DE10257001A1 - Preparation of nanoscale pyrogenic magnesium-aluminum spinel, used e.g. as filler, carrier, catalyst, polish, gas sensor, involves using compounds, solution or dispersion - Google Patents

Preparation of nanoscale pyrogenic magnesium-aluminum spinel, used e.g. as filler, carrier, catalyst, polish, gas sensor, involves using compounds, solution or dispersion Download PDF

Info

Publication number
DE10257001A1
DE10257001A1 DE10257001A DE10257001A DE10257001A1 DE 10257001 A1 DE10257001 A1 DE 10257001A1 DE 10257001 A DE10257001 A DE 10257001A DE 10257001 A DE10257001 A DE 10257001A DE 10257001 A1 DE10257001 A1 DE 10257001A1
Authority
DE
Germany
Prior art keywords
magnesium
spinel
aluminum
compounds
aluminum spinel
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.)
Ceased
Application number
DE10257001A
Other languages
German (de)
Inventor
Michael Dr. Günther
Stipan Katusic
Andreas Dr. Gutsch
Geoffrey J. Varga
Horst Miess
Edwin Staab
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Evonik Operations GmbH
Original Assignee
Degussa GmbH
Priority date (The priority date 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 date listed.)
Filing date
Publication date
Application filed by Degussa GmbH filed Critical Degussa GmbH
Priority to DE10257001A priority Critical patent/DE10257001A1/en
Publication of DE10257001A1 publication Critical patent/DE10257001A1/en
Ceased legal-status Critical Current

Links

Classifications

    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B35/00—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
    • C04B35/622—Forming processes; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
    • C04B35/626—Preparing or treating the powders individually or as batches ; preparing or treating macroscopic reinforcing agents for ceramic products, e.g. fibres; mechanical aspects section B
    • C04B35/62605—Treating the starting powders individually or as mixtures
    • C04B35/62645—Thermal treatment of powders or mixtures thereof other than sintering
    • C04B35/62665—Flame, plasma or melting treatment
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B82—NANOTECHNOLOGY
    • B82Y—SPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
    • B82Y30/00—Nanotechnology for materials or surface science, e.g. nanocomposites
    • 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
    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B35/00—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
    • C04B35/01—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics
    • C04B35/44—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics based on aluminates
    • C04B35/443—Magnesium aluminate spinel
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
    • C01P2002/00—Crystal-structural characteristics
    • C01P2002/01—Crystal-structural characteristics depicted by a TEM-image
    • 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
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
    • C01P2004/00—Particle morphology
    • C01P2004/01—Particle morphology depicted by an image
    • C01P2004/04—Particle morphology depicted by an image obtained by TEM, STEM, STM or AFM
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
    • C01P2004/00—Particle morphology
    • C01P2004/60—Particles characterised by their size
    • C01P2004/64—Nanometer sized, i.e. from 1-100 nanometer
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
    • C01P2006/00—Physical properties of inorganic compounds
    • C01P2006/12—Surface area
    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
    • C04B2235/02—Composition of constituents of the starting material or of secondary phases of the final product
    • C04B2235/30—Constituents and secondary phases not being of a fibrous nature
    • C04B2235/32—Metal oxides, mixed metal oxides, or oxide-forming salts thereof, e.g. carbonates, nitrates, (oxy)hydroxides, chlorides
    • C04B2235/3205—Alkaline earth oxides or oxide forming salts thereof, e.g. beryllium oxide
    • C04B2235/3206—Magnesium oxides or oxide-forming salts thereof
    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
    • C04B2235/02—Composition of constituents of the starting material or of secondary phases of the final product
    • C04B2235/30—Constituents and secondary phases not being of a fibrous nature
    • C04B2235/32—Metal oxides, mixed metal oxides, or oxide-forming salts thereof, e.g. carbonates, nitrates, (oxy)hydroxides, chlorides
    • C04B2235/3217—Aluminum oxide or oxide forming salts thereof, e.g. bauxite, alpha-alumina
    • C04B2235/3222—Aluminates other than alumino-silicates, e.g. spinel (MgAl2O4)
    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
    • C04B2235/02—Composition of constituents of the starting material or of secondary phases of the final product
    • C04B2235/30—Constituents and secondary phases not being of a fibrous nature
    • C04B2235/44—Metal salt constituents or additives chosen for the nature of the anions, e.g. hydrides or acetylacetonate
    • C04B2235/443—Nitrates or nitrites
    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
    • C04B2235/02—Composition of constituents of the starting material or of secondary phases of the final product
    • C04B2235/30—Constituents and secondary phases not being of a fibrous nature
    • C04B2235/44—Metal salt constituents or additives chosen for the nature of the anions, e.g. hydrides or acetylacetonate
    • C04B2235/444—Halide containing anions, e.g. bromide, iodate, chlorite
    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
    • C04B2235/02—Composition of constituents of the starting material or of secondary phases of the final product
    • C04B2235/50—Constituents or additives of the starting mixture chosen for their shape or used because of their shape or their physical appearance
    • C04B2235/54—Particle size related information
    • C04B2235/5409—Particle size related information expressed by specific surface values
    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
    • C04B2235/70—Aspects relating to sintered or melt-casted ceramic products
    • C04B2235/80—Phases present in the sintered or melt-cast ceramic products other than the main phase

