Method of manufacturing metal oxide and / or metalloid oxide

Abstract

The invention relates to a flame hydrolysis process for producing metal and / or metalloid oxides by means of a burner having a burner head with at least two gas channels and an outlet end, wherein the metal or metalloid oxide is selected from the group consisting of oxides of aluminum (Al), titanium (Ti), zirconium (Zr), yttrium (Y), lithium (Li), magnesium (Mg), lanthanum (La), cerium (Ce), iron (Fe), zinc (Zn) and silicon (Si) or mixtures thereof, the process comprising the steps of providing an oxygen-containing gas, a fuel gas and a gaseous metal precursor and / or a mixture containing a gaseous metal precursor to the burner head, providing a flame by combusting at least a portion of the oxygen-containing gas and the fuel gas at the outlet end of the burner head, releasing the MP and / or the MP-containing mixture into the provided flame, and providing gaseous ammonia (NH3) and / or a gaseous mixture containing ammonia (NH3) in at least one gas channel to the outlet end of the burner head and releasing the gaseous ammonia into the flame, and wherein ammonia (NH3) is not pre-mixed with the metal precursor before the outlet end of the burner head.

Description

Technical Field

[0001] This invention provides a method for synthesizing pyrolytic metal oxide powder and pyrolytic quasi-metal oxide powder, and their uses in various applications. Background Technology

[0002] Flame hydrolysis processes, such as the Aerosil® process, are well-known methods for producing vapor-phase (pyrolytic) metals and quasi-metal oxides such as SiO2, Al2O3, TiO2, etc.

[0003] This method involves the intense exothermic combustion of hydrogen feedstock to produce water (H2 + 0.5O2). H2O) and the simultaneous hydrolysis of metal precursors, such as SiCl4 or AlCl3, using the water obtained therefrom. Taking SiCl4 as an example, the overall process (1) is exothermic:

[0004] SiCl4 + 2H2 + O2 SiO2 + 4HCl -102 kJ / mol (SiCl4) (1)

[0005] The production of metal oxides with relatively high BET surface areas typically requires reducing the flame temperature. This is usually achieved through measures or combinations thereof: (a) using a hydrogen feedstock in a minimum amount relative to the reaction stoichiometry and / or (b) using additional air or steam to “dilute” and cool the flame. The method using a minimum amount of hydrogen feedstock is described, for example, in US 2014 / 0030525 A1. This method produces BET surface areas of 400 to 600 m². 2 A method for producing / g of silica powder includes: igniting a gas mixture comprising an oxidizable and / or hydrolyzable silicon compound, hydrogen, and an oxygen-containing first gas in a burner, and burning the resulting flame into a reaction chamber, introducing an oxygen-containing second gas into the reaction chamber, and separating the resulting solid material from the gaseous material, wherein the quotient formed in the burner by the amount of hydrogen supplied and the amount of hydrogen required for stoichiometry is 0.70 to 1.30.

[0006] According to EP 0015315 A1, the use of additional air and a minimum amount of additional water vapor in flame hydrolysis processes is described as beneficial for higher BET surface area and particle size.

[0007] However, using a more diluted feed stream, such as additional air or additional steam, typically leads to an unavoidable reduction in production capacity and higher production costs. Therefore, reducing the flame temperature without adding a diluted feed stream would be beneficial. Summary of the Invention

[0008] The object of this invention is to provide a method for producing metal and / or quasi-metal oxides with relatively high BET surface area under high throughput of the production apparatus and improved mechanical and / or chemical stability of the metal and / or quasi-metal oxides.

[0009] These requirements can be addressed by a method for producing metal oxides and / or quasi-metal oxides using a burner having a burner head with at least two (internal) channels and an outlet end, wherein the metal oxide or quasi-metal oxide is selected from oxides of aluminum (Al), titanium (Ti), zirconium (Zr), yttrium (Y), lithium (Li), magnesium (Mg), lanthanum (La), cerium (Ce), iron (Fe), zinc (Zn), and silicon (Si), including mixtures thereof.

[0010] The method includes the following steps:

[0011] - Supply oxygen-containing gas and fuel gas to the burner head

[0012] - Provide gaseous metal precursors and / or gaseous quasi-metal precursors (MP) to the burner head;

[0013] - A flame is provided by burning at least a portion of the oxygen-containing gas and the fuel gas at the outlet end of the burner head;

[0014] - Release the MP into the provided flame, and

[0015] - Gaseous ammonia (NH3) is supplied to the outlet end of the burner head via the at least one channel and the ammonia (NH3) is released into the flame, wherein the ammonia (NH3) is not premixed with the MP before the outlet end of the burner head.

[0016] Oxygen-containing gas, fuel gas, and gaseous MP are supplied to the outlet end of the burner head via at least one (internal) gas passage. At least two of the four different gases used in this method can be premixed and supplied to the outlet end of the burner head via a common gas passage. However, gaseous ammonia (NH3) must be guided to the outlet end of the burner head via at least one separate gas passage without contact with or premixing with MP, and released directly into the flame. The term "separate gas passage" refers to the separation of ammonia and MP before combustion and / or the flame chamber. While not wishing to be bound by any theory, it is believed that if ammonia is premixed with MP, it may react prematurely with metallic and / or quasi-metallic precursors, leading to blockage of the gas passage in the burner head.

[0017] In the context of this invention, the term "MP" refers to the corresponding substance, i.e., a metal precursor and / or a quasi-metal precursor, and a mixture containing a metal precursor and / or a quasi-metal precursor, which exists in a gaseous form (e.g., gas, vapor, or the like) at least at the outlet end of the burner head under reaction conditions.

[0018] In the context of this invention, "ammonia" refers to a gaseous substance, existing in a gaseous form (e.g., gas or vapor), at least at the outlet end of the burner head, under reaction conditions, as well as a mixture containing ammonia (NH3).

[0019] Overall, it was surprisingly found that using ammonia to at least partially replace typical fuel gases, such as hydrogen, in flame hydrolysis resulted in a significant reduction in flame temperature and the production of gases with a temperature of at least 300 m. 2 Metal oxides and quasi-metal oxides with a high BET surface area per g.

[0020] I do not wish to be bound by any theory, but I believe that the beneficial results of the method of the present invention can be explained by the overall endothermic process (2) of flame hydrolysis of metal precursors compared with the exothermic reaction (1) using hydrogen:

[0021] SiCl4 + 2H2 + O2 SiO2 + 4HCl -102 kJ / mol (SiCl4) (1)

[0022] SiCl4 + 4 / 3NH3 + O2 SiO2 + 4HCl + 2N2 + 48 kJ / mol (SiCl4) (2)

[0023] The feedstock ammonia (NH3) can preferably be used as a mixture with fuel gas, oxygen-containing gas, vaporized water (H2O), and / or N2. One benefit of adding water vapor or N2 gas to the feedstock NH3 is that it can enhance the control of the flame temperature when needed.

