WO2024251744A1 - Réacteurs servant à la décomposition de nh3 à hautes températures - Google Patents

Réacteurs servant à la décomposition de nh3 à hautes températures Download PDF

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WO2024251744A1
WO2024251744A1 PCT/EP2024/065354 EP2024065354W WO2024251744A1 WO 2024251744 A1 WO2024251744 A1 WO 2024251744A1 EP 2024065354 W EP2024065354 W EP 2024065354W WO 2024251744 A1 WO2024251744 A1 WO 2024251744A1
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Prior art keywords
metal alloy
content
total weight
chromium
weight
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PCT/EP2024/065354
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German (de)
English (en)
Inventor
Ruth Kremer
Tobias Fischer
Thorsten Brakhane
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ThyssenKrupp AG
ThyssenKrupp Industrial Solutions AG
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ThyssenKrupp AG
ThyssenKrupp Uhde GmbH
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Priority claimed from LU103141A external-priority patent/LU103141B1/de
Priority claimed from DE102023114700.5A external-priority patent/DE102023114700A1/de
Application filed by ThyssenKrupp AG, ThyssenKrupp Uhde GmbH filed Critical ThyssenKrupp AG
Priority to JP2025570650A priority Critical patent/JP2026524761A/ja
Priority to KR1020257040274A priority patent/KR20260005380A/ko
Priority to EP24731874.4A priority patent/EP4719640A1/fr
Priority to CN202480038060.4A priority patent/CN121335750A/zh
Publication of WO2024251744A1 publication Critical patent/WO2024251744A1/fr
Anticipated expiration legal-status Critical
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    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen; Reversible storage of hydrogen
    • C01B3/02—Production of hydrogen; Production of gaseous mixtures containing hydrogen
    • C01B3/04—Production of hydrogen; Production of gaseous mixtures containing hydrogen by decomposition of inorganic compounds
    • C01B3/047—Decomposition of ammonia
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J19/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J19/02—Apparatus characterised by being constructed of material selected for its chemically-resistant properties
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J19/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J19/24—Stationary reactors without moving elements inside
    • B01J19/2415—Tubular reactors
    • B01J19/2425—Tubular reactors in parallel
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
    • B01J23/70—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper
    • B01J23/76—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper combined with metals, oxides or hydroxides provided for in groups B01J23/02 - B01J23/36
    • B01J23/84—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper combined with metals, oxides or hydroxides provided for in groups B01J23/02 - B01J23/36 with arsenic, antimony, bismuth, vanadium, niobium, tantalum, polonium, chromium, molybdenum, tungsten, manganese, technetium or rhenium
    • B01J23/85—Chromium, molybdenum or tungsten
    • B01J23/86—Chromium
    • B01J23/866—Nickel and chromium
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
    • B01J23/70—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper
    • B01J23/76—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper combined with metals, oxides or hydroxides provided for in groups B01J23/02 - B01J23/36
    • B01J23/84—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper combined with metals, oxides or hydroxides provided for in groups B01J23/02 - B01J23/36 with arsenic, antimony, bismuth, vanadium, niobium, tantalum, polonium, chromium, molybdenum, tungsten, manganese, technetium or rhenium
    • B01J23/85—Chromium, molybdenum or tungsten
    • B01J23/88—Molybdenum
    • B01J23/887—Molybdenum containing in addition other metals, oxides or hydroxides provided for in groups B01J23/02 - B01J23/36
    • B01J23/8878—Chromium
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J7/00—Apparatus for generating gases
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/00049—Controlling or regulating processes
    • B01J2219/00051—Controlling the temperature
    • B01J2219/00159—Controlling the temperature controlling multiple zones along the direction of flow, e.g. pre-heating and after-cooling

Definitions

  • the invention relates to reactors and reactor components which have good resistance to NFL and N2 and possibly H2O at high temperatures and medium pressure, so that they can be used in the catalytic decomposition of NH3 to N2 and H2 on an industrial scale.
  • H2 can be obtained electrolytically from H2O using renewable energy and then converted into NH3 with N2.
  • NH3 can be stored and transported much more safely than H2.
  • NH3 can then be broken down into H2 and N2. After N2 has been separated, H2 has a wide variety of industrial applications.
  • the reaction temperature at which the catalytic decomposition of NH3 takes place is determined in particular by the choice of the NH3 decomposition catalyst.
  • a variety of materials have been proposed as catalysts for the decomposition of NH3, which are active at different temperatures (see, for example, II. Lucentini et al., Ind. Eng. Chem. Res. 2021, 60, 18560-18611).
  • Ruthenium-based NFL decomposition catalysts have the advantage that conversions of more than 90% can be achieved at comparatively low temperatures. However, the maximum achievable conversions are limited, so that a considerable residual content of non-decomposed NH3 remains in the product gas, which, given the amount, may have to be separated by additional measures.
  • Nickel-based NFL decomposition catalysts have the advantage that significantly higher conversions can be achieved. In the product gas, therefore, only a small residual content of non-decomposed NH3 remains, which can be removed by conventional measures for purifying FL, in particular by pressure swing adsorption, without the need for additional measures. However, the temperatures required for nickel-based NHs decomposition catalysts are significantly higher.
  • Reactors designed analogously to primary reformers are particularly suitable for such a reaction.
  • the combustion gas and the reaction gas are physically separated from one another and passed through the reactor, but are in heat exchange with one another.
  • the combustion gas is burned with the aid of burners and with the supply of combustion air in a combustion chamber, from which a heat flow flows into at least one physically separated reaction chamber.
  • the NFF reduction catalyst is arranged in the reaction chamber and the reaction gas flows through it, so that the catalyzed reaction takes place there.
  • several reaction chambers can be designed as tubes, each of which is filled with NFF reduction catalyst and the reaction gas flows through it in parallel. These tubes are arranged, for example, as a bundle within the combustion chamber, without the combustion gas and reaction gas mixing.
  • the materials from which the reaction chambers and other components of such reactors are made must withstand considerable loads at considerable temperatures.
  • the temperatures generated by the combustion of the combustion gas in the combustion chamber are significantly higher than the temperatures of the reaction gas in the reaction chamber.
  • the heat flow from the combustion chamber to the reaction chamber is based on this temperature gradient, among other things.
  • K. Tjorko et al., Oxidation of Metals Vol. 44, 453-474 (1995) relates to a comparison of internal nitridation in NH; and in N2.
  • Nitriding requires the dissociation of N2 or NH3.
  • the dissociation of N2 only occurs to a significant extent above about 700°C. Therefore, at temperatures below about 700°C, nitriding is determined by the presence of NH3. Even at very high temperatures (1000°C), nitriding is stronger with NH3 than with N2.
  • HJ Grabke et al., Materials and Corrosion 2003, 54(11), 895-902 concerns investigations in which iron, nickel, ferritic 1-18%Cr steels, austenitic 18%Cr-9%Ni and 20%Cr-3 ⁇ Ni steels and a 16% CrNi base alloy were exposed at 500°C in He-30%H 2 O and 70%H 2 O-30% NH 3 in order to compare the corrosion behaviour of these materials in water vapour as in conventional power plants with their behaviour in a NH 3 TUO mixture, ie under the conditions of the "Kalina cycle".
  • Nitridation explains why nitridation occurs and how it attacks various metals, in some cases penetrating deeper than oxidation. Nitridation and its effects on metals and alloys in high temperature air as well as in NH3-H 2 O, NH3, H2-N2-NH3 and N2 environments are discussed.
  • MO Cojocaru et al., Materials 2021, 14, 2432 concerns the effects of modifying the activity of nitrating agents by diluting ammonia with nitrogen.
  • E. Wolowiec-Korecka et al., Coatings 2023, 13, 257, 1-12 concerns the stability of layered nitrides during nitriding under low pressure.