Landscapes

  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Ceramic Engineering (AREA)
  • Organic Chemistry (AREA)
  • Manufacturing & Machinery (AREA)
  • Materials Engineering (AREA)
  • Physics & Mathematics (AREA)
  • Structural Engineering (AREA)
  • Inorganic Chemistry (AREA)
  • Nanotechnology (AREA)
  • Thermal Sciences (AREA)
  • Plasma & Fusion (AREA)
  • Geology (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Composite Materials (AREA)
  • Condensed Matter Physics & Semiconductors (AREA)
  • General Physics & Mathematics (AREA)
  • Crystallography & Structural Chemistry (AREA)
  • Compounds Of Alkaline-Earth Elements, Aluminum Or Rare-Earth Metals (AREA)

Abstract

Preparation of nanoscale pyrogenic magnesium (Mg)-aluminum (Al) spinel with a Mg:Al molar ratio of 1:(0.01-20) involves using compounds, solution or dispersion. An Independent claim is also included for a spinel produced as above.

Description

Die Erfindung betrifft nanoskaliges pyrogen hergestelltes Magnesium-Aluminium-Spinell (MgAl2O4), ein Verfahren zur seiner Herstellung, sowie seine Verwendung.The invention relates to nanoscale pyrogenically produced magnesium aluminum spinel (MgAl 2 O 4 ), a process for its production and its use.

Es ist bekannt, pyrogene Oxide sowie Mischoxide durch Flammenhydrolyse von verdampfbaren Metallchloriden, beziehungsweise Metalloidchloriden, herzustellen (Ullmanns Enzyklopädie der technischen Chemie, 4. Auflage, Band 21, Seite 44 (1982)).It is known to be pyrogenic oxides as well Mixed oxides by flame hydrolysis of evaporable metal chlorides, or metalloid chlorides. (Ullmanns Encyclopedia of technical chemistry, 4th edition, volume 21, page 44 (1982)).

Es ist weiterhin bekannt, nanoskalige pyrogen hergestellte Oxide und/oder Mischoxide von Metallen und/oder Metalloiden herzustellen, indem man metallorganische und/oder metalloidorganische Stoffe, gegebenenfalls in einem Lösungsmittel gelöst, gegebenenfalls in einer Flamme, bei Temperaturen oberhalb von 200°C in die Oxide umwandelt ( EP 1 142 830 A1 ).It is also known to produce nanoscale pyrogenic oxides and / or mixed oxides of metals and / or metalloids by organometallic and / or organometallic substances, optionally dissolved in a solvent, optionally in a flame, at temperatures above 200 ° C. in the Converts oxides ( EP 1 142 830 A1 ).

Weiterhin ist es bekannt, MgAl2O4-Membrane durch Aufbringen von Suspensionen oder Solen auf poröse Träger und anschließender Sinterung herzustellen (Fraunhofer IGB, 1999).It is also known to produce MgAl 2 O 4 membranes by applying suspensions or sols to porous supports and subsequent sintering (Fraunhofer IGB, 1999).

Es besteht somit die Aufgabe, ein nanoskaliges pyrogen hergestelltes Magnesium-Aluminium-Spinell herzustellen, welches sich beispielsweise nach dem Trockenverpressen und Sintern bei niedrigen Temperaturen direkt auf einfache Weise zu flexiblen Membranen verarbeiten lässt.So there is a task to produce nanoscale fumed magnesium aluminum spinel, which occurs, for example, after dry pressing and sintering flexible at low temperatures Can process membranes.