[0024] The term "raw material" refers to at least one substance, reactant, and / or mixture thereof supplied to the burner and / or burner head that is not formed, at least temporarily, during or by the flame process.

[0025] According to a preferred embodiment of the method, the metal oxide or quasi-metal oxide is selected from the group consisting of aluminum oxide (Al2O3), titanium dioxide (TiO2), and / or silicon dioxide (SiO2) and mixtures thereof. Most preferably, the metal oxide or quasi-metal oxide is silicon dioxide (SiO2), or a mixture of metals and / or quasi-metal oxides containing silicon dioxide (SiO2).

[0026] According to a further preferred embodiment of the method, the amounts of oxygen and fuel gas are adjusted to approximately 1 to 3, preferably 1.2 to 2.5. (ratio ) and approximately 1 to 5, preferably 1.1 to 3 (ratio ).

[0027] in, (ratio ) is defined as the ratio of the amount of hydrogen supplied to the burner head to the stoichiometric amount of hydrogen required for the hydrolysis reaction of MP; and (ratio In this paper, is defined as the ratio of the amount of oxygen supplied to the burner head to the stoichiometric amount of hydrogen required for the combustion of all fuels (gases).

[0028] It has been surprisingly found that NH3 must be released directly into the flame at the outlet end of the burner head and any premixing of ammonia with MP must be avoided, as MP such as SiCl4 may react with ammonia prematurely and cause undesirable reactor blockage.

[0029] The main benefit of the method of the present invention is the reduction in the demand for flame cooling gases such as air or water vapor, which in turn leads to increased device throughput and / or more economical synthesis of metal and metal quasi-metal oxides, especially metal and metal quasi-metal oxides with higher BET surface areas.

[0030] The burner head, as part of the burner, can be at least partially mounted and positioned inside the burner housing. The burner may further include a combustion chamber, also called a flame chamber, into which the flame ignited at the outlet end of the burner head extends. The housing is typically connected to an outlet (line) or a product line. This product line and / or burner housing may contain a flame tube. Preferably, the flame tube forms the outlet portion of the flame chamber, which is part of the housing, and / or the first section of the product line. According to an advantageous solution, the flame tube is connected to a (subsequent) cooling line, whereby the cooling line may also be a section of the product line and / or form a cooling unit connectable to the product line.

[0031] In the context of this invention, the term "outlet end" refers to the outer portion of the burner head, that is, the respective outlet end of the corresponding gas passage of the burner head, where the gas leaves the corresponding passage of the burner head and forms a flame.

[0032] Gaseous MP can be obtained by evaporation of MP in liquid or solid form, wherein evaporation occurs in a suitable evaporation unit prior to the burner and / or burner head. The evaporated MP feedstock can be premixed with oxygen-containing gas, nitrogen (N2), and / or gaseous fuel gas before being fed into the flame for reaction.

[0033] The term "oxygen-containing gas" preferably refers to air, oxygen (O2), or O2-rich air. In the context of this invention, "fuel gas" can be hydrogen (H2) or a mixture of hydrogen-containing gases, carbon monoxide (CO), and / or an organic compound having at least one hydrogen and at least one carbon atom, wherein the organic compound can preferably be a hydrocarbon or an alcohol, or a mixture thereof. Hydrocarbons can be of the general formula C n H 2n+2 The alkane, wherein "n" is preferably an integer from 1 to 6, and most preferably an integer from 1 to 4. The alcohol may be a primary alcohol, a secondary alcohol, and / or a tertiary alcohol. Most preferably, the fuel gas is hydrogen or a mixture of hydrogen-containing gases. These "fuel gases" mentioned above can be understood as examples of "primary fuel gases" used for overall exothermic combustion and MP hydrolysis / pyrolysis in flame processes (see equation (1) above).

[0034] Alternatively, a mixture of other gases, such as inert gases, such as, but not limited to, N2, CO2 and / or oxygen-containing gases, can be used as a "fuel gas".

[0035] Gaseous ammonia can serve as an “auxiliary fuel gas”, which burns with the total endothermic properties of combustion and MP hydrolysis / pyrolysis (see equation (2) above).

[0036] The term "gaseous" refers to any non-solid and non-liquid form of the corresponding substance, such as, but not limited to, gas or vapor. Furthermore, "gaseous" as a non-liquid form should exclude droplets, aerosols, or any liquid spray. According to one aspect of the method of the invention, gaseous ammonia (NH3) or a gaseous mixture containing ammonia (NH3) is guided to the outlet end of the burner head via at least one gas passage. To optimize flame control and expand the range of possible outlet gas velocities of ammonia, the gaseous ammonia mixture may include oxygen-containing gas and / or gaseous fuel gas. For example, but not limited to, gaseous H2 or gaseous alkanes (C... n H 2n+2 ).

[0037] According to a preferred embodiment of the method for limiting the complexity of the burner head, it may be advantageous to include a step of (pre)mixing at least a portion of the fuel gas with ammonia and optionally with an oxygen-containing gas before the outlet end of the burner head. Preferably, the method includes a step of mixing at least a portion of the fuel gas with ammonia and an oxygen-containing gas before the outlet end of the burner head.

[0038] Similarly, it may be advantageous to (pre) mix at least a portion of the fuel gas with MP and optionally with an oxygen-containing gas before the outlet end of the burner head. Preferably, the method includes the step of mixing at least a portion of the fuel gas (other than ammonia) with MP and an oxygen-containing gas before the outlet end of the burner head. Thus, the burner head may be in fluid communication with or contain a (second) mixing chamber having at least a fuel gas inlet, an MP inlet, and an outlet leading to one of the burner head and the passage. However, this mixing chamber for mixing MP is then not in fluid communication with the ammonia (NH3) guide passage.

[0039] According to a further preferred embodiment of the method, it may be advantageous for the fuel gas to contain hydrogen (H2), carbon monoxide (CO), alcohols, and / or have the general formula C n H 2n+2 At least one of the alkanes.

[0040] In alkanes (C n H 2n+2 When the fuel is a gaseous fuel, "n" is preferably an integer from 1 to 6, and most preferably from 1 to 4. The alcohol contained in the fuel and / or forming the fuel gas is preferably selected from primary alcohols, secondary alcohols, and tertiary alcohols.