  • NH3 is often mixed with traces of H2O for storage and transport in order to reduce the risk of stress corrosion cracking for unalloyed steel. This increases the oxygen partial pressure in the reactor at high temperatures, so that oxidation can also play a role in addition to nitriding.
  • the reverse process is the synthesis of NH3 from N2 and H2 in the Haber-Bosch process.
  • Alloy 600 Another material suitable for the Haber-Bosch process is Alloy 600, which, however, is only approved for temperatures of up to 649°C according to The American Society of Mechanical Engineers (ASME) Boiler and Pressure Vessel Code (BPVC) Sec II-D.
  • ASME American Society of Mechanical Engineers
  • BPVC Pressure Vessel Code
  • the reaction mechanisms that take place can usually correspond more to those of a fluid or a gas. This typically depends on the medium itself and on other different parameters.
  • the density is a determining parameter. At low density, the behavior is more like that of a gas, while at high density the behavior of a liquid predominates (limit low - high approx. 0.2 g/ml).
  • supercritical CO2 for example, the water content, the content of impurities and the temperature are determining parameters. At high temperatures, in dry CO2, classic high-temperature processes. Traces of water lead to significant erosive corrosion.
  • the supercritical behavior of CO2 and NH3 can be considered comparable to a first approximation. NH3 often contains traces of water. As with supercritical CO2, condensation would be possible and not just gas phase reactions.
  • the other properties of the metal alloy are also crucial, in particular hardness, tensile strength, elongation, elongation at break, yield strength, elastic modulus, density, electrical resistance, melting range, thermal conductivity, specific heat capacity, etc. Processability, in particular weldability, also plays a role.
  • the production of H2 should be safe, economical and possible on an industrial scale.
  • a first aspect of the invention relates to a plant for producing H2 by catalytic decomposition of NH3 to N2 and H2; wherein the plant comprises a reactor which contains an NFF decomposition catalyst; wherein the reactor comprises at least one component which is at least partially made of a metal alloy; wherein the metal alloy comes into direct contact with the NH3 and/or N2 at least in one area of its surface during operation of the reactor; preferably with NH3, N2 and H2O or their dissociation products; and wherein the metal alloy contains nickel, chromium or both nickel and chromium, wherein the total content of nickel and/or chromium is at least 15% by weight, based on the total weight of the metal alloy.
  • total content of "A and/or B” means that the metal alloy according to the invention contains either (i) both A and B, and the total content is then the sum of the two individual contents of A and B, or (ii) does not contain B, so that the total content then refers to the content of A alone, or (iii) does not contain A, so that the total content then refers to the content of B alone.
  • the metal alloy contains nickel and chromium with a total content of nickel and chromium of at least 15 wt.%, based on the total weight of the metal alloy.
  • the metal alloy according to the invention contains at least two metals selected from the group consisting of nickel, cobalt, chromium, iron, molybdenum, manganese, niobium, cerium, aluminum, titanium, silicon, tungsten, copper, boron, zirconium, lanthanum and yttrium.
  • the metal alloy according to the invention contains at least three metals selected from the group consisting of nickel, cobalt, chromium, iron, molybdenum, manganese, niobium, cerium, aluminum, titanium, silicon, tungsten, copper, boron, zirconium, lanthanum and yttrium.
  • the metal alloy according to the invention contains at least four metals selected from the group consisting of nickel, cobalt, chromium, iron, molybdenum, manganese, niobium, cerium, aluminum, titanium, silicon, tungsten, copper, boron, zirconium, lanthanum and yttrium.
  • the metal alloy according to the invention contains at least five metals selected from the group consisting of nickel, cobalt, chromium, iron, molybdenum, manganese, niobium, cerium, aluminum, titanium, silicon, tungsten, copper, boron, zirconium, lanthanum and yttrium.
  • the content of nickel and possibly also cobalt is an important parameter for sufficient resistance to nitriding. This is particularly due to the fact that nickel and cobalt in iron-based alloys reduce the solubility of nitrogen, which makes internal nitriding more difficult.
  • the total content of nickel or nickel and cobalt is preferably at least 40% by weight, based on the total weight of the metal alloy.
  • chromium is rather disadvantageous in terms of resistance to nitriding. This is particularly due to the fact that chromium increases the solubility of nitrogen in nickel-based alloys and thus the tendency towards nitriding.
  • an oxide covering layer is formed when the partial pressure of O 2 is sufficiently high.
  • the partial pressure of O 2 and H 2 is determined thermodynamically by the equilibrium 2 H 2 O «-> 2 H 2 + O 2. If the partial pressure of O 2 is lower than the equilibrium pressure of O 2 for the metal/metal oxide equilibrium, no oxide is formed.
  • chromium has a beneficial effect on corrosion resistance, because chromium forms the stable oxide CYOs.
  • CYO3 is also very low partial pressures of O 2 , unlike iron oxides. Even a low content of a few ppm of H 2 O can lead to a covering layer of C'nCf, which significantly reduces nitriding. This is the case, for example, when the NH3 gas mixtures at 900°C contain only 45 ppm H 2 O.
  • the chromium content must be high enough so that a sufficiently dense covering layer of C'nCh can form and is also maintained. The latter means that the supply of chromium must be guaranteed in order to ensure the stable growth of a covering layer of Cr20s.
  • the chromium content is preferably at least 18 wt.%, based on the total weight of the metal alloy.
  • the metal alloy according to the invention therefore contains at least 30% by weight, preferably at least 33% by weight of nickel and/or cobalt (total content) and at least 15% by weight, preferably at least 19% by weight of chromium, in each case based on the total weight of the metal alloy. In preferred embodiments, the metal alloy according to the invention contains at least 40% by weight of nickel and/or cobalt (total content) and at least 20% by weight of chromium, in each case based on the total weight of the metal alloy.
  • the metal alloy according to the invention therefore contains at least 30% by weight, preferably at least 33% by weight, of nickel and at least 15% by weight, preferably at least 19% by weight, of chromium, in each case based on the total weight of the metal alloy. In preferred embodiments, the metal alloy according to the invention contains at least 40% by weight of nickel and at least 20% by weight of chromium, in each case based on the total weight of the metal alloy.
  • the metal alloy according to the invention therefore contains at least 33% by weight of cobalt and at least 15% by weight of chromium, each based on the total weight of the metal alloy. In preferred embodiments, the metal alloy according to the invention contains at least 40% by weight of cobalt and at least 20% by weight of chromium, each based on the total weight of the metal alloy.
  • the metal alloy according to the invention contains nickel, chromium and iron, wherein the nickel content is preferably greater than the chromium content.
  • the metal alloy according to the invention contains nickel, cobalt, chromium and iron, wherein the total content of nickel and cobalt is preferably greater than the content of chromium.
  • a "reactor” is a device for the catalytic decomposition of NH3 to N2 and H2.
  • the reactor according to the invention is typically a confined space which has been specially designed and manufactured in order to be able to carry out and control the catalytic decomposition of NH3 to N2 and H2 under defined conditions.
  • a "metal alloy” is a macroscopically homogeneous metallic material which is typically obtained by melting together various metals, whereby non-metals and/or semi-metals can also be included. The metals, non-metals and/or semi-metals can be present in elemental form, as intermetallic phases and/or as other compounds.
  • the metal alloy can be crystalline, semi-crystalline or amorphous.
  • Metals which are particularly important according to the invention and which can be included in the metal alloy according to the invention are nickel, cobalt, chromium and iron, but also possibly aluminum and titanium.
  • Other metals which can be included in the metal alloy according to the invention are, for example, molybdenum, tungsten, niobium, copper, aluminum, titanium, silicon, boron, lanthanum, manganese, vanadium, cerium, yttrium, zirconium, lead and others.