Die nanoskaligen Spinelle sollten auch bei hohen Temperaturen einsetzbar sein. Weiterhin sollten die nanoskaligen Spinelle auf Grund einer hohen chemischen Beständigkeit, die auch in starken Säuren und Laugen gegeben ist und in Verbindung mit der nanoskaligen Struktur in anspruchsvollen Poliersystemen (beispielsweise zum Polieren von Silizium-Scheiben (CMP)) verwendbar sein.The nanoscale spinels should can also be used at high temperatures. Furthermore, the nanoscale Spinels due to their high chemical resistance, even in strong ones acids and alkalis and in connection with the nanoscale structure in sophisticated polishing systems (e.g. for polishing Silicon wafers (CMP)) can be used.

Gegenstand der Erfindung ist ein nanoskaliges, pyrogen hergestelltes Magnesium-Aluminium-Spinell mit einem Molverhältnis von Mg zu Al von 1:0,01 bis 1:20.The invention relates to a nano-scale, pyrogenic magnesium-aluminum spinel with a molar ratio from Mg to Al from 1: 0.01 to 1:20.

Unter nanoskaligem Magnesium-Aluminium-Spinell (MgAl2O4-Spinell) wird ein Spinell mit einer Teilchengröße von gleich oder kleiner 100 Nanometer verstanden.Nanoscale magnesium-aluminum spinel (MgAl 2 O 4 spinel) is understood to mean a spinel with a particle size equal to or less than 100 nanometers.

Ein weiterer Gegenstand der Erfindung ist ein Verfahren zur Herstellung des nanoskaligen pyrogen hergestellten Magnesium-Aluminium-Spinell (MgAl2O4-Spinell), welches dadurch gekennzeichnet ist, daß man Magnesium-Verbindungen und Aluminium-Verbindungen, gegebenenfalls in einem Lösungsmittel gelöst oder dispergiert, zerstäubt und in einer Flamme, vorzugsweise einer Knallgasflamme, bei Temperaturen oberhalb von 200 °C in das Magnesium-Aluminium-Spinell (MgAl2O4-Spinell) umwandelt.Another object of the invention is a method for producing the nanoscale pyrogenically produced magnesium-aluminum spinel (MgAl 2 O 4 spinel), which is characterized in that magnesium compounds and aluminum compounds, optionally dissolved or dispersed in a solvent , atomized and converted in a flame, preferably an oxyhydrogen gas flame, at temperatures above 200 ° C. into the magnesium-aluminum spinel (MgAl 2 O 4 spinel).

Das erfindungsgemäße Verfahren ist schematisch in 1 dargestellt.The method according to the invention is shown schematically in 1 shown.

Geeignete Verbindungen des Magnesiums und des Aluminiums können in flüssiger Form als sehr fein verteiltes Spray einem Hochtemperatur-Reaktionsraum zugeführt werden, wobei in dem Hochtemperatur-Reaktionsraum, der vorzugsweise als geschlossenes Strömungsrohr ausgebildet ist, bei Temperaturen oberhalb von 200°C die Partikelbildung erfolgen kann. Hierzu können Lösungen von metallorganischen und/oder metalloid-organischen Stoffen (Precursor) in organis chen Lösungsmitteln oder auch die reinen Stoffe (Precursor) , gegebenenfalls in einer Flamme, bei höheren Temperaturen, gegebenenfalls oberhalb 200 °C, zu den Oxiden umgewandelt werden.Suitable compounds of magnesium and aluminum can in liquid Form as a very finely divided spray in a high temperature reaction space supplied be in the high temperature reaction space, which is preferably as a closed flow tube is formed, the formation of particles at temperatures above 200 ° C. can be done. You can do this solutions of organometallic and / or metalloid-organic substances (precursor) in organic solvents or also the pure substances (precursor), optionally in one Flame, at higher Temperatures, optionally above 200 ° C, converted to the oxides become.

Als Precursor können Verbindungen des Typs MeR eingesetzt werden, wobei R einen organischen Rest, wie beispielsweise Methyl, Ethyl, Propyl, Butyl, oder die entsprechende Alkoxyvarianten oder auch ein Nitration beziehungsweise ein Chloridion darstellt.Compounds of the type can be used as precursors MeR are used, where R is an organic radical, such as methyl, Ethyl, propyl, butyl, or the corresponding alkoxy variants or also represents a nitrate ion or a chloride ion.