[0041] According to a further preferred embodiment of the method, it may be advantageous to use an MP mixture containing at least one gaseous fuel gas and / or an oxygen-containing gas. The gaseous fuel gas, other than ammonia, can be selected from hydrogen (H2) and gases having the general formula C2. n H 2n+2 Alkanes, alcohols, carbon monoxide (CO), and mixtures thereof.

[0042] According to a further preferred embodiment of the method, it may be advantageous to supply hydrogen (H2) and ammonia (NH3) as feedstock at a molar ratio R1 in the range of 0.05 to 1.0, preferably 0.1 to 0.9, more preferably 0.2 to 0.8, wherein the molar ratio R1 is defined as the ratio of the amount of ammonia (NH3) to the total amount of ammonia and hydrogen (NH3 + H2). At molar ratios R1 below 0.05-0.2, the introduction of ammonia has the least positive effect on the method. Hydrogen may not be used in this method (R1 = 1.0). However, it has been found that relatively low amounts of hydrogen (R1~0.8) may result in some improvement in flame stability in this method.

[0043] According to a further preferred embodiment of the method, it may be advantageous that the molar ratio R2 of the total amount of all gaseous feedstock to the amount of MP is less than 8.3. Therefore, the term "gaseous feedstock" refers to feedstock expressed in Nm³. 3The total amount or sum of gas supplied to the burner head, calculated per hour. Preferably, R2 is less than 8.0, more preferably less than 7.8, and even more preferably 4 to 7.8. Maintaining R2 at a relatively low level (R2 < 8.3) implies a higher throughput of the device, while the lower range of R2 to 4 generally represents the technically feasible minimum value of R2. Preferably, the gaseous feedstock is, for example, but not limited to, H2, NH3, O2, N2, and MP.

[0044] Gaseous N2 is typically supplied to the burner head as part of the feed gas air and / or as a separate feed gas.

[0045] According to a further preferred embodiment of the method, it may be advantageous that MP is selected from at least one of the following substances: aluminum chloride (AlCl3), aluminum oxychloride (AlOCl), titanium tetrachloride (TiCl4), titanium trichloride (TiCl3), titanium oxychloride (TiOCl2), tetraalkoxytitanates such as tetraethoxytitanate Ti(OC2H5)4, tetraalkoxysilicates such as tetraethoxysilicate Si(OC2H5)4, cyclic siloxanes ([O-SiR2)). n Examples include octamethylcyclotetrasiloxane (D4) and acyclic siloxanes (R3Si-[O-SiR2)). n -O-SiR3) such as silicone oil, silicon tetrachloride (SiCl4), trichlorosilane (HSiCl3), methyltrichlorosilane (CH3Cl3Si), dichlorosilane (SiH2Cl2) and / or monochlorosilane (SiH3Cl).

[0046] The MPs mentioned are the preferred MPs, but the method is not limited to these MPs.

[0047] According to a further preferred embodiment of the method, particularly in terms of sustainability, it may be advantageous to use at least part of the hydrogen (H2) obtained from the electrolysis of water or aqueous solution, preferably using renewable energy sources such as solar, wind, geothermal, hydropower from flowing water, tidal, energy obtained from the combustion of biomass, waste or biofuels, and combinations of these energy sources to produce the feedstock ammonia (NH3).

[0048] When supplied to the burner and / or burner head, the feedstock ammonia (NH3) is preferably gaseous and / or vaporized.

[0049] According to a further preferred embodiment of the method, the metal oxide and / or quasi-metal oxide has a thickness of 10 to 600 μm. 2 / g, more preferably 15 to 600 m² / g, more preferably 20 to 600 m² / g, more preferably 30 to 550 m² / g, more preferably 50 to 500 m² / g, and most preferably 80 to 400 m² / g BET surface area.

[0050] According to a further particularly preferred embodiment of the method, the metal oxide and / or quasi-metal oxide has a thickness of 150 to 500 μm. 2 The BET surface area is 240 to 300 m² / g, more preferably 240 to 400 m² / g, and most preferably 240 to 300 m² / g.

[0051] The method of the present invention can obtain metal oxides and / or quasi-metal oxides with some unique properties, such as, but not limited to, an increased nitrogen content in the resulting metal oxides and / or quasi-metal oxides compared with products obtained by conventional methods.

[0052] According to a further preferred embodiment of the method, the burner head includes at least two central channels radially, and a concentric (auxiliary) channel surrounds these central channels, wherein the (first) central channel is concentrically surrounded by the second (central) channel, and wherein the central channels form a tube-in-tube system. The auxiliary channel is radially outside the (central) outer channel, and at least one feed line leads into the auxiliary channel. During the process of this method, auxiliary air can be guided into the auxiliary channel and subsequently into the flame chamber. Thus, the burner includes an auxiliary channel located between the outer channel and the casing. According to another preferred embodiment, the auxiliary channel is formed by the flame chamber itself, which at least partially surrounds the central channels, and auxiliary air or (auxiliary) oxygen-containing gas is directly supplied to the flame chamber.

[0053] The burner head preferably includes two (central) channels, wherein ammonia (NH3) and hydrogen (H2) as a fuel gas mixture are preferably guided directly into the pyrolysis flame via a radially outer (central) channel, wherein the fuel gas guided via the outer (central) channel may contain hydrogen (H2) and / or additional gases, such as, but not limited to, nitrogen (N2), N2-containing gases, and / or oxygen-containing gases (O2). The MP or MP-gas mixture is guided into the flame via an inner (central) channel. As an alternative and reversed embodiment, the fuel gas including ammonia is guided into the flame via a first (central) channel, and the MP is guided via an outer (central) channel.

[0054] This arrangement, in which the inner (central) channel is directly and most closely adjacent, results in the direct release of ammonia into the flame and the beneficial high BET surface of the metal oxides and / or quasi-metal oxides, as well as a high nitrogen content, which is only associated with metal and / or quasi-metal nitrides, such as silicon nitride (Si3N4), aluminum nitride (AlN), titanium nitride (TiN and / or Ti3N4).

[0055] The present invention further comprises pyrolytic metal oxides and / or quasi-metal oxides selected from oxides of aluminum (Al), titanium (Ti), zirconium (Zr), yttrium (Y), lithium (Li), magnesium (Mg), lanthanum (La), cerium (Ce), iron (Fe), zinc (Zn), and silicon (Si), or mixtures thereof, wherein the metal oxides and / or the quasi-metal oxides have a BET surface area of ​​10 to 600 m². 2 / g and nitrogen content in weight % (wt%) and in m 2 The ratio R3 of the BET surface area per g is at least 1.0. 10 -4 weight% g / m 2 Preferably, R3 is at least 1.1. 10 -4 weight% g / m 2 More preferably at least 1.2 10 -4 weight% g / m 2 More preferably at least 1.3 10 -4 weight% g / m 2 More preferably at least 1.5 10 -4 weight% g / m 2 More preferably at least 1.7 10 -4 weight% g / m 2 More preferably at least 1.9 10 -4 weight% g / m 2 More preferably at least 2.0 10 -4 weight% g / m 2 More preferably at least 2.5 10 -4 weight% g / m 2 More preferably at least 3.0 10 -4 weight% g / m 2 The optimal value is at least 4.0. 10 -4 weight% g / m 2 The nitrogen content is only related to the nitrides of metals and / or metalloids.

