interlayer charge- balancing anions are replaced with other anions.
- Said other anions are the ones commonly present in anionic clays and include pillaring anions such as V- Q O ⁇ "6 , MO 7 0 24 6" .
- Said ion exchange can be conducted before drying or after the anionic clay formed in the slurry.
- the process of the invention provides wide flexibility in preparing products with a wide range of Mg:AI ratios.
- the Mg:AI ratio can vary from 0.1 to 10 , preferably from 1 to 6, more preferred from 2 to 4, and especially preferred to close to 3.
- a composition which contains anionic clay and also unreacted boehmite.
- the anionic clay and boehmite are intimately mixed, rather than present as separate phases such as in physically mixed mixtures of anionic clay and boehmite.
- Said composition appears to be highly suitable for use as an additive of as a matrix for catalysts for hydrocarbon conversion. This composition appears especially suitable for sulphur removal from the gasoline and diesel fraction in FCC, SO x and NO x removal in FCC, and as a metal trap.
- the present invention is also directed to a composition containing anionic clay and boehmite. Said composition is obtainable by the process of the invention in which only part of the boehmite is reacted with magnesium source to obtain anionic clay. The rest of the boehmite remains unreacted in the composition.
- magnesium sources may also be used in excess to obtain a composition containing anionic clay and a magnesium compound, ususally in the form of an oxide or hydroxide. It is even possible to prepare compositions containing anionic clay, boehmite and a magnesium compound with the process according to the invention by controlling the process conditions. In said compositions the anionic clay, magnesium compound, and optionally boehmite are intimately mixed, rather than present as separate phases such as in physically mixed mixtures of anionic clay, magnesium compound and boehmite. These compositions appear to be highly suitable for use as an additive or as a matrix for catalysts for hydrocarbon conversion. These compositions appear to be especially suitable for use as a metal trap in FCC.
- metals and non- metals such as rare earth metals, Si, P, B, group VI, group VIII, alkaline earth (for instance Ca and Ba) and/or transition metals (for example Mn, Fe, Ti, Zr, Cu, Ni, Zn, Mo, Sn), present.
- Said metals can easily be deposited on the anionic clay, the solid solution according to the invention, the composition containing anionic clay and boehmite or the composition containing magsesium source, anionic clay and optionally bohmite. They can also be added either to the alumina or magnesia source or to the slurry during preparation of the anionic clay.
- This comparative example illustrates the co-precipitation method where Mg and Al salt solutions are added to a solution of base.
- Thermogravimetric analysis showed three weight losses: at approximately 100, 250 and 450 °C which are ascribed to loss of physisorbed water, interlayer water and loss of C0 2 and lattice dehydroxylation.
- a slurry of 60.95 g Disperal P3 in 206 g deionized water was mixed in a blender for 5 minutes.
- the P3 slurry was peptized with HNO 3 (70 wt%) at a pH 1.32 for 15 minutes in a blender.
- a slurry containing 72.59 g MgO in 109 deinonized water was added and blended for 10 minutes.
- the Mg/AI ratio was 2.3.
- the pH of the resulting slurry was 8.5.
- the pH of the final slurry was adjusted to 9.2 with dilute NH 4 OH solution resulting in a final slurry solids of 25 wt%.
- the resulting slurry was heated in a sealed container at 90 °C for 48 hours, and the aged gel was dried overnight at 110 °C.
- the XRD pattern proved that an anionic clay was formed.
- a slurry of 60.95 g Disperal P3 in 206 g deionized water was mixed in a blender for 5 minutes.
- the P3 slurry was peptized with HNO 3 (70 wt%) at a pH 1.32 for 15 minutes in a blender.
- a slurry containing 72.59 g MgO in 109 deinonized water was added and blended for 10 minutes.
- the Mg/AI ratio was 2.3.
- the pH of the resulting slurry was 8.5.
- the pH of the final slurry was adjusted to 9.2 with dilute NH 4 OH solution resulting in a final slurry solids of 25 wt%.
- the resulting slurry was heated in a sealed container at 120 °C for 48 hours, and the aged gel was dried overnight at 110 °C.
- the XRD pattern proved that an anionic clay was formed.
- a slurry of 50.00 g Catapal A in 204 g deionized water was mixed in a blender for 5 minutes.
- the Catapal slurry was peptized with HNO 3 (70 wt%) at a pH 3.7 for 15 minutes in a blender.
- a solution containing 161.5 g magnesium nitrate (corresponding with 18.3 wt% MgO) was added and blended for 5 minutes.