Als Lösungsmittel können organische Lösungsmittel, wie Alkohole, wie zum Beispiel Propanol, n-Butanol, iso-Propanol, und/oder Wasser eingesetzt werden.Organic Solvent, such as alcohols, such as propanol, n-butanol, isopropanol, and / or Water can be used.

Das Aluminium kann weiterhin in Form einer wässrigen Dispersion des Aluminiumoxides der Flamme zugeführt werden.The aluminum can still be in shape an aqueous Dispersion of the aluminum oxide are fed to the flame.

Der Precursor kann mit einem Druck von 1 bis 10000 bar, bevorzugt von 2 bis 100 bar zugeführt werden.The precursor can be pressed from 1 to 10000 bar, preferably from 2 to 100 bar.

Die Zerstäubung des Precursors kann mittels Ultraschallvernebler durchgeführt werden.The precursor can be atomized using Ultrasonic nebulizer performed become.

Die Temperatur kann mindestens 200 °C betragen.The temperature can be at least 200 ° C.

Bei einer Temperatur von 1800 °C bis 2400 °C können feine Teilchen erzielt werden.At a temperature of 1800 ° C to 2400 ° C fine Particles can be obtained.

Zusätzlich können dem Hochtemperatur-Reaktionsraum inerte oder reaktive Gase zugeführt werden. Die Abtrennung der Pulver kann durch bekannte Methoden der Gas-Feststofftrennung mittels Filter, Zyklon, Wäscher oder anderen geeigneten Abscheidern erfolgen.In addition, the high temperature reaction space inert or reactive gases supplied become. The powder can be separated off by known methods of Gas-solid separation using filters, cyclones, scrubbers or other suitable separators.

Ein Vorteil des erfindungsgemäßen Verfahrens ist, daß die Precursoren nicht gasförmig, sondern flüssig in die Brennkammer eingeführt werden können. Dabei kann durch mindest ens eine Einstoffdüse bei Drücken bis zu 10000 bar ein sehr feines Tropfenspray (mittlere Tropfengröße je nach Druck in der Düse zwischen < 1-500 μm) erzeugt werden, welches dann verbrennt und dabei das MgAl2O4-Spinell als Feststoff erzeugt.An advantage of the method according to the invention is that the precursors can be introduced into the combustion chamber not in gaseous form, but rather in liquid form. A very fine droplet spray (average droplet size depending on the pressure in the nozzle between <1-500 μm) can be generated by at least one single-substance nozzle at pressures up to 10000 bar, which then burns and the MgAl 2 O 4 spinel as a solid generated.

Weiterhin kann mindestens eine Zweistoffdüse bei Drücken bis zu 1 00 bar eingesetzt werden.Furthermore, at least one two-component nozzle at pressures up to at 1 00 bar.

Die Tropfenerzeugung kann durch Verwendung einer oder mehrerer Zweistoffdüsen erfolgen, wobei das bei der Zweistoffzerstäubung eingesetzte Gas reaktiv oder inert sein kann.The drop generation can be done by using one or more two-substance nozzles take place, the gas used in the two-substance atomization reactive or can be inert.

Bei Verwendung einer Zweistoffdüse ergibt sich der Vorteil, daß die Tropfen mit einem Gasstrahl erzeugt werden. Dieser Gasstrahl kann Sauerstoff oder Stickstoff enthalten.If a two-substance nozzle is used, there is the advantage that the drops with a gas jet be fathered. This gas jet can contain oxygen or nitrogen.

Dadurch kann eine sehr intensive Vermischung der Oxidationsmittel mit dem Precursor erreicht werden. Es ist auch eine zusätzliche Brennstoffzufuhr in unmittelbarer Umgebung der Tropfen möglich, falls der Precursor nicht reaktiv, beziehungsweise der Dampfdruck des Precursor nicht hoch genug ist, um eine schnelle Reaktion zu gewährleisten.This can be a very intense Mixing of the oxidizing agent can be achieved with the precursor. It is also an additional one Fuel supply possible in the immediate vicinity of the drops, if the precursor is not reactive, or the vapor pressure of the Precursor is not high enough to ensure a quick response.