  • Particularly important non-metals and semi-metals according to the invention, which can be contained in the metal alloy according to the invention are boron, carbon, silicon, nitrogen, phosphorus, sulfur, and others.
  • an "NH 3 decomposition catalyst” catalyzes the decomposition of NH 3 to N 2 and H 2. To achieve yields greater than 90%, elevated temperatures of the NH 3 are usually required, preferably at least 500°C.
  • in direct contact with the NH3 and/or N2 means that at least in one area between the metal alloy and the NH3 and/or N2 no further material is arranged and that the NH3 and/or N2 can interact with the surface of the metal alloy in at least this area.
  • modifications to the surface of the metal alloy are permissible for direct contact within the meaning of the invention, for example the formation of covering layers of oxides and nitrides.
  • the metal alloy does not have to come into complete contact with the NH3 and/or N2, or its surface does not have to come into full contact with the NH3 and/or N2.
  • the metal alloy comes into direct contact with NH3, N2 and H2O or their dissociation products (N2, H2 or O2) at least in one area of its surface.
  • the plant according to the invention comprises a reactor in which, during operation of the plant, NH3 is catalytically decomposed to form a product gas which comprises N2, H2 and possibly undecomposed NH3.
  • the system according to the invention comprises one or more of the following devices which are in fluid communication with one another:
  • the reactor according to the invention preferably comprises a plurality of chambers which are physically separated from one another.
  • the reactor preferably comprises at least one reaction chamber and at least one combustion chamber.
  • the reactor according to the invention is preferably designed analogously to a primary reformer.
  • the reactor according to the invention preferably comprises
  • combustion chambers for the combustion of a combustion gas to produce combustion heat and a flue gas (exhaust gas);
  • reaction chambers for the catalytic decomposition of NH3 to produce a product gas comprising N2, H2 and possibly undecomposed NH3.
  • Combustion chamber(s) and reaction chamber(s) are preferably physically separated from one another so that there is no mixing of combustion gas on the one hand and NH3 (reactant gas) or product gas on the other hand during operation of the reactor.
  • Combustion chamber(s) and reaction chamber(s) are preferably configured such that when the reactor is operating, a heat flow of the generated combustion heat occurs from the combustion chamber(s) to the reaction chamber(s). When the reactor is operating, this heat flow preferably serves to maintain the endothermic catalytic decomposition of NH3.
  • the reaction chamber(s) are tubular, i.e. have a cylindrical shape.
  • several such tubular reaction chambers are arranged parallel to one another as a bundle in a common combustion chamber.
  • Each combustion chamber preferably contains one or more burners for the combustion of combustion gas.
  • the flame formed in this way is preferably located in spatial proximity to the outer wall of at least one reaction chamber which contains NfL formation catalyst during operation of the reactor.
  • combustion heat then preferably flows from the interior of the combustion chamber through the wall of the at least one reaction chamber and thus carries heat up to towards the NHs decomposition catalyst, through which NH3 flows and where the endothermic decomposition of NH3 takes place.
  • the reactor according to the invention also comprises at least one component which is at least partially constructed from a metal alloy which comes into direct contact with the NH3 and/or N2 during operation of the reactor.
  • the component is a reaction chamber or an element of a reaction chamber, wherein the NH3 decomposition catalyst is arranged in the interior of the reaction chamber.
  • the reactor according to the invention then preferably contains a reaction chamber which comprises the component and the NH3 decomposition catalyst.
  • the component is constructed entirely from the metal alloy according to the invention, i.e. the component consists entirely of the metal alloy.
  • the wall of the reaction chamber consists of the component and thus entirely of the metal alloy.
  • the inner surface of the wall of the reaction chamber faces the NEE decomposition catalyst and the metal alloy from which the wall of the reaction chamber is made comes into direct contact with the NH3 and/or N2 in at least one area when the reactor is in operation.
  • the wall of the reaction chamber preferably comprises the component.
  • the component can be tubular and arranged concentrically within another tubular element with which it together forms the wall of the reaction chamber.
  • the inner surface of the component then faces the NCH decomposition catalyst and the metal alloy from which the inner component of the wall is made comes into direct contact with the NH3 and/or N2 in at least one area when the reactor is in operation.
  • the component is only partially constructed from the metal alloy according to the invention.
  • the component can be multi-layered, with one of the layers of the component, preferably an outer layer, being constructed from the metal alloy according to the invention, i.e. this layer of the component consists of the metal alloy, whereas other layers of the component can consist of other materials and/or of alloys according to the invention of the same or a different composition.
  • the component only partially constructed from the metal alloy according to the invention is a reaction chamber in the interior of which the NIL decomposition catalyst is arranged
  • the component can be a reaction chamber with a multi-layer wall, wherein the multi-layer wall has an inner layer and an outer layer.
  • the inner surface of the inner layer of the The component then faces the NH3 decomposition catalyst and the metal alloy of which the inner layer is made comes into direct contact with the NH3 and/or N2 in at least one area during operation of the reactor.
  • the entire inner surface of the reaction chamber which faces the NH3 decomposition catalyst and which comes into direct contact with the NH3 and/or N2 during operation of the reactor, is constructed from the metal alloy.
  • the entire inner surface of the reactor which comes into direct contact with the NH3 and/or N2 during operation of the reactor, is constructed from the metal alloy.
  • the reactor according to the invention contains an NH3 decomposition catalyst. If NH3 flows through the NfU decomposition catalyst under reaction conditions, it catalyzes the decomposition of NH3 to N2 and H2.
  • NH3 decomposition catalyst various materials can be considered as NH3 decomposition catalyst.
  • the reaction temperature at which the catalytic decomposition of NH3 takes place is determined in particular by the choice of the NH3 decomposition catalyst.
  • the NPh decomposition catalyst is catalytically active with respect to the decomposition of NH3 at a temperature in the range of at least 500°C, preferably at least 520°C, more preferably at least 540°C, even more preferably at least 550°C, most preferably at least 580°C and in particular at least 600°C.
  • Catalyst active means that conversions of at least 90% of decomposition products N2 and H2 are obtained in relation to the amount of NH3 used (measured under standard conditions in pure NH3 at a pressure of 1013 hPa and a space velocity of 36 LgKat' 1 ).
  • the NH3 decomposition catalyst has an apparent activation energy E app of at least 50 kJ-mol 1 , more preferably at least 75 kJ-mol 1 , even more preferably at least 100 kJ-mol 1 , most preferably at least 125 kJ-mol 1 , and in particular at least 150 kJ-mol 1 with respect to the decomposition of NH3.
  • apparent activation energy E app is known to a person skilled in the art, for example by determination from Arrhenius plots based on measurements under standard conditions in pure NH3 at a pressure of 1013 hPa and a space velocity of 36 LgKat 1 .
  • a nickel-based NFF decomposition catalyst is used.
  • the reaction temperature determines the equilibrium conversion. At 900°C and 20 bar pressure, the decomposition of NH3 is almost quantitative. At 650°C, the conversion of NH3 is about 98.5%, at 500°C only about 95%.
  • reaction temperatures are preferably set in the range from about 600°C to about 900°C, preferably about 600°C to about 700°C, so that a high conversion is achieved. With regard to energy balance and conversion, optimal Reaction temperatures in the range of about 630°C to 640°C.
  • Nickel-based NH 3 decomposition catalysts are advantageous despite the comparatively high reaction temperature.
  • the NH 3 decomposition catalyst preferably comprises supported nickel.
  • Preferred carrier materials are selected from the group consisting of Al2O3, MgO, SiO2, mesoporous SiO2 (e.g. MCF-17, MCM-41, SBA-15), zeolite (e.g.
  • the metal alloy according to the invention contains nickel and chromium with a total nickel and chromium content of at least 15% by weight, based on the total weight of the metal alloy.