- a slurry of 113.2 g MgO in 400 g deionized water was added and mixed for 10 minutes in the blender.
- the Mg/Alo ratio was 5.0.
- the pH of the resulting slurry was 8.5 with a solids content of 19 wt%.
- the resulting slurry was heated in a sealed container at 80 °C for 48 hours, and the aged gel was dried overnight at 100 °C.
- the XRD pattern proved that an anionic clay was formed.
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Abstract
L'invention concerne des procédés économiques et écologiques pour la synthèse d'argiles anioniques, par réaction hydrothermique avec une source de magnésium d'une suspension contenant de la boehmite, peptisée avec un acide inorganique. Il n'est pas nécessaire de laver ou de filtrer le produit obtenu, que l'on peut directement sécher par pulvérisation afin de former des microsphères ou que l'on peut extruder afin de former des corps moulés. On peut associer le produit obtenu à d'autres ingrédients afin de fabriquer des catalyseurs, des adsorbants, des produits pharmaceutiques et cosmétiques, des détergents et d'autres biens de consommation contenant des argiles anioniques.
Applications Claiming Priority (2)
Application Number | Priority Date | Filing Date | Title |
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US11793499P | 1999-01-29 | 1999-01-29 | |
US60/117,934 | 1999-01-29 |
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WO2000044672A1 true WO2000044672A1 (fr) | 2000-08-03 |
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PCT/EP2000/000611 WO2000044672A1 (fr) | 1999-01-29 | 2000-01-27 | Procede de production hydrothermique d'argile anionique a l'aide de boehmite peptisee avec un acide inorganique |
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Cited By (8)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
WO2002064504A1 (fr) | 2001-02-09 | 2002-08-22 | Akzo Nobel N.V. | Argiles anioniques dopees |
WO2002064499A2 (fr) * | 2001-02-09 | 2002-08-22 | Akzo Nobel N.V. | Procede de preparation de compositions renfermant de l'argile anionique et de la boehmite |
WO2004000731A2 (fr) * | 2002-06-25 | 2003-12-31 | Akzo Nobel N.V. | Utilisation de materiaux cationiques en couches, compositions comprenant lesdits materiaux et preparation de materiaux cationiques en couches |
WO2004020092A1 (fr) * | 2002-08-28 | 2004-03-11 | Albemarle Netherlands B.V. | Preparation de catalyseurs renfermant un zeolite de type pentasile |
US6887457B2 (en) | 2002-08-28 | 2005-05-03 | Akzo Nobel N.V. | Process for the preparation of catalysts comprising a pentasil-type zeolite |
WO2006035004A1 (fr) * | 2004-09-27 | 2006-04-06 | Akzo Nobel N.V. | Substrat avec couche exterieure d'argile anionique, procede de fabrication du substrat et utilisation de ce substrat |
JP2007500593A (ja) * | 2003-05-22 | 2007-01-18 | アルベマーレ ネザーランズ ビー.ブイ. | 金属含有組成物及び触媒組成物としてのそれらの使用 |
US7303654B2 (en) | 2002-11-19 | 2007-12-04 | Akzo Nobel N.V. | Cellulosic product and process for its production |
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US4454244A (en) * | 1983-03-28 | 1984-06-12 | Ashland Oil, Inc. | New compositions |
US4774212A (en) * | 1987-12-22 | 1988-09-27 | Amoco Corporation | Pillared hydrotalcites |
US5426083A (en) * | 1994-06-01 | 1995-06-20 | Amoco Corporation | Absorbent and process for removing sulfur oxides from a gaseous mixture |
WO1995021127A1 (fr) * | 1994-02-03 | 1995-08-10 | Chemson Polymer-Additive Gesellschaft Mbh | Composes basiques a reseau stratifie |
EP0725038A1 (fr) * | 1995-02-03 | 1996-08-07 | SNAMPROGETTI S.p.A. | Matériau de type hydrotalcite ayant une structure en couches et son utilisation |
WO1998003430A1 (fr) * | 1996-07-19 | 1998-01-29 | Aristech Chemical Corporation | Synthese simplifiee d'hydrotalcite a anions intercales |