[0056] The term "nitrogen content associated with nitrides of metals and / or metalloids" (N) 氮化物 In the context of this invention, N is defined as: 氮化物 = N 总量 – N (非氮化物) ,

[0057] in:

[0058] -“N 总量 "" refers to the total nitrogen (N) content in metals and / or metalloid oxides, expressed as a percentage by weight (wt%), preferably determined by elemental analysis according to EN ISO 3262-20:2000 (Chapter 8).

[0059] -“N 非氮化物 "N" refers to the nitrogen content, expressed as a percentage by weight, of all non-nitrogen compounds, including but not limited to ammonia, amines, ammonium salts, nitro compounds, and / or nitroso compounds. 非氮化物 It is preferable to calculate using the chemical formula of the nitrogen compound of the corresponding non-nitride and the carbon, hydrogen and / or oxygen content of the metal and / or quasi-metal oxides determined by elemental analysis.

[0060] Therefore, if the aforementioned non-nitride components such as ammonia or amines are not used or formed in this method, then N 氮化物 equals N 总量 (N) 氮化物 = N 总量 If non-nitride nitrogen compounds such as ammonia are present in metal and / or quasi-metal oxides, then the non-nitride nitrogen (“N”) associated with ammonia is... 非氮化物 ) content (N NH3 The hydrogen content of the oxide can be calculated from the hydrogen content determined by elemental analysis. The method according to the invention typically involves the complete combustion of all oxidizable nitrogen components (such as ammonia and amines), and therefore, no ammonia, amine, or ammonium salts are typically detected in the resulting metal and / or quasi-metal oxides. Furthermore, nitroso compounds and / or nitro compounds are typically not added or formed by this method. Therefore, in the method of the invention, N is typically... 氮化物 =N 总量 .

[0061] While not wishing to be bound by any theory, it is believed that the nitrogen contained in the metal oxides and / or quasi-metal oxides of the present invention and / or those produced by the methods of the present invention is firmly bonded to the metal / quasi-metal and is present at least partially, preferably completely, in the form of the corresponding nitride (e.g., Si3N4) or similar compounds. These nitrogen-containing compounds appear to be well-distributed within the metal / quasi-metal oxide particles, and even small amounts may have a significant impact on some metal / quasi-metal oxide properties, such as their mechanical strength, abrasion resistance (and grain formation), improved electrical conductivity, and / or improved electrostatic behavior, which may be beneficial for various applications. Furthermore, higher chemical stability is possible because the metal oxides and / or quasi-metal oxides are at least partially passivated by the corresponding metal nitride coating.

[0062] In a preferred embodiment of the invention, the pyrolytic metal oxides and / or quasi-metal oxides have a nitrogen content associated only with nitrides of the following metals and / or quasi-metals: silicon nitride (Si3N4), aluminum nitride (AlN), and titanium nitrides (TiN and / or Ti3N4).

[0063] Improved pyrolytic metal oxides and / or quasi-metal oxides may have up to 20 10 -4 weight% g / m 2 , up to 10 10- 4 weight% g / m 2 More preferably up to 8.0 10 -4 weight% g / m 2 More preferably up to 6 10 -4 weight% g / m 2 More preferably up to 5.0 10 -4 weight% g / m 2 Nitrogen content in weight % and in m 2 The ratio R3 of BET surface area per g. Additionally, the nitrogen content, expressed as a percentage by weight, is compared with the nitrogen content expressed as a percentage by weight. 2 The ratio R3 of the BET surface area per g can be within the range defined by the lower and upper limits as described above.

[0064] The thickening effect (also known as the thixotropic index) can be measured according to the method described in Example 2 of WO2013 / 156337: 3.85% by weight of a vapor-phase oxide is introduced and dispersed in Renlam® M1 epoxy resin (manufacturer: Huntsman Corporation) using a vacuum dissolver VMA-Getzmann Dispermat® CA 20-M1 at a rotational speed of 3000 rpm over a period of 5 minutes. The resulting viscosity of the epoxy resin filled with the vapor-phase oxide can be measured using an Anton-Paar Physica® rheometer MCR 301, system CP25-2, at 23°C for 5 s. -1 and 50 s -1 The thixotropic index of the gas-phase oxide can be calculated at a shear rate of 5 s. -1 The corresponding viscosity at 50 s -1 The quotient is calculated based on the viscosity obtained below.

[0065] The thixotropic index of the pyrolytic metal and / or quasi-metal oxides according to the present invention is preferably at least 1750, more preferably at least 1800, and even more preferably at least 2000.

[0066] Preferably, the pyrolytic metal oxide and / or quasi-metal oxide is silicon dioxide (silica, SiO2) or a mixture containing silicon dioxide.

[0067] The pyrolytic metal oxides and / or quasi-metal oxides preferably have a content of 10 μm. 2 / g to 600 m 2 The BET surface area is 15 to 600 m² / g, more preferably 20 to 600 m² / g, more preferably 30 to 550 m² / g, more preferably 50 to 500 m² / g, and most preferably 80 to 400 m² / g. The BET surface area can be determined according to DIN ISO 9277:2003-05.

[0068] The tamped density of the metal oxides and / or quasi-metal oxides of the present invention is generally less than 200 g / L, preferably up to 100 g / L, and more preferably up to 50 g / L.

[0069] Tamped density (also known as tapped density) can be determined according to DIN ISO 787-11:1995 "General methods of test for pigments and extenders - Part 11: Determination of tamped volume and apparent density after tamping".

[0070] In a preferred embodiment of the invention, the pyrolytic metal oxides and / or quasi-metal oxides have a nitrogen content of at least 0.03% by weight, preferably at least 0.04% by weight, and more preferably 0.05-0.20% by weight. Furthermore, in a further preferred embodiment, the pyrolytic metal oxides and / or quasi-metal oxides have a nitrogen content of at least 0.03% by weight, preferably at least 0.04% by weight, and more preferably 0.05-0.20% by weight. It may be advantageous to produce the pyrolytic metal oxides and / or quasi-metal oxides of the invention according to one of the versions and / or embodiments of the pyrolysis method as described herein.