Durch die Verwendung von metallorganischen Precursoren in Lösungsmitteln können homogene Lösungsmittelgemische aus verschiedenen Verbindungen der Formel MeR (Precursor) in beliebigen Konzentrationsverhältnissen ohne besonderen Aufwand hergestellt und bevorzugt in flüssiger Form einer Flamme zugeführt werden, um die entsprechenden pyrogenen Spinelle zu erhalten.Through the use of organometallic Precursors in solvents can homogeneous solvent mixtures from various compounds of the formula MeR (precursor) in any concentration ratios Manufactured without special effort and preferably in liquid form fed to a flame to obtain the corresponding pyrogenic spinels.

Mit dem erfindungsgemäßen Verfahren können Magnesium-Aluminium-Spinelle (MgAl2O4-Spinelle), die auf Grund des stark unterschiedlichen Verdampfungsverhalten der Ausgangsverbindungen schlecht, beziehungsweise nicht herstellbar waren, leicht hergestellt werden.With the method according to the invention, magnesium-aluminum spinels (MgAl 2 O 4 spinels) which, owing to the strongly different evaporation behavior of the starting compounds, were difficult to produce or could not be produced can easily be produced.

Ein weiterer Vorteil des erfindungsgemäßen Verfahrens ist, daß man dem flüssigen Precursor nicht nur andere flüssige Precursoren, sondern auch feine Partikel, wie zum Beispiel pyrogene Oxide, wie Aluminiumoxid hinzugegeben und dadurch bei der Reaktion ein Coating der in dem Precursor dispergierten Partikeln erhalten kann.Another advantage of the method according to the invention is that one the liquid Precursor not just other liquid ones Precursors, but also fine particles, such as pyrogenic Oxides, such as alumina, are added and thereby during the reaction obtain a coating of the particles dispersed in the precursor can.

Die Umsetzung der Precursor zu den Oxiden kann bevorzugt in einer Knallgasflamme erfolgen.Implementation of the precursor to the Oxides can preferably be produced in a detonating gas flame.

Als Brenngas können außer Wasserstoff weitere brennbare Gase, wie beispielsweise Methan, Propan, Ethan, eingesetzt werden.In addition to hydrogen, other combustible can be used as fuel gas Gases such as methane, propane, ethane can be used.

Metallorganische Precursoren stellen allein betrachtet einen guten Brennstoff dar. Daher ist ein weiterer Vorteil des erfindungsgemäßen Verfahrens darin begründet, daß man gegebenenfalls auf eine Stützflamme gänzlich verzichten und somit beispielsweise Wasserstoff als teueren Rohstoff einsparen kann.Organometallic precursors considered alone is a good fuel. Therefore, another one Advantage of the method according to the invention based on that he if necessary, do without a support flame altogether and thus save hydrogen as an expensive raw material, for example can.

Durch die Variation der Luftmenge (für die Verbrennung) und/oder durch die Variation der Düsenparameter ist eine Einflussnahme auf die Oxideigenschaften, beispielweise auf die BET-Oberfläche, möglich.By varying the amount of air (for the Combustion) and / or by varying the nozzle parameters is an influence on the oxide properties, for example on the BET surface.

Das erfindungsgemäße pyrogen hergestellte Magnesium-Aluminium-Spinell (MgAl2O4-Spinell) kann als Füllstoff, als Trägermaterial, als katalytisch aktive Substanz, als Ausgangsmaterial zur Herstellung von Dispersionen, als Poliermaterial zum Polieren von Metall-, beziehungsweise Siliziumscheiben in der Elektronikindustrie (CMP-Anwendung), als keramischer Grundstoff für Gassensoren, in Brennstoffzellen, als Dentalwerkstoff, zur Herstellung von Membranen, in der Kosmetikindustrie, als Additiv in der Silikon- und Kautschukindustrie, zur Einstellung der Rheologie von flüssigen Systemen, zur Hitzeschutzstabilisierung, in der Lackindustrie, als Farbpigment, als Wärmedämmmaterial, als Antiblockdingmittel verwendet werden.The pyrogenically produced magnesium aluminum spinel (MgAl 2 O 4 spinel) can be used as a filler, as a carrier material, as a catalytically active substance, as a starting material for the production of dispersions, as a polishing material for polishing metal or silicon wafers in the electronics industry ( CMP application), as a ceramic base material for gas sensors, in fuel cells, as a dental material, for the manufacture of membranes, in the cosmetics industry, as an additive in the silicone and rubber industry, for adjusting the rheology of liquid systems, for heat protection stabilization, in the paint industry, as a pigment, as a thermal insulation material, as an anti-blocking agent.