  • the total nickel and chromium content is at least 15.5% by weight, preferably at least 16.0% by weight, preferably at least 16.5% by weight, more preferably at least 17.0% by weight, even more preferably at least 17.5% by weight, most preferably at least 18.0% by weight, and in particular at least 18.5% by weight, in each case based on the total weight of the metal alloy.
  • the total content of nickel and chromium is at least 20 wt.%, preferably at least 25 wt.%, more preferably at least 30 wt.%, even more preferably at least 35 wt.%, most preferably at least 40 wt.%, and in particular at least 45 wt.%, in each case based on the total weight of the metal alloy.
  • the total content of nickel and chromium is at least 50 wt.%, preferably at least 55 wt.%, more preferably at least 60 wt.%, even more preferably at least 65 wt.%, most preferably at least 70 wt.%, and in particular at least 75 wt.%, in each case based on the total weight of the metal alloy.
  • the total content of nickel and chromium is at least 80 wt.%, preferably at least 85 wt.%, more preferably at least 90 wt.%, in each case based on the total weight of the metal alloy.
  • the total content of nickel and chromium is at most 85 wt.%, preferably at most 80 wt.%, more preferably at most 75 wt.%. %, more preferably at most 70 wt. %, most preferably at most 65 wt. %, and in particular at most 60 wt. %, each based on the total weight of the metal alloy.
  • the metal alloy according to the invention contains nickel.
  • the nickel content is at least 5.0 wt.%, preferably at least 10 wt.%, more preferably at least 15 wt.%, even more preferably at least 20 wt.%, most preferably at least 30 wt.%, and in particular at least 35 wt.%, in each case based on the total weight of the metal alloy.
  • the nickel content is at least 40 wt.%, preferably at least 45 wt.%, more preferably at least 50 wt.%, even more preferably at least 55 wt.%, most preferably at least 60 wt.%, and in particular at least 65 wt.%, in each case based on the total weight of the metal alloy.
  • the nickel content is at least 70 wt.%, preferably at least 75 wt.%, in each case based on the total weight of the metal alloy.
  • the nickel content is in increasing order of preference in the range of 20 ⁇ 15 wt.%, 20 ⁇ 10 wt.%, or 20 ⁇ 5.0 wt.%, each based on the total weight of the metal alloy.
  • the nickel content is in ascending order of preference in the range of 30 ⁇ 25 wt.%, 30 ⁇ 20 wt.%, 30 ⁇ 15 wt.%, 30 ⁇ 10 wt.%, or 30 ⁇ 5.0 wt.%, each based on the total weight of the metal alloy.
  • the nickel content is in increasing order of preference in the range of 40 ⁇ 35 wt.%, 40 ⁇ 30 wt.%, 40 ⁇ 25 wt.%, 40 ⁇ 20 wt.%, 40 ⁇ 15 wt.%, 40 ⁇ 10 wt.%, or 40 ⁇ 5.0 wt.%, each based on the total weight of the metal alloy.
  • the nickel content is in increasing order of preference in the range of 50 ⁇ 30 wt.%, 50 ⁇ 25 wt.%, 50 ⁇ 20 wt.%, 50 ⁇ 15 wt.%, 50 ⁇ 10 wt.%, or 50 ⁇ 5.0 wt.%, each based on the total weight of the metal alloy.
  • the nickel content is in the range of 60 ⁇ 20 wt.%, 60 ⁇ 15 wt.%, 60 ⁇ 10 wt.%, or 60 ⁇ 5.0 wt.%, in increasing order of preference, in each case based on the total weight of the metal alloy.
  • the nickel content is, with increasing preference, in the range of 70 ⁇ 10 wt.%, or 70 ⁇ 5.0 wt.%, in each case based on the total weight of the metal alloy.
  • the nickel content is at most 60 wt.%, preferably at most 55 wt.%, more preferably at most 50 wt.%, even more preferably at most 45 wt.%, most preferably at most 40 wt.%, and in particular at most 35 wt.%, in each case based on the total weight of the metal alloy.
  • the metal alloy according to the invention contains chromium.
  • the chromium content is at most 40 wt.%, preferably at most 38 wt.%, more preferably at most 36 wt.%, even more preferably at most 35 wt.%, most preferably at most 34 wt.%, and in particular at most 32 wt.%, in each case based on the total weight of the metal alloy.
  • the chromium content is at most 30 wt.%, preferably at most 28 wt.%, more preferably at most 26 wt.%, even more preferably at most 24 wt.%, most preferably at most 22 wt.%, and in particular at most 20 wt.%, in each case based on the total weight of the metal alloy.
  • the chromium content is at least 12% by weight, preferably at least 15% by weight, more preferably at least 18% by weight, even more preferably at least 21% by weight, most preferably at least 24% by weight, and in particular at least 27% by weight, in each case based on the total weight of the metal alloy.
  • the chromium content is, with increasing preference, in the range of 10 ⁇ 7.5 wt.%, 10 ⁇ 5.0 wt.%, or 10 ⁇ 2.5 wt.%, in each case based on the total weight of the metal alloy.
  • the chromium content is, with increasing preference, in the range of 12.5 ⁇ 10 wt.%, 12.5 ⁇ 7.5 wt.%, 12.5 ⁇ 5.0 wt.%, or 12.5 ⁇ 2.5 wt.%, in each case based on the total weight of the metal alloy.
  • the chromium content is, with increasing preference, in the range of 15 ⁇ 12.5 wt.%, 15 ⁇ 10 wt.%, 15 ⁇ 7.5 wt.%, 15 ⁇ 5.0 wt.%, or 15 ⁇ 2.5 wt.%, in each case based on the total weight of the metal alloy.
  • the chromium content is in the range of 17.5 ⁇ 15 wt.%, 17.5 ⁇ 12.5 wt.%, 17.5 ⁇ 10 wt.%, 17.5 ⁇ 7.5 wt.%, 17.5 ⁇ 5.0 wt.%, or 17.5 ⁇ 2.5 wt.%, in increasing order of preference, in each case based on the total weight of the metal alloy.
  • the chromium content is in the range of 19 ⁇ 17.5 wt.%, 19 ⁇ 15 wt.%, 19 ⁇ 12.5 wt.%, 19 ⁇ 10 wt.%, 19 ⁇ 7.5 wt.%, 19 ⁇ 5.0 wt.%, or 19 ⁇ 2.5 wt.%, in increasing order of preference, in each case based on the total weight of the metal alloy.
  • the chromium content is in increasing order of preference in the range of 20 ⁇ 17.5 wt.%, 20 ⁇ 15 wt.%, 20 ⁇ 12.5 wt.%, 20 ⁇ 10 wt.%, 20 ⁇ 7.5 wt.%, 20 ⁇ 5.0 wt.%, or 20 ⁇ 2.5 wt.%, each based on the total weight of the metal alloy.
  • the chromium content is in increasing order of preference in the range of 22.5 ⁇ 20 wt.%, 22.5 ⁇ 17.5 wt.%, 22.5 ⁇ 15 wt.%, 22.5 ⁇ 12.5 wt.%, 22.5 ⁇ 10 wt.%, 22.5 ⁇ 7.5 wt.%, 22.5 ⁇ 5.0 wt.%, or 22.5 ⁇ 2.5 wt.%, each based on the total weight of the metal alloy.
  • the chromium content is in increasing order of preference in the range of 25 ⁇ 22.5 wt.%, 25 ⁇ 20 wt.%, 25 ⁇ 17.5 wt.%, 25 ⁇ 15 wt.%, 25 ⁇ 12.5 wt.%, 25 ⁇ 10 wt.%, 25 ⁇ 7.5 wt.%, 25 ⁇ 5.0 wt.%, or 25 ⁇ 2.5 wt.%, each based on the total weight of the metal alloy.