[0071] The present invention further provides uses of metal oxides and / or quasi-metal oxides produced as described herein and optionally according to versions and / or embodiments of the method according to the invention, wherein said uses are as components of paints or coatings, silicones, pharmaceutical or cosmetic formulations, adhesives or sealants, toner compositions, for modifying the rheological properties of liquid systems, as anti-settling agents, for improving the flowability of powders, for improving the mechanical or optical properties of silicone compositions, and as components of lithium-ion batteries.

[0072] The following figures are intended to illustrate the method of the invention and suitable burners and burner heads in more detail. These figures represent only some exemplary and suitable embodiments of the equipment used (e.g., burners and burner heads) and should not be construed as limiting the scope of the invention itself in any way. Attached Figure Description

[0073] Therefore, as shown below:

[0074] Figure 1 : As two cross-sectional views (I, II), the first burner and the burner head are parallel to and include the longitudinal axis, and the other is perpendicular to the longitudinal axis;

[0075] Figure 2The second burner and burner head are shown in two cross-sectional views (I, II), one parallel to and including the longitudinal axis, and the other perpendicular to the longitudinal axis.

[0076] Figure 3 : The third burner head as a cross-sectional view; and

[0077] Figure 4 : A cross-sectional view perpendicular to the longitudinal axis, serving as a partial view of another type of burner head.

[0078] Burner 200 in Figure 1 Partial view I schematically shows a burner head 100 with longitudinal axis A, several feed lines 150, 152, a housing 160, and a product line 170 (outlet). Reference numeral 190 indicates a flame, shown schematically as a dashed line, having a flame axis parallel to or the same as longitudinal axis A. Figure 1 The overall flow direction of the burner head 100 shown in (I) is indicated by arrow B. The burner head 100 includes an inlet end 102, an outlet end 104, and two channels 112, 114, each channel having an outlet opening 140, 142 at the outlet end 104. In one version, the outlet openings are generally arranged in a common plane. No additional equipment required for operating the burner and the method discussed is shown in the figures, such as, but not limited to, additional processing units, pumps, compressors, tanks, sensors, actuators, ignition devices, power supplies, etc. Additional processing units may be present in the flow direction B and connected to the product line 170, such as, but not limited to, cooling units, deacidification units, and separation units (not shown) for metal oxides and / or quasi-metal oxides produced by the method of the present invention.

[0079] Furthermore, the flame tube may be part of the product line 170, for example, as a first section and / or as a connection portion to the flame chamber 162 of the housing 160 (not shown). Alternatively, the flame tube may be an integrated portion of the flame chamber 162 and / or the housing 160 (not shown). Such a flame tube may have a conical shape in the axial direction.

[0080] The term "flame axis" is defined by the main or central axis of the gas released from the burner head and / or the pyrolysis flame; the terms "flame axis" and "central axis" are used synonymously herein. Although a single flame axis is mentioned, it should be understood that the dynamic gas release or flame defines a corridor containing multiple axes rather than a single axis in a mathematical sense. Therefore, the central axis refers to the position and orientation of the axis with the highest statistical probability. Furthermore, this axis is alternatively or additionally defined by the symmetry of the outlet opening of the burner head and / or the flame-forming gas. Similarly, "center" should refer to something radially close to or overlapping the central axis and / or close to or overlapping the flame axis.

[0081] The term "plane" refers to a surface area, projected plane, and / or direct surface in a technical, rather than mathematical, sense. It is used for illustrative and explanatory purposes. Therefore, a "plane" can have not only two dimensions but also a finite third dimension, such as height or depth, and can be a narrow passageway. The terms "combustion chamber" and "flame chamber" are used synonymously.

[0082] According to the partial view I shown Figure 1 In this example, the burner head 100 includes two radially spaced channels 112 and 114, surrounded by a concentric (auxiliary) channel 118. Channel 112 is concentrically surrounded by the second channel 114, forming a tube-in-tube system. A plane 148, oriented perpendicular to the longitudinal axis A, defines the starting point or inlet of the flame chamber 162 in the flow direction B. Figure 1 In the illustrated embodiment, the outlet openings 140, 142 (generally) of the channels 112, 114 of the burner head 100 are located in this plane 148. The burner 200 includes a combustion chamber 162, or "flame chamber," in which pyrolysis occurs. Each incoming feed line 150, 152 is connected to one of the inner channels 112, 114 of the burner head 100.

[0083] The burner 200 includes an auxiliary passage 118 located between the outer passage 114 and the housing 160. The auxiliary passage 118 is radially outside the outer passage 114. At least one feed line 157, for example, connected to at least one flange element 158, leads into the auxiliary passage 118. In this process, auxiliary air can be directed into the auxiliary passage 118 and subsequently into the flame chamber 162. According to an embodiment not shown in the figures, the burner 100 does not include such an auxiliary passage and supplies auxiliary air or (auxiliary) oxygen-containing gas directly into the flame chamber 162 via at least one feed line.

[0084] Figure 1 Partial view II shows the concentric orientation of the channels 112, 114, 118 of the burner 200 and the housing 160. The DD line markings indicate the orientation of the cross-section, which is the same as, similar to, and / or parallel to the plane 148.

[0085] The auxiliary passage 118 opens to the atmosphere via flange 158 and draws in an auxiliary oxygen-containing gas, such as air, via the orifice and flange 158. The auxiliary passage 118 may be defined as a passage of the burner 200 or as a transition space between the burner head 100 and the housing 160 of the burner 200. According to an alternative embodiment (not shown), the auxiliary passage 118 is part of the burner head 100 and concentrically surrounds the outer passage 114.

[0086] The outlet openings 140, 142, and 148 of channels 112, 114, and 118 are (approximately) located within plane 148. Plane 148 represents the inlet end of the inner combustion chamber 162 in which the flame 190 expands in the flow direction B.

[0087] In this method, the feedstock ammonia (NH3) and hydrogen (H2) are supplied as a mixture through feed line 152 to the (second) channel 114, which is oriented parallel to the longitudinal axis A. Additionally, feedstock MP and (primary) air supplied by feed line 156 are directly supplied to the flame 190 via central channel 112. Premixing of NH3 and MP does not occur before the pyrolysis flame and / or combustion chamber 162.

[0088] The fuel gas guided via channel 114 can be a fuel gas mixture containing hydrogen (H2) and / or an auxiliary gas. The auxiliary gas can be nitrogen (N2), N2-containing gas, and / or oxygen-containing gas (O2). The auxiliary gas has a dilution effect and can also be supplied by a third feed line (not shown).