BeispieleExamples

Als Magnesium-Precursoren werden Mg (NO3)2 oder MgCl2 und als Aluminium-Precursoren Al(NO3)3, AlCl3 oder Aluminiumoxid in einer Wasserstofflamme entsprechend dem Verfahren wie in EP 1 142 8 3 0 A1 beschrieben umgesetzt.Mg (NO 3 ) 2 or MgCl 2 are used as magnesium precursors and Al (NO 3 ) 3 , AlCl 3 or aluminum oxide as aluminum precursors in a hydrogen flame according to the method as in EP 1 142 8 3 0 A1 described implemented.

Die erfindungsgemäß verwendbare Brenneranordnung ist in 2 schematisch dargestellt.The burner arrangement which can be used according to the invention is shown in 2 shown schematically.

Die Lösungen mit den Mg-Precursoren und Al-Precursoren gemäß Tabelle 1 werden unter Stickstoffdruck mit Hilfe der Düse in das Reaktionsrohr verstäubt. Hier brennt eine Knallgasflamme aus Wasserstoff und Luft. Die Temperatur 0,5 m unterhalb der Flamme beträgt 500 bis 1000 °C. Das erhaltene MgAl2O4-Spinell wird in Filtern abgeschieden.The solutions with the Mg precursors and Al precursors according to Table 1 are atomized into the reaction tube under nitrogen pressure using the nozzle. A detonating gas flame made of hydrogen and air burns here. The temperature 0.5 m below the flame is 500 to 1000 ° C. The MgAl 2 O 4 spinel obtained is separated off in filters.

Die erhaltenen Produkte weisen die in der Tabelle 2 aufgeführten Daten auf.The products obtained have the listed in Table 2 Dates on.

Tabelle 1

Figure 00060001
Table 1
Figure 00060001

Tabelle 2

Figure 00070001
Table 2
Figure 00070001

Eine weitere Charakterisierung der erfindungsgemäßen Magnesium-Aluminium-Spinelle ist den Figuren zu entnehmen:
Gemäß 3 zeigt die TEM-Aufnahme die Feinteiligkeit der Partikel.A further characterization of the magnesium-aluminum spinels according to the invention can be seen in the figures:
According to 3 the TEM image shows the fine particle size of the particles.

Gemäß 4 zeigt die hochauflösende TEM-Aufnahme anhand der Gitterebenen das Vorliegen der Spinell-Struktur.According to 4 shows the high-resolution TEM image based on the lattice planes the presence of the spinel structure.

Gemäß den 5 bis 7 kann die Spinell-Struktur ebenfalls den XRD-Diagrammen entnommen werden.According to the 5 to 7 the spinel structure can also be seen in the XRD diagrams.

Gemäß 8 lassen sich die Zetapotenzialkurven der Spinelle durch die Zusammensetzung beeinflussen, wie ein Vergleich der Beispiele 1, 2 und 7 zeigt.According to 8th the zeta potential curves of the spinels can be influenced by the composition, as a comparison of Examples 1, 2 and 7 shows.

Die Zetapotenziale der erfindungsgemäßen Magnesium-Aluminium-Spinelle unterscheiden sich deutlich von der Kurve die reinem Aluminiumoxid zuzuordnen ist.The zeta potentials of the magnesium-aluminum spinels according to the invention the pure aluminum oxide differ significantly from the curve is to be assigned.

Claims (3)