  • the chromium content is in ascending order of preference in the range of 27.5 ⁇ 25 wt.%, 27.5 ⁇ 22.5 wt.%, 27.5 ⁇ 20 wt.%, 27.5 ⁇ 17.5 wt.%, 27.5 ⁇ 15 wt.%, 27.5 ⁇ 12.5 wt.%, 27.5 ⁇ 10 wt.%, 27.5 ⁇ 7.5 wt.%, 27.5 ⁇ 5.0 wt.%, or
  • the chromium content is in the range of 30 ⁇ 27.5 wt.%, 30 ⁇ 25 wt.%, 30 ⁇ 22.5 wt.%, 30 ⁇ 20 wt.%,
  • the chromium content is in increasing order of preference in the range of 32.5 ⁇ 30 wt.%, 32.5 ⁇ 27.5 wt.%, 32.5 ⁇ 25 wt.%, 32.5 ⁇ 22.5 wt.%, 32.5 ⁇ 20 wt.%, 32.5 ⁇ 17.5 wt.%, 32.5 ⁇ 15 wt.%, 32.5 ⁇ 12.5 wt.%, 32.5 ⁇ 10 wt.%,
  • Preferred embodiments ZI to Z72 have the following nickel and chromium content in wt.%, each based on the total weight of the metal alloy:
  • the metal alloy according to the invention additionally contains cobalt.
  • the total content of nickel and optionally cobalt is at least 20 wt.%, preferably at least 25 wt.%, more preferably at least 30 wt.%, even more preferably at least 35 wt.%, most preferably at least 40 wt.%, and in particular at least 45 wt.%, in each case based on the total weight of the metal alloy.
  • the total content of nickel and optionally cobalt is at least 50% by weight, preferably at least 54% by weight, more preferably at least 58% by weight, even more preferably at least 62% by weight, most preferably at least 66% by weight, and in particular at least 70% by weight, in each case based on the total weight of the metal alloy.
  • the total content of nickel and optionally cobalt is at least 70% by weight, preferably at least 75% by weight, in each case based on the total weight of the metal alloy.
  • the total content of nickel and optionally cobalt is, with increasing preference, in the range of 20 ⁇ 15 wt.%, 20 ⁇ 10 wt.%, or 20 ⁇ 5.0 wt.%, in each case based on the total weight of the metal alloy.
  • the total content of nickel and optionally cobalt is, with increasing preference, in the range of 30 ⁇ 25 wt.%, 30 ⁇ 20 wt.%, 30 ⁇ 15 wt.%, 30 ⁇ 10 wt.%, or 30 ⁇ 5.0 wt.%, in each case based on the total weight of the metal alloy.
  • the total content of nickel and optionally cobalt is in the range of 40 ⁇ 35 wt.%, 40 ⁇ 30 wt.%, 40 ⁇ 25 wt.%, %, 40 ⁇ 20 wt.%, 40 ⁇ 15 wt.%, 40 ⁇ 10 wt.%, or 40 ⁇ 5.0 wt.%, each based on the total weight of the metal alloy.
  • the total content of nickel and optionally cobalt is, with increasing preference, in the range of 50 ⁇ 30 wt.%, 50 ⁇ 25 wt.%, 50 ⁇ 20 wt.%, 50 ⁇ 15 wt.%, 50 ⁇ 10 wt.%, or 50 ⁇ 5.0 wt.%, in each case based on the total weight of the metal alloy.
  • the total content of nickel and optionally cobalt is, with increasing preference, in the range of 60 ⁇ 20 wt.%, 60 ⁇ 15 wt.%, 60 ⁇ 10 wt.%, or 60 ⁇ 5.0 wt.%, in each case based on the total weight of the metal alloy.
  • the total content of nickel and optionally cobalt is, with increasing preference, in the range of 70 ⁇ 10 wt.%, or 70 ⁇ 5.0 wt.%, in each case based on the total weight of the metal alloy.
  • the total content of nickel and optionally cobalt is at most 60 wt.%, preferably at most 55 wt.%, more preferably at most 50 wt.%, even more preferably at most 45 wt.%, most preferably at most 40 wt.%, and in particular at most 35 wt.%, in each case based on the total weight of the metal alloy.
  • total content of nickel and optionally cobalt means that the metal alloy according to the invention either (i) contains both nickel and cobalt, and the total content then refers to the sum of the two individual contents of nickel and cobalt, or (ii) contains no cobalt, so that the total content then refers to the content of nickel alone.
  • the cobalt content is at least 4.0 wt.%, preferably at least 8.0 wt.%, more preferably at least 12 wt.%, even more preferably at least 16 wt.%, most preferably at least 20 wt.%, and in particular at least 24 wt.%, in each case based on the total weight of the metal alloy.
  • the cobalt content is at most 15% by weight, preferably at most 12.5% by weight, more preferably at most 10% by weight, even more preferably at most 7.5% by weight, most preferably at most 5.0% by weight, and in particular at most 2.5% by weight, in each case based on the total weight of the metal alloy.
  • the metal alloy according to the invention contains at most very small amounts of cobalt, preferably at most 1.0 wt.%, more preferably at most 0.5 wt.%, even more preferably at most 0.1 wt.%, most preferably cobalt is nominally not contained.
  • Preferred embodiments Al to ⁇ 72 have the following content of nickel, optionally cobalt and chromium in wt.%, each based on the total weight of the metal alloy:
  • the content of nickel or the total content of nickel and cobalt in the metal alloy according to the invention has an important influence on the solubility of nitrogen and thus on nitridation. As the content of nickel or the total content of nickel and cobalt increases, the solubility of nitrogen in the metal alloy decreases. The lower the solubility of nitrogen, the lower the tendency towards (internal) nitridation.
  • the metal alloy according to the invention can additionally contain aluminum and/or titanium. Even if aluminum and titanium are not preferred per se, it may be advantageous, e.g. for reasons of strength, to use raw materials which may contain comparatively small amounts of aluminum and/or titanium to produce the metal alloy according to the invention. Even if aluminum and titanium are not preferred per se, certain amounts can be tolerated.
  • Both aluminum and titanium are often contained in technical metal alloys, although not always in large quantities, in order to increase mechanical strength and creep resistance. Aluminum can also improve oxidation resistance. Both metals have a pronounced tendency to form nitrides at high temperatures and in contact with nitrogen, particularly in their depth (internal nitriding). It has been found that the depth of internal nitriding of metal alloys containing aluminum and/or titanium is increased compared to metal alloys containing neither aluminum nor titanium. It has also been found that higher chromium contents additionally promote the internal nitriding of aluminum and titanium.
  • the total content of aluminum and/or titanium is at most 5.5 wt.%, preferably at most 5.0 wt.%, more preferably at most 4.5 wt.%, even more preferably at most 4.0 wt.%, most preferably at most 3.5 wt.%, and in particular at most 3.0 wt.%, in each case based on the total weight of the metal alloy.
  • total content of aluminum and/or titanium means that the metal alloy according to the invention either (i) contains both aluminum and titanium, and the total content then refers to the sum of the two individual contents of aluminum and titanium, or (ii) contains no aluminum, so that the total content then refers to the content of titanium alone, or (iii) contains no titanium, so that the total content then refers to the content of aluminum alone.
  • the metal alloy according to the invention contains at most very small amounts of aluminum and/or titanium, preferably at most 1.0 wt.%, more preferably at most 0.5 wt.%, even more preferably at most 0.1 wt.%, most preferably aluminum and titanium are nominally not contained.
  • the metal alloy according to the invention may additionally contain aluminum.
  • the aluminum content is preferably at most 6.0 wt.%, preferably at most 5.5 wt.%, more preferably at most 5.0 wt.%, even more preferably at most 4.5 wt.%, most preferably at most 4.0 wt.%, and in particular at most 3.5 wt.%, in each case based on the total weight of the metal alloy.