[0089] In similar Figure 1 In the reverse implementation scheme, the ammonia guiding channel is the central channel 112, and the MP guiding channel is the outer channel 114.

[0090] according to Figure 2 The alternative embodiment shown (in two partial views I, II) includes a burner 200 with a burner head 100 along a longitudinal axis A, several feed lines 152, 154, 156, a housing 160, and a product line 170. The burner head 100 includes an inlet end 102, an outlet end 104, and several channels 112, 114, 116, each channel having an outlet opening 140, 142, 144 at the outlet end 104. The outlet openings may be generally arranged in a common plane 146. The burner 200 is generally connected to and can be controlled by a control unit 120, with data connections indicated by dashed data lines 122. Any additional equipment or units required to operate the burner and the method discussed are generally known and therefore not shown in the figures.

[0091] according to Figure 2For example, burner 200 includes three channels 112, 114, and 116 in the radial direction. These channels form a tube-in-tube system. The first central channel 112 is concentrically surrounded by the second channel 114 and the third (outer) channel 116. The third channel 116 is the final channel of the burner head 100 in the radial direction. In the longitudinal direction, burner 200 includes three main sections 130, 132, and 134. The main sections in the axial direction are as follows: feed section 130, guide section 132, and release section 134. A plane 148 oriented perpendicular to the longitudinal axis A defines the end point of guide section 132 and the beginning point of release section 134 and / or flame chamber 162 in the flow direction B. Figure 2 In the illustrated embodiment, the outlet openings 140, 142, 144 (generally) of the channels 112, 114, 116 of the burner head 100 are located in this plane 148. The release section 134 includes a combustion chamber 162, also referred to as a flame chamber, in which pyrolysis occurs. The feed section 130 is defined as a section including at least partially inserted feed lines 152, 154, 156, each feed line connected to at least one of the internal channels 112, 114, 116 of the burner head 100.

[0092] according to Figure 2 In one embodiment, the burner 200 includes an auxiliary passage 118 located between the third (outer) passage 116 and the housing 160. The auxiliary passage 118 is at least partially radially outside the outer passage 116. For example, at least one feed line 157 connected to at least one flange element 158 ​​enters the auxiliary passage 118 and can direct auxiliary air into the auxiliary passage 118 and subsequently into the flame chamber 162. According to one embodiment not shown in the figures, the burner does not include such an auxiliary passage and provides auxiliary air or (auxiliary) oxygen-containing gas directly into the flame chamber 162 through at least one orifice and / or at least one feed line.

[0093] Figure 2 Partial view II shows the concentric orientation of the channels 110-118 of the burner 200 and the housing 160. The DD line indicates the orientation of the cross section, which is oriented in the same or similar manner as plane 148.

[0094] The guide section 132 is downstream of the feed section 130 in the flow direction, and is thus defined by the feeding of any raw material (reactant) in at least one of the internal channels 112, 114, 116 of the burner head 100, and, if applicable, by the auxiliary channel 118 for air supply to the burner 200. In other words, in the guide section 132, the (main) feed line is no longer connected, and a final gas flow is formed in the flow direction B. The channel 118 opens to the atmosphere via a flange 158 and draws in an auxiliary oxygen-containing gas, such as air, by means of at least one suitable element.

[0095] Release section 134 is located at the opposite end of guide section 132 (relative to section 130). The end of guide section 132 is substantially defined and restricted in the flow direction B by the outlet openings 140, 142, 144 of channels 112, 114, 116 within plane 148. Plane 148 in the flow direction B represents the inner combustion chamber 162 in which the flame 190 extends and the inlet end of release section 134.

[0096] In this method, the raw material MP and the main air can be similar to Figure 1 Ammonia (NH3) and fuel gas, such as hydrogen (H2), are supplied via feed line 156 to a central channel 112 oriented concentrically with the longitudinal axis A. Additionally, ammonia (NH3) and fuel gas, such as hydrogen (H2), are supplied via feed line 152 to a second (next) channel 114 and released directly into the flame 190, without premixing of ammonia (NH3) with MP before reaching the pyrolysis flame and / or combustion chamber 162. Thus, a first portion of the fuel gas is supplied via feed line 152 to form the pyrolysis flame 190. A second portion of the fuel gas and additional gases (such as nitrogen and / or optionally oxygen-containing gases) are supplied via feed line 154 to a third (outer) channel 116. The gas guided via the outer (jacketed) channel 116 is intended to form a jacketed flame (not shown). Finally, an auxiliary oxygen-containing gas, such as atmospheric air, is drawn into an auxiliary channel 118 and released into the flame chamber 162 once the flame is ignited.

[0097] exist Figure 3 In the embodiment shown, the burner 200 is substantially similar to Figure 2 The burner is constructed as shown in the accompanying drawings, so any missing components can be obtained from one of the other figures. However, the burner head 100 includes four inner channels 110, 112, 114, and 116, and provides flame 190 formation by means of a conical section 136. The conical section 136 is part of the guide section 132. Additionally, the conical section 136 includes an optional (short) annular section 138 at the outlet end (plane 148). The conical section 136 has a favorable effect on forming a stable and uniform pyrolysis flame.

[0098] according to Figure 3The burner head 100 includes a mixing chamber 180 and / or is connected to the mixing chamber 180, which is connected to a feed line 154 leading to an external passage 116, wherein a gas, such as a fuel gas mixture, is premixed. Figure 3 The implementation scheme's channels are designed to pipe gas into combustion chamber 162 in the following manner:

[0099] - First channel 112, first section of fuel gas

[0100] - Second channel 114, MP and the first part of the main air supply

[0101] - Third channel 110, the second part of ammonia and main air, and

[0102] - Fourth (outer) channel 116, the second part of fuel gas and nitrogen-containing gas.

[0103] Similar to Figure 1 or Figure 2 The auxiliary channel 118 may be part of the burner 200.

[0104] Finally, Figure 4 In one embodiment, a concept is shown where a set of smaller pipes 115, 117 form a concentric channel. This embodiment is... Figure 3 An alternative solution to the burner 200 shown is available. However, the concept of a set of (smaller) pipes can be used for at least one concentric (gas) passage in any of the described embodiments. The term "smaller" refers to the diameter of these "pipes" 115, 117 compared to the associated passage formed by the respective set of pipes. The smaller pipes 115, 117 have a circular cross-sectional area. Figure 4 The diagram only shows some of the smaller pipes in the group that form a channel. Nevertheless, as indicated by their respective dashed lines, the entire channel is constructed and / or filled by this group of smaller pipes. However, the smaller pipes in a group may be in direct contact with each other or be spaced apart in the circumferential direction (not shown). Alternatively, the (smaller) smaller pipes in a group may have a non-circular shape (not shown).