Nanoskaliges, pyrogen hergestelltes Magnesium-Aluminium-Spinell mit einem Molverhältnis von Mg zu Al von 1:0,01 bis 1:20.Nanoscale, fumed magnesium-aluminum spinel with one molar ratio from Mg to Al from 1: 0.01 to 1:20. Verfahren zur Herstellung des nanoskaligen, pyrogen hergestellten Magnesium-Aluminium-Spinells gemäß Anspruch 1, dadurch gekennzeichnet, daß man Magnesium-Verbindungen und Aluminium-Verbindungen, gegebenenfalls in einem Lösungsmittel gelöst oder dispergiert, zerstäubt und in einer Flamme bei Temperaturen oberhalb von 200 °C in Magnesium-Aluminium-Spinell (MgAl2O4-Spinell) umwandelt.Process for the preparation of the nanoscale, pyrogenically produced magnesium-aluminum spinel according to claim 1, characterized in that magnesium compounds and aluminum compounds, optionally dissolved or dispersed in a solvent, atomized and in a flame at temperatures above 200 ° C converted into magnesium aluminum spinel (MgAl 2 O 4 spinel). Verwendung des Magnesium-Aluminium-Spinells gemäß Anspruch 1 als Füllstoff, als Trägermaterial, als katalytisch aktive Substanz, als Ausgangsmaterial zur Herstellung von Dispersionen, als Poliermaterial zum Polieren von Metall-, beziehungsweise Siliziumscheiben in der Elektronikindustrie (CMP-Anwendung), als keramischer Grundstoff für Gassensoren, in Brennstoffzellen, als Dentalwerkstoff, zur Herstellung von Membranen, in der Kosmetikindustrie, als Additiv in der Silikon- und Kautschukindustrie, zur Einstellung der Rheologie von flüssigem Systemen, zur Hitzeschutzstabilisierung, in der Lackindustrie, als Farbpigment, als Wärmedämmmaterial, als Antiblocking-Mittel.Use of the magnesium-aluminum spinel according to claim 1 as filler, as carrier material, as catalytically active substance, as a starting material for production of dispersions, as a polishing material for polishing metal, respectively Silicon wafers in the electronics industry (CMP application), as ceramic Basic material for Gas sensors, in fuel cells, as a dental material, for manufacturing of membranes, in the cosmetics industry, as an additive in silicone and rubber industry, to adjust the rheology of liquid systems, for heat protection stabilization, in the paint industry, as a color pigment, as thermal insulation material, as an anti-blocking agent.
DE10257001A 2002-12-06 2002-12-06 Preparation of nanoscale pyrogenic magnesium-aluminum spinel, used e.g. as filler, carrier, catalyst, polish, gas sensor, involves using compounds, solution or dispersion Ceased DE10257001A1 (en)

Priority Applications (1)

Application Number Priority Date Filing Date Title
DE10257001A DE10257001A1 (en) 2002-12-06 2002-12-06 Preparation of nanoscale pyrogenic magnesium-aluminum spinel, used e.g. as filler, carrier, catalyst, polish, gas sensor, involves using compounds, solution or dispersion

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
DE10257001A DE10257001A1 (en) 2002-12-06 2002-12-06 Preparation of nanoscale pyrogenic magnesium-aluminum spinel, used e.g. as filler, carrier, catalyst, polish, gas sensor, involves using compounds, solution or dispersion

Publications (1)

Publication Number Publication Date
DE10257001A1 true DE10257001A1 (en) 2004-06-24

Family

ID=32336035

Family Applications (1)

Application Number Title Priority Date Filing Date
DE10257001A Ceased DE10257001A1 (en) 2002-12-06 2002-12-06 Preparation of nanoscale pyrogenic magnesium-aluminum spinel, used e.g. as filler, carrier, catalyst, polish, gas sensor, involves using compounds, solution or dispersion

Country Status (1)

Country Link
DE (1) DE10257001A1 (en)

Cited By (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE102006032582A1 (en) * 2006-07-13 2008-01-24 Clariant International Limited Process for the production of nanoparticles from aluminum spinels and their use
CN103934759A (en) * 2013-01-19 2014-07-23 河南工业大学 Novel glass polishing plate and manufacturing method thereof
WO2015140459A1 (en) * 2014-03-18 2015-09-24 Saint-Gobain Centre De Recherches Et D'etudes Europeen Fused grains of magnesium-rich magnesium aluminate
CN103934759B (en) * 2013-01-19 2016-11-30 河南工业大学 Glass polishing disk and manufacture method thereof
FR3040993A1 (en) * 2015-09-14 2017-03-17 Saint-Gobain Centre De Rech Et D'Etudes Europeen MAGNESIUM RICH MAGNESIUM ALUMINATE FUSED GRAIN
US10072195B2 (en) 2014-03-14 2018-09-11 Dainichiseika Color & Chemicals Mfg. Co., Ltd. Thermally conductive complex oxide, production method therefor, thermally conductive complex oxide-containing composition, and use therefor

Citations (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP1142830A1 (en) * 2000-04-03 2001-10-10 Degussa AG Nano-sized pyrogenic oxides, process for their preparation and their use

Patent Citations (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP1142830A1 (en) * 2000-04-03 2001-10-10 Degussa AG Nano-sized pyrogenic oxides, process for their preparation and their use