  • the aluminum content is preferably at most 3.0 wt.%, preferably at most 2.5 wt.%, more preferably at most 2.0 wt.%, even more preferably at most 1.5 wt.%, most preferably at most 1.0 wt.%, and in particular at most 0.5 wt.%, in each case based on the total weight of the metal alloy.
  • Al2O3 is also very stable, even at low partial pressures of O2.
  • oxide covering layers made of Al2O3 grow even more slowly than oxide covering layers made of C ⁇ CE, since the formation of Al2O3 is kinetically inhibited at comparatively low temperatures.
  • higher contents of aluminum > 5 wt. %) make the weldability of the metal alloy more difficult and there is also a strong tendency to form highly embrittled nitrides.
  • the metal alloy according to the invention contains at most very small amounts of aluminum, preferably at most 1.0 wt.%, more preferably at most 0.5 wt.%, even more preferably at most 0.1 wt.%, most preferably aluminum is nominally not contained.
  • the metal alloy according to the invention may additionally contain titanium.
  • the titanium content is preferably at most 4.5 wt.%, preferably at most 4.0 wt.%, more preferably at most 3.5 wt.%, even more preferably at most 3.0 wt.%, most preferably at most 2.5 wt.%, and in particular at most 2.0 wt.%, in each case based on the total weight of the metal alloy.
  • the metal alloy according to the invention contains at most very small amounts of titanium, preferably at most 1.0 wt.%, more preferably at most 0.6 wt.%, even more preferably at most 0.5 wt.%, most preferably at most 0.1 wt.%, and in particular titanium is nominally not contained.
  • the metal alloy according to the invention additionally contains iron.
  • the metal alloy according to the invention is a steel, preferably an austenitic steel.
  • the iron content is at most 85 wt.%, preferably at most 80 wt.%, more preferably at most 75 wt.%, even more preferably at most 70 wt.%, most preferably at most 65 wt.%, and in particular at most 50 wt.%, in each case based on the total weight of the metal alloy.
  • the iron content is at most 45 wt.%, preferably at most 40 wt.%, more preferably at most 35 wt.%, even more preferably at most 30 wt.%, most preferably at most 25 wt.%, and in particular at most 20 wt.%, in each case based on the total weight of the metal alloy.
  • the iron content is at most 15 wt.%, preferably at most 10 wt.%, more preferably at most 5.0 wt.%, in each case based on the total weight of the metal alloy.
  • the iron content is in the range of 10 ⁇ 5 wt.%, based on the total weight of the metal alloy.
  • the iron content is, with increasing preference, in the range of 20 ⁇ 15 wt.%, 20 ⁇ 10 wt.%, or 20 ⁇ 5.0 wt.%, in each case based on the total weight of the metal alloy.
  • the iron content is in increasing order of preference in the range of 30 ⁇ 25 wt.%, 30 ⁇ 20 wt.%, 30 ⁇ 15 wt.%, 30 ⁇ 10 wt.%, or 30 ⁇ 5.0 wt.%, each based on the total weight of the metal alloy.
  • the iron content is in the range of 40 ⁇ 35 wt.%, 40 ⁇ 30 wt.%, 40 ⁇ 25 wt.%, 40 ⁇ 20 wt.%, 40 ⁇ 15 % by weight, 40 ⁇ 10 % by weight, or 40 ⁇ 5.0 % by weight, each based on the total weight of the metal alloy.
  • the iron content is in increasing order of preference in the range of 50 ⁇ 30 wt.%, 50 ⁇ 25 wt.%, 50 ⁇ 20 wt.%, 50 ⁇ 15 wt.%, 50 ⁇ 10 wt.%, or 50 ⁇ 5.0 wt.%, each based on the total weight of the metal alloy.
  • the iron content is in increasing order of preference in the range of 60 ⁇ 20 wt.%, 60 ⁇ 15 wt.%, 60 ⁇ 10 wt.%, or 60 ⁇ 5.0 wt.%, each based on the total weight of the metal alloy.
  • the iron content is, with increasing preference, in the range of 70 ⁇ 10 wt.%, or 70 ⁇ 5.0 wt.%, in each case based on the total weight of the metal alloy.
  • the metal alloy according to the invention contains at most small amounts of iron, preferably at most 1.5% by weight, more preferably at most 1.0% by weight, even more preferably at most 0.5% by weight, most preferably at most 0.1% by weight, and in particular iron is nominally not contained.
  • the metal alloy according to the invention preferably contains silicon.
  • SiCE is thermodynamically more stable than CnO;.
  • SiC>2 can therefore form on the surface in oxygen-poor atmospheres instead of CnO; and thus hinder nitridation.
  • the silicon content is limited metallurgically. Therefore, a dense SiO2 layer is usually not formed, which reduces the protective effect. If the CnO; is stable, SiO2 can form at the inner phase boundary, which also reduces the tendency to nitride. But here too, the SiO2 layer is usually not continuous or mixed oxides are formed.
  • the silicon content is at least 0.1 wt.%, preferably at least 0.2 wt.%, more preferably at least 0.3 wt.%, even more preferably at least 0.4 wt.%, most preferably at least 0.5 wt.%, and in particular at least 0.6 wt.%, in each case based on the total weight of the metal alloy.
  • the silicon content is at most 4.0 wt.%, preferably at most 3.5 wt.%, more preferably at most 3.0 wt.%, even more preferably at most 2.5 wt.%, most preferably at most 2.0 wt.%, and in particular at most 1.5 wt.%, in each case based on the total weight of the metal alloy.
  • the metal alloy according to the invention preferably contains carbon.
  • the carbon content is at least 0.010 wt.%, preferably at least 0.020 wt.%, more preferably at least 0.030 wt.%, even more preferably at least 0.040 wt.%, most preferably at least 0.050 wt.%, and in particular at least 0.060 wt.%, in each case based on the total weight of the metal alloy.
  • the carbon content is in the range of 0.1 to 0.5% by weight, based on the total weight of the metal alloy. This is preferably the case in particular with cast alloys.
  • the carbon content is at most 0.10 wt.%, preferably at most 0.09 wt.%, more preferably at most 0.08 wt.%, even more preferably at most 0.07 wt.%, most preferably at most 0.06 wt.%, and in particular at most 0.05 wt.%, in each case based on the total weight of the metal alloy.
  • iron-based alloys In iron-based alloys, atomic hydrogen can react with carbides such as iron carbide to form methane.
  • carbides such as iron carbide
  • Low-alloyed chromium and chromium-molybdenum steels become increasingly more stable against this form of high-temperature embrittlement (HTHA) with increasing Cr content, since chromium carbides are significantly more stable than iron carbide.
  • Austenitic steels and nickel-based alloys are therefore highly resistant to high-temperature embrittlement.
  • nickel-based alloys can become embrittled due to hydrogen "trapping" on chromium carbides during thermal aging.
  • the metal alloy according to the invention preferably contains molybdenum.
  • the molybdenum content is at least 0.1 wt.%, preferably at least 0.2 wt.%, more preferably at least 0.3 wt.%, even more preferably at least 0.4 wt.%, most preferably at least 0.5 wt.%, and in particular at least 0.6 wt.%, in each case based on the total weight of the metal alloy.
  • the metal alloy contains molybdenum and the molybdenum content is at least 1.0 wt.%, preferably at least 2.0 wt.%, more preferably at least 3.0 wt.%, even more preferably at least 4.0 wt.%, most preferably at least 5.0 wt.%, and in particular at least 6.0 wt.%, in each case based on the total weight of the metal alloy.
  • the molybdenum content is at most 12 wt.%, preferably at most 11 wt.%, more preferably at most 10 wt.%, even more preferably at most 9.0 wt.%, most preferably at most 8.0 wt.%, and in particular at most 7.0 wt.%, in each case based on the total weight of the metal alloy.