[0105] exist Figure 4 In the middle, the third channel 110 and the outer channel 116 are constructed from a set of smaller pipes 115 and 117. In an alternative embodiment, only one of channels 110, 112, 114 or 116 is constructed from a set of smaller pipes, or more than two channels are constructed from a set of smaller pipes.

[0106] It will be apparent to those skilled in the art that the burner 200 and / or burner head 100 may have any orientation different from that shown in the accompanying drawings, and any details provided herein require similar understanding in conjunction with different orientations of the burner or burner head. Furthermore, the burner 200 and / or burner head 100 need not have the simplified elongated form shown in the accompanying drawings, but rather have any available internal and external curved and / or angled geometry.

[0107] Generally speaking, any tips, advantages, and details provided regarding burners and burner heads, especially those related to... Figures 1 to 4 The discussion, together with the previous one, should apply in the same way, or if necessary, similarly to this method, and vice versa: the implementation scheme and details of the method can be related to the following. Figures 1 to 4 The discussion describes the details together with the application. Detailed Implementation

[0108] experiment

[0109] General method description:

[0110] exist Figure 1 The burner 200, schematically shown including a burner head 100, delivers 0.395 Nm 3 / h SiCl4 vapor premixed with (primary) air is introduced into the burner 100 via the central channel 112. The burner head 100 includes two channels 112 and 114, wherein the central channel 112 is also referred to as the first (inner) channel 112, and the radially outer channel 114 is also referred to as the second (outer) channel 114. Ammonia (NH3) and hydrogen (H2) as a fuel gas mixture are guided into the pyrolysis flame 190 and the combustion chamber 162 via the radially outer channel 114.

[0111] Auxiliary air is introduced separately into the burner 200 via auxiliary channel 118 located between the second channel 114 and the housing 160. "Main" oxygen-containing gas, also known as "main air," is defined as oxygen-containing gas or air directly guided through at least one channel of the burner head. "Auxiliary" oxygen-containing gas, also known as "auxiliary" air, generally refers to air that surrounds the flame outside the burner head and / or is drawn into or pumped into the flame during pyrolysis synthesis. In all embodiments except Comparative Example 6, if ammonia is used, it is introduced separately into the burner head via the second outer channel 114.

[0112] In all experiments, the amounts of oxygen and fuel gas (H2 + NH3) were adjusted such that the γ ratio (for H2 + NH3) = 1.5 and the λ ratio (for H2 + NH3) = 1.

[0113] The introduced gas is mixed and ignited at the outlet of the burner head, causing the flame to spread along flame axis A into combustion chamber 162. The particulate gas mixture is further cooled, and the resulting fumed silica powder is separated from the gas and deacidified using steam at 600°C in a conventional deacidification unit. The specific flow rates of ammonia, H2, (mainly) air, O2, and N2 used in the comparative examples and Examples 1-6 of this invention are given in Table 1. The properties of the obtained fumed silica samples are given in Table 2 below.

[0114] In all experiments and as used in this paper, Nm 3 / h means and is defined as the gas throughput (volume / time) at standard temperature (0°C; 273.15K) and pressure (1 atm; 1013.25 mbar).

[0115] “ "Defined as the ratio of the amount of hydrogen supplied to the burner head to the stoichiometric amount of hydrogen required for the SiCl4 hydrolysis reaction; and " "It is defined as the ratio of the amount of oxygen supplied to the burner head to the stoichiometric amount of hydrogen required for the combustion of fuel gases H2 and NH3. The volumetric flow rate of SiCl4 is 0.395 Nm³ / h."

[0116] about , Or, as with any other ratio provided herein, the volume of auxiliary air drawn into the combustion chamber and pyrolysis flame via the auxiliary passage 118 surrounding the burner head 100 is not taken into account.

[0117] Table 1: Method Parameters

[0118]

[0119] Where: R1 = NH3 / (H2+NH3); R2 = (H2+NH3+air+O2+N2+SiCl4) / SiCl4

[0120] Regarding Comparative Example 6, the SiCl4 and ammonia feedstock, serving as MP, were premixed before being introduced into the flame and before reaching the burner head. This premixing resulted in rapid reactor blockage observed at the burner outlet. Therefore, a continuous process over the expected production time was not feasible. Consequently, no product was separated in Comparative Example 6.

[0121] Refer to Table 1 and Figure 1 The channels of the burner head 100 are used for the corresponding airflows as given in Table 1A:

[0122] Table 1A: Method Parameters

[0123]

[0124] Table 2: Product Properties

[0125]

[0126] Adding ammonia and separating it from the metal precursor during the process of feeding it into the flame enables continuous production of fumed silica without any blockages.

[0127] Therefore, as shown in the last column of Table 1, the use of gaseous ammonia can improve the productivity of the apparatus, which shows the R2 ratio, i.e., the ratio of the total amount of gas per unit of given SiCl4, from 8.32 mol / mol (Comparative Example 1) to 6.22 mol / mol (Example 5). As shown in Table 2, it can also increase the thickening effect of the resulting silica from 1740 (Comparative Example 1) to 2455 (Example 3), and in Experiments 2 and 3 (with ammonia added, but no additional oxygen added), the BET surface area is significantly increased relative to Comparative Example 1 (without ammonia added).

[0128] BET surface area was determined according to DIN ISO 9277:2003-05.

[0129] The thickening effect (also known as the thixotropic index) was measured according to the method described in Example 2 of WO2013 / 156337:

[0130] 3.85 wt% fumed silica was introduced and dispersed in Renlam® M1 epoxy resin (manufacturer: Huntsman Corporation) over a 5-minute process at 3000 rpm using a VMA-Getzmann Dispermat® CA 20-M1 vacuum dissolver. The resulting viscosity of the silica-filled epoxy resin was measured using an Anton-Paar Physica® rheometer MCR 301 with a CP25-2 system at 23°C for 5 s. -1 and 50 s -1 The thixotropic index of the silica sample was calculated at a shear rate of 5 s. -1 The corresponding viscosity at 50 s -1 The quotient is calculated based on the viscosity obtained below.

[0131] Silica obtained using ammonia is characterized by a significantly higher nitrogen content (as determined by elemental analysis) compared to silica prepared under the same reaction conditions but without ammonia (Table 2).