WO1998051615A1 (fr) * | 1997-05-14 | 1998-11-19 | Aristech Chemical Corporation | Synthese simplifiee d'hydrotalcites a anions intercales |
WO1999041195A1 (fr) * | 1998-02-11 | 1999-08-19 | Akzo Nobel N.V. | Procede continu permettant de produire de l'argile anionique |
-
2000
- 2000-01-27 WO PCT/EP2000/000611 patent/WO2000044672A1/fr active Application Filing
Patent Citations (8)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US4454244A (en) * | 1983-03-28 | 1984-06-12 | Ashland Oil, Inc. | New compositions |
US4774212A (en) * | 1987-12-22 | 1988-09-27 | Amoco Corporation | Pillared hydrotalcites |
WO1995021127A1 (fr) * | 1994-02-03 | 1995-08-10 | Chemson Polymer-Additive Gesellschaft Mbh | Composes basiques a reseau stratifie |
US5426083A (en) * | 1994-06-01 | 1995-06-20 | Amoco Corporation | Absorbent and process for removing sulfur oxides from a gaseous mixture |
EP0725038A1 (fr) * | 1995-02-03 | 1996-08-07 | SNAMPROGETTI S.p.A. | Matériau de type hydrotalcite ayant une structure en couches et son utilisation |
WO1998003430A1 (fr) * | 1996-07-19 | 1998-01-29 | Aristech Chemical Corporation | Synthese simplifiee d'hydrotalcite a anions intercales |
WO1998051615A1 (fr) * | 1997-05-14 | 1998-11-19 | Aristech Chemical Corporation | Synthese simplifiee d'hydrotalcites a anions intercales |
WO1999041195A1 (fr) * | 1998-02-11 | 1999-08-19 | Akzo Nobel N.V. | Procede continu permettant de produire de l'argile anionique |
Cited By (16)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
WO2002064499A2 (fr) * | 2001-02-09 | 2002-08-22 | Akzo Nobel N.V. | Procede de preparation de compositions renfermant de l'argile anionique et de la boehmite |
WO2002064499A3 (fr) * | 2001-02-09 | 2002-11-07 | Akzo Nobel Nv | Procede de preparation de compositions renfermant de l'argile anionique et de la boehmite |
WO2002064504A1 (fr) | 2001-02-09 | 2002-08-22 | Akzo Nobel N.V. | Argiles anioniques dopees |
US6710004B2 (en) | 2001-02-09 | 2004-03-23 | Akzo Nobel Nv | Process for the preparation of anionic clay and boehmite-containing compositions |
KR100839313B1 (ko) * | 2001-02-09 | 2008-06-17 | 아크조 노벨 엔.브이. | 도프된 음이온성 클레이 |
US7022304B2 (en) | 2001-02-09 | 2006-04-04 | Akzo Nobel N.V. | Doped anionic clays |
KR100796101B1 (ko) * | 2001-02-09 | 2008-01-21 | 아크조 노벨 엔.브이. | 음이온 클레이와 베마이트-함유 조성물의 제조 방법 |
US7025873B2 (en) | 2002-06-25 | 2006-04-11 | Albemarle Netherlands Bv. | Use of cationic layered materials, compositions, comprising these materials, and the preparation of cationic layered materials |
WO2004000731A2 (fr) * | 2002-06-25 | 2003-12-31 | Akzo Nobel N.V. | Utilisation de materiaux cationiques en couches, compositions comprenant lesdits materiaux et preparation de materiaux cationiques en couches |
WO2004000731A3 (fr) * | 2002-06-25 | 2004-04-01 | Akzo Nobel Nv | Utilisation de materiaux cationiques en couches, compositions comprenant lesdits materiaux et preparation de materiaux cationiques en couches |
WO2004020092A1 (fr) * | 2002-08-28 | 2004-03-11 | Albemarle Netherlands B.V. | Preparation de catalyseurs renfermant un zeolite de type pentasile |
CN1320960C (zh) * | 2002-08-28 | 2007-06-13 | 阿尔伯麦尔荷兰有限公司 | 包含pentasil型沸石的催化剂的制备方法 |
US6887457B2 (en) | 2002-08-28 | 2005-05-03 | Akzo Nobel N.V. | Process for the preparation of catalysts comprising a pentasil-type zeolite |
US7303654B2 (en) | 2002-11-19 | 2007-12-04 | Akzo Nobel N.V. | Cellulosic product and process for its production |
JP2007500593A (ja) * | 2003-05-22 | 2007-01-18 | アルベマーレ ネザーランズ ビー.ブイ. | 金属含有組成物及び触媒組成物としてのそれらの使用 |
WO2006035004A1 (fr) * | 2004-09-27 | 2006-04-06 | Akzo Nobel N.V. | Substrat avec couche exterieure d'argile anionique, procede de fabrication du substrat et utilisation de ce substrat |
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