  • the molybdenum content is at most 4.0 wt.%, preferably at most 3.5 wt.%, more preferably at most 3.0 wt.%, even more preferably at most 2.5 wt.%, most preferably at most 2.0 wt.%, and in particular at most 1.5 wt.%, each based on the total weight of the metal alloy.
  • the metal alloy according to the invention contains at most very small amounts of molybdenum, preferably at most 1.0 wt.%, more preferably at most 0.5 wt.%, even more preferably at most 0.1 wt.%, most preferably molybdenum is nominally not contained.
  • the metal alloy contains molybdenum and the total content of nickel, chromium and molybdenum is at most 85 wt.%, preferably at most 80 wt.%, more preferably at most 75 wt.%, even more preferably at most 70 wt.%, most preferably at most 65 wt.%, and in particular at most 60 wt.%, in each case based on the total weight of the metal alloy.
  • the metal alloy according to the invention preferably contains vanadium.
  • the content of vanadium is at least 0.1 wt.%, preferably at least 0.2 wt.%, more preferably at least 0.3 wt.%, even more preferably at least 0.4 wt.%, most preferably at least 0.5 wt.%, and in particular at least 0.6 wt.%, in each case based on the total weight of the metal alloy.
  • the content of vanadium is at most 4.0 wt.%, preferably at most 3.5 wt.%, more preferably at most 3.0 wt.%, even more preferably at most 2.5 wt.%, most preferably at most 2.0 wt.%, and in particular at most 1.5 wt.%, in each case based on the total weight of the metal alloy.
  • the metal alloy according to the invention contains at most very small amounts of vanadium, preferably at most 1.0 wt.%, more preferably at most 0.5 wt.%, even more preferably at most 0.1 wt.%, most preferably vanadium is nominally not contained.
  • the metal alloy according to the invention preferably contains manganese.
  • the manganese content is at least 0.1 wt.%, preferably at least 0.2 wt.%, more preferably at least 0.3 wt.%, even more preferably at least 0.4 wt.%, most preferably at least 0.5 wt.%, and in particular at least 0.6 wt.%, in each case based on the total weight of the metal alloy.
  • the manganese content is at most 4.0 wt.%, preferably at most 3.5 wt.%, more preferably at most 3.0 wt.%, even more preferably at most 2.5 wt.%, most preferably at most 2.0 wt.%, and in particular at most 1.5 wt.%, in each case based on the total weight of the metal alloy.
  • the metal alloy according to the invention contains at most very small amounts of manganese, preferably at most 1.0 wt.%, more preferably at most 0.5 wt.%, even more preferably at most 0.2 wt.%, most preferably manganese is nominally not contained.
  • the metal alloy according to the invention preferably contains zirconium.
  • the zirconium content is at least 0.1 wt.%, preferably at least 0.2 wt.%, more preferably at least 0.3 wt.%, even more preferably at least 0.4 wt.%, most preferably at least 0.5 wt.%, and in particular at least 0.6 wt.%, in each case based on the total weight of the metal alloy.
  • the zirconium content is at most 4.0 wt.%, preferably at most 3.5 wt.%, more preferably at most 3.0 wt.%, even more preferably at most 2.5 wt.%, most preferably at most 2.0 wt.%, and in particular at most 1.5 wt.%, in each case based on the total weight of the metal alloy.
  • the metal alloy according to the invention contains at most very small amounts of zirconium, preferably at most 1.0 wt.%, more preferably at most 0.5 wt.%, even more preferably at most 0.1 wt.%, most preferably zirconium is nominally not contained.
  • the metal alloy according to the invention preferably contains copper.
  • the copper content is at least 0.1 wt.%, preferably at least 0.2 wt.%, more preferably at least 0.3 wt.%, even more preferably at least 0.4 wt.%, most preferably at least 0.5 wt.%, and in particular at least 0.6 wt.%, in each case based on the total weight of the metal alloy.
  • the copper content is at most 4.0 wt.%, preferably at most 3.5 wt.%, more preferably at most 3.0 wt.%, even more preferably at most 2.5 wt.%, most preferably at most 2.0 wt.%, and in particular at most 1.5 wt.%, in each case based on the total weight of the metal alloy.
  • the metal alloy according to the invention contains at most very small amounts of copper, preferably at most 1.0 wt.%, more preferably at most 0.5 wt.%, even more preferably at most 0.1 wt.%, most preferably copper is nominally not contained.
  • the metal alloy according to the invention preferably contains niobium.
  • the content of niobium is at least 0.1 wt.%, preferably at least 0.2 wt.%, more preferably at least 0.3 wt.%, even more preferably at least 0.4 wt.%, most preferably at least 0.5 wt.%, and in particular at least 0.6 wt.%, in each case based on the total weight of the metal alloy.
  • the content of niobium is at most 5.5 wt.%, preferably at most 5.0 wt.%, more preferably at most 4.5 wt.%, even more preferably at most 4.0 wt.%, most preferably at most 3.5 wt.%, and in particular at most 3.0 wt.%, in each case based on the total weight of the metal alloy.
  • the metal alloy according to the invention contains at most very small amounts of niobium, preferably at most 1.5 wt.%, more preferably at most 1.0 wt.%, even more preferably 0.5 wt.%, even more preferably at most 0.1 wt.%, most preferably niobium is nominally not contained.
  • the metal alloy according to the invention preferably contains tungsten.
  • the tungsten content is at least 0.1 wt.%, preferably at least 0.2 wt.%, more preferably at least 0.3 wt.%, even more preferably at least 0.4 wt.%, most preferably at least 0.5 wt.%, and in particular at least 0.6 wt.%, in each case based on the total weight of the metal alloy.
  • the metal alloy contains tungsten and the tungsten content is at least 1.0 wt.%, preferably at least 2.0 wt.%, more preferably at least 3.0 wt.%, even more preferably at least 4.0 wt.%, most preferably at least 5.0 wt.%, and in particular at least 6.0 wt.%, in each case based on the total weight of the metal alloy.
  • the tungsten content is at most 20 wt.%, preferably at most 19 wt.%, more preferably at most 18 wt.%, even more preferably at most 17 wt.%, most preferably at most 16 wt.%, and in particular at most 15 wt.%, in each case based on the total weight of the metal alloy.
  • the tungsten content is at most 5.0 wt.%, preferably at most 4.0 wt.%, more preferably at most 3.0 wt.%, even more preferably at most 2.5 wt.%, most preferably at most 2.0 wt.%, and in particular at most 1.5 wt.%, in each case based on the total weight of the metal alloy.
  • the metal alloy according to the invention contains at most very small amounts of tungsten, preferably at most 1.0 wt.%, more preferably at most 0.5 % by weight, more preferably at most 0.1 % by weight, most preferably tungsten is nominally not included.
  • the metal alloy contains tungsten and the total content of nickel, chromium and tungsten is at most 95 wt.%, preferably at most 90 wt.%, more preferably at most 85 wt.%, even more preferably at most 80 wt.%, most preferably at most 75 wt.%, and in particular at most 70 wt.%, in each case based on the total weight of the metal alloy.
  • the metal alloy according to the invention preferably contains molybdenum and tungsten.
  • the metal alloy contains molybdenum and tungsten and the total content of nickel, chromium, molybdenum and tungsten is at most 95 wt. %, preferably at most 90 wt. %, more preferably at most 85 wt. %, even more preferably at most 80 wt. %, most preferably at most 75 wt. %, and in particular at most 70 wt. %, in each case based on the total weight of the metal alloy.
  • the content of ⁇ [(molybdenum content) + 0.5 x (tungsten content)] ⁇ is less than 1.5 wt.%.