Claims

1. A method for producing metal oxides and / or quasi-metal oxides using a burner (200), said burner (200) comprising a burner head (100) having at least two channels (112, 114) and an outlet end (104), The metal oxide or near-metal oxide mentioned above is selected from oxides of the following substances: aluminum (Al), titanium (Ti), zirconium (Zr), yttrium (Y), lithium (Li), magnesium (Mg), lanthanum (La), cerium (Ce), iron (Fe), zinc (Zn), and silicon (Si), or mixtures thereof. The method includes the following steps: - Provide oxygen-containing gas and fuel gas to the burner head (100); - Provide gaseous metal precursors and / or gaseous quasi-metal precursors (MP) to the burner head (100); - A flame (190) is provided by burning at least a portion of the oxygen-containing gas and the fuel gas at the outlet end (104) of the burner head (100); - Release the MP and / or the MP-containing mixture into the provided flame (190), Its features Gaseous ammonia (NH3) and / or a mixture of gaseous ammonia is supplied to the outlet end (104) of the burner head (100) via at least one gas passage (112, 114) and the ammonia (NH3) is released into the flame (190), wherein the ammonia (NH3) is not premixed with the MP or a mixture containing MP before the outlet end (104) of the burner head (100).

2. The method according to claim 1, wherein the method includes the step of mixing at least a portion of the fuel gas with ammonia and / or with the oxygen-containing gas before the outlet end (104) of the burner head (100).

3. The method according to claim 1 or 2, wherein the method includes the step of mixing at least a portion of the fuel gas with MP and / or with the oxygen-containing gas before the outlet end (104) of the burner head (100).

4. The method according to any one of the preceding claims, wherein the fuel gas comprises hydrogen (H2), carbon monoxide (CO), alcohol and / or has the general formula C n H 2n+2 Alkanes.

5. The method according to claim 4, wherein the molar ratio R1 of the amount of ammonia (NH3) to the total amount of ammonia and hydrogen (NH3+H2) is in the range of 0.05 to 1.0, preferably 0.1 to 0.9, and more preferably 0.2 to 0.

8.

6. The method according to any one of the preceding claims, wherein the molar ratio R2 of the total amount of gaseous raw material to the amount of MP is less than 8.3, preferably less than 8.0, more preferably less than 7.8, and even more preferably 4.0 to 7.

8.

7. The method according to any one of the preceding claims, wherein the MP is selected from at least one of the following substances: aluminum chloride (AlCl3), aluminum oxychloride (AlOCl), titanium tetrachloride (TiCl4), titanium trichloride (TiCl3), titanium oxychloride (TiOCl2), tetraalkoxytitanates such as tetraethoxytitanate Ti(OC2H5)4, tetraalkoxysilicates such as tetraethoxysilicate Si(OC2H5)4, cyclic siloxanes ([O-SiR2)). n Examples include octamethylcyclotetrasiloxane (D4) and acyclic siloxanes (R3Si-[O-SiR2)). n -O-SiR3) such as silicone oil, silicon tetrachloride (SiCl4), trichlorosilane (HSiCl3), methyltrichlorosilane (CH3SiCl3), dichlorosilane (H2SiCl2) and / or monochlorosilane (H3SiCl).

8. The method according to any one of the preceding claims, wherein the raw material ammonia (NH3) is produced at least in part from hydrogen (H2) obtained from the electrolysis of water or aqueous solution, preferably from renewable energy sources such as solar energy, wind energy, geothermal energy, hydropower from flowing water, tidal energy, energy obtained from the combustion of biomass, waste or biofuel, and combinations of these energy sources.

9. The method according to any one of the preceding claims, wherein the metal oxide and / or quasi-metal oxide has a molecular weight of 10 to 600 μm. 2 / g, preferably 20 to 600 m 2 / g of BET surface area.

10. The method according to any one of the preceding claims, wherein the burner head (100) includes at least two central channels (112, 114) in the radial direction, and a concentric (auxiliary) channel (118) surrounds these central channels (112, 114), wherein the channel (112) is concentrically surrounded by the second channel (114), and wherein the channels (112, 114) form a tube-in-tube system.

11. Pyrolytic metal oxides and / or quasi-metal oxides, selected from oxides of aluminum (Al), titanium (Ti), zirconium (Zr), yttrium (Y), lithium (Li), magnesium (Mg), lanthanum (La), cerium (Ce), iron (Fe), zinc (Zn), and silicon (Si), or mixtures thereof, wherein the metal oxides and / or the quasi-metal oxides have a BET surface area of ​​10 to 600 m². 2 / g and nitrogen content in weight % and in m 2 The ratio R3 of the BET surface area per g is at least 1.

0. 10 -4 weight% g / m 2 Preferably at least 1.1 10- 4 weight% g / m 2 More preferably at least 1.2 10 -4 weight% g / m 2 More preferably at least 1.3 10 -4 weight% g / m 2 More preferably at least 1.5 10 -4 weight% g / m 2 More preferably at least 1.9 10 -4 weight% g / m 2 More preferably at least 2.5 10 -4 weight% g / m 2 More preferably at least 3.0 10 -4 weight% g / m 2 The nitrogen content mentioned therein is only related to metals and / or metalloid nitrides.

12. The pyrolytic metal oxide and / or quasi-metal oxide according to claim 11, wherein the nitrogen content of the metal oxide and / or quasi-metal oxide is only related to metal and / or quasi-metal nitrides from the group consisting of silicon nitride (Si3N4), aluminum nitride (AlN), and titanium nitrides (TiN and / or Ti3N4).

13. The pyrolytic metal oxide and / or quasi-metal oxide according to claim 11 or 12, wherein the pyrolytic metal oxide and / or quasi-metal oxide has a content of at most 20 10 -4 weight% g / m 2 , up to 10 10- 4 weight% g / m 2 More preferably up to 8.0 10 -4 weight% g / m 2 More preferably up to 6 10 -4 weight% g / m 2 More preferably up to 5.0 10 -4 weight% g / m 2 Nitrogen content in weight % and in m 2 R3 is the ratio of BET surface area per g.

14. The pyrolytic metal oxide and / or quasi-metal oxide according to any one of claims 11 to 13, wherein the nitrogen content of the metal oxide and / or quasi-metal oxide is at least 0.03% by weight, preferably at least 0.04% by weight, more preferably 0.05-0.20% by weight.

15. The pyrolytic metal oxide and / or quasi-metal oxide according to any one of claims 11 to 14, obtained by the pyrolysis method according to any one of claims 1 to 10.

16. The use of the metal oxide and / or quasi-metal oxide according to any one of claims 11 to 15 as a component of paint or coating, organosilicon, pharmaceutical or cosmetic preparation, adhesive or sealant, colorant composition, for modifying the rheological properties of a liquid system, as an anti-settling agent, for improving the flowability of powder, for improving the mechanical or optical properties of organosilicon compositions, and as a component of a lithium-ion battery.

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