Cited By (11)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE102006032582A1 (en) * 2006-07-13 2008-01-24 Clariant International Limited Process for the production of nanoparticles from aluminum spinels and their use
CN103934759A (en) * 2013-01-19 2014-07-23 河南工业大学 Novel glass polishing plate and manufacturing method thereof
CN103934759B (en) * 2013-01-19 2016-11-30 河南工业大学 Glass polishing disk and manufacture method thereof
US10072195B2 (en) 2014-03-14 2018-09-11 Dainichiseika Color & Chemicals Mfg. Co., Ltd. Thermally conductive complex oxide, production method therefor, thermally conductive complex oxide-containing composition, and use therefor
EP3118160B1 (en) * 2014-03-14 2019-05-08 Dainichiseika Color & Chemicals Mfg. Co., Ltd. Thermally conductive complex oxide, production method therefor, thermally conductive complex oxide-containing composition, and use therefor
WO2015140459A1 (en) * 2014-03-18 2015-09-24 Saint-Gobain Centre De Recherches Et D'etudes Europeen Fused grains of magnesium-rich magnesium aluminate
FR3018804A1 (en) * 2014-03-18 2015-09-25 Saint Gobain Ct Recherches FADE GRAINS OF MAGNESIUM ALUMINATE RICH IN MAGNESIUM.
US9845266B2 (en) 2014-03-18 2017-12-19 Saint-Gobain Centre De Recherches Et D'etudes Europeen Fused grains of magnesium-rich magnesium aluminate
FR3040993A1 (en) * 2015-09-14 2017-03-17 Saint-Gobain Centre De Rech Et D'Etudes Europeen MAGNESIUM RICH MAGNESIUM ALUMINATE FUSED GRAIN
WO2017046517A1 (en) * 2015-09-14 2017-03-23 Saint-Gobain Centre De Recherches Et D'etudes Europeen Melted magnesium aluminate grain rich in magnesium
US10494308B2 (en) 2015-09-14 2019-12-03 Saint-Gobain Centre De Recherches Et D'etudes European Melted magnesium aluminate grain rich in magnesium

Similar Documents

Publication Publication Date Title
EP1142830A1 (en) Nano-sized pyrogenic oxides, process for their preparation and their use
EP1688394B1 (en) Method for making metal oxides
US20010036437A1 (en) Nanoscale pyrogenic oxides
EP1997776B1 (en) Pyrogenetically produced silicon dioxide with low thickening effect
EP0995718B1 (en) Alumina doped silica prepared pyrogenically using an aerosol
US7749322B2 (en) Aluminium oxide powder produced by flame hydrolysis and having a large surface area
EP1785395B1 (en) Process for the preparation of doped metal oxide particles
EP3408227B1 (en) Method for producing tungsten oxide and mixed tungsten oxides
DE10312970A1 (en) Fumed silica powder and dispersion thereof
DE102006027302A1 (en) Process for the preparation of mixed oxide powders
DE102006027334A1 (en) Process for the preparation of metal oxide powders
DE102006027335A1 (en) Process for the preparation of mixed metal oxide powders
JPH11349849A (en) Oxidation post-treated carbon black
DE10212680A1 (en) Nanoscale zinc oxide, process for its production and use
WO2008006565A1 (en) Method for the production of nanocrystalline metal oxide
DE10258857A1 (en) Fumed silica and dispersion thereof
EP1270511B9 (en) Indium-Tin-Oxides
EP3112319A1 (en) Method for the preparation of metal oxide powders using flame spray pyrolysis
US7465431B2 (en) Nanoscalar pyrogenically produced yttrium-zirconium mixed oxide
DE10257001A1 (en) Preparation of nanoscale pyrogenic magnesium-aluminum spinel, used e.g. as filler, carrier, catalyst, polish, gas sensor, involves using compounds, solution or dispersion
DE102004039139A1 (en) Yttrium-zirconium mixed oxide powder
DE10138573A1 (en) Nanoscale pyrogenic yttrium-zirconium mixed oxide
DE10258858A1 (en) Fumed silica
EP1216956B1 (en) Potassium doped pyrogenic oxide
DE10317067A1 (en) Domains in a metal oxide matrix

Legal Events

Date Code Title Description
OP8 Request for examination as to paragraph 44 patent law
8131 Rejection