  • the content of ⁇ [(content of molybdenum) + 0.5 x (content of tungsten)] ⁇ is at most 1.4 wt. %, preferably at most 1.2 wt. %, more preferably at most 1.0 wt. %, even more preferably at most 0.8 wt. %, most preferably at most 0.6 wt. %, and in particular at most 0.4 wt. %, in each case based on the total weight of the metal alloy.
  • the content of ⁇ [(molybdenum content) + 0.5 x (tungsten content)] ⁇ is more than 8.5 wt.%.
  • the content of ⁇ [(content of molybdenum) + 0.5 x (content of tungsten)] ⁇ is at least 8.6 wt.%, preferably at least 8.8 wt.%, more preferably at least 9.0 wt.%, even more preferably at least 10 wt.%, most preferably at least 13 wt.%, and in particular at least 16 wt.%, in each case based on the total weight of the metal alloy.
  • the content of (1.8 x chromium / ⁇ [(molybdenum content) + 0.5 x (tungsten content)] ⁇ ) is less than 3.0 wt.%.
  • the content of (1.8 x chromium / ⁇ [(content of molybdenum) + 0.5 x (content of tungsten)] ⁇ ) is at most 2.9 wt. %, preferably at most 2.6 wt. %, more preferably at most 2.3 wt. %, even more preferably at most 2.0 wt. %, most preferably at most 1.7 wt. %, and in particular at most 1.4 wt. %, in each case based on the total weight of the metal alloy.
  • the content of (1.8 x chromium / ⁇ [(content of molybdenum) + 0.5 x (content of tungsten)] ⁇ ) is more than 10 wt.%.
  • the content of (1.8 x chromium / ⁇ [(content of molybdenum) + 0.5 x (content of tungsten)] ⁇ ) is at least 30 wt.%, preferably at least 50 wt.%, more preferably at least 70 wt.%, even more preferably at least 75 wt.%, most preferably at least 80 wt.%, and in particular at least 85 wt.%, in each case based on the total weight of the metal alloy.
  • the metal alloy according to the invention preferably contains a rare earth metal, preferably selected from the group consisting of scandium, lanthanum, cerium, praseodymium, neodymium, promethium, samarium, europium, yttrium, gadolinium, terbium, dysprosium, holmium, erbium, thulium, ytterbium and lutetium; more preferably scandium, lanthanum, cerium, neodymium and yttrium. It has been found that rare earths (in particular cerium and yttrium) can improve the adhesion of the nitride in the case of external nitriding (low oxygen partial pressure).
  • the total content of rare earth metals is at least 0.01 wt.%, preferably at least 0.02 wt.%, more preferably at least 0.03 wt.%, even more preferably at least 0.04 wt.%, most preferably at least 0.05 wt.%, and in particular at least 0.06 wt.%, in each case based on the total weight of the metal alloy.
  • the total content of rare earth metals is at most 0.6 wt.%, preferably at most 0.5 wt.%, more preferably at most 0.4 wt.%, even more preferably at most 0.3 wt.%, most preferably at most 0.2 wt.%, and in particular at most 0.1 wt.%, in each case based on the total weight of the metal alloy.
  • the metal alloy according to the invention contains at most very small amounts of rare earth metals, preferably at most 0.10 wt.%, more preferably at most 0.09 wt.%, even more preferably at most 0.08 wt.%, most preferably rare earth metals are nominally not contained.
  • the metal alloy according to the invention preferably contains cerium.
  • the cerium content is at least 0.01 wt.%, preferably at least 0.02 wt.%, more preferably at least 0.03 wt.%, even more preferably at least 0.04 wt.%, most preferably at least 0.05 wt.%, and in particular at least 0.06 wt.%, in each case based on the total weight of the metal alloy.
  • the cerium content is at most 0.6 wt.%, preferably at most 0.5 wt.%, more preferably at most 0.4 wt.%, even more preferably at most 0.3 wt.%, most preferably at most 0.2 wt.%, and in particular at most 0.1 wt.%, each based on the total weight of the metal alloy.
  • the metal alloy according to the invention contains at most very small amounts of cerium, preferably at most 1.0 wt.%, more preferably at most 0.5 wt.%, even more preferably at most 0.1 wt.%, most preferably cerium is nominally not contained.
  • the metal alloy according to the invention preferably contains yttrium.
  • the yttrium content is at least 0.01 wt.%, preferably at least 0.02 wt.%, more preferably at least 0.03 wt.%, even more preferably at least 0.04 wt.%, most preferably at least 0.05 wt.%, and in particular at least 0.06 wt.%, in each case based on the total weight of the metal alloy.
  • the yttrium content is at most 0.6 wt.%, preferably at most 0.5 wt.%, more preferably at most 0.4 wt.%, even more preferably at most 0.3 wt.%, most preferably at most 0.2 wt.%, and in particular at most 0.1 wt.%, in each case based on the total weight of the metal alloy.
  • the metal alloy according to the invention contains at most very small amounts of yttrium, preferably at most 0.10 wt.%, more preferably at most 0.09 wt.%, even more preferably at most 0.08 wt.%, most preferably yttrium is nominally not contained.
  • the metal alloy according to the invention preferably contains lanthanum.
  • the content of lanthanum is at least 0.01 wt.%, preferably at least 0.02 wt.%, more preferably at least 0.03 wt.%, even more preferably at least 0.04 wt.%, most preferably at least 0.05 wt.%, and in particular at least 0.06 wt.%, in each case based on the total weight of the metal alloy.
  • the content of lanthanum is at most 0.6 wt.%, preferably at most 0.5 wt.%, more preferably at most 0.4 wt.%, even more preferably at most 0.3 wt.%, most preferably at most 0.2 wt.%, and in particular at most 0.15 wt.%, in each case based on the total weight of the metal alloy.
  • the metal alloy according to the invention contains at most very small amounts of lanthanum, preferably at most 0.10 wt.%, more preferably at most 0.09 wt.%, even more preferably at most 0.08 wt.%, most preferably lanthanum is nominally not contained.
  • the metal alloy according to the invention preferably contains boron.
  • the boron content is at least 0.1 wt.%, preferably at least 0.2 wt.%, more preferably at least 0.3 wt.%, even more preferably at least 0.4 wt.%, most preferably at least 0.5 wt.%, and in particular at least 0.6 wt.%, in each case based on the total weight of the metal alloy.
  • the boron content is at most 4.0 wt.%, preferably at most 3.5 wt.%, more preferably at most 3.0 wt.%, even more preferably at most 2.5 wt.%, most preferably at most 2.0 wt.%, and in particular at most 1.5 wt.%, in each case based on the total weight of the metal alloy.
  • the metal alloy according to the invention contains at most very small amounts of boron, preferably at most 0.1% by weight, more preferably at most 0.01% by weight, even more preferably at most 0.001% by weight, most preferably boron is nominally not contained.
  • the total content of aluminium and/or titanium does not exceed 2.1% by weight, based on the total weight of the metal alloy.
  • the chromium content is at least 26% by weight, based on the total weight of the metal alloy.
  • the chromium content is in the range of 15 to 35 wt.%
  • the aluminium content does not exceed 2.5% by weight
  • the titanium content does not exceed 0.6% by weight, based on the total weight of the metal alloy.
  • the chromium content is in the range of 19 to 35 wt.%
  • the aluminium content does not exceed 2.5% by weight
  • the titanium content does not exceed 0.6% by weight, each based on the total weight of the metal alloy.
  • the metal alloy is selected from the group consisting of metal alloys Al to A 12, Bl to Bl 7, CI to CI 7, Dl to D17, or El to El 7, which each contain the following content of chromium and nickel in wt.% based on the total weight of the metal alloy, wherein further components not listed in the tables may be included:
  • the metal alloy is selected from the group consisting of metal alloys Fl to Fl 2, Gl to Gl 7, Hl to Hl 7, II to 117, or J1 to J17, which each contain the following content of iron, chromium and nickel in % by weight based on the total weight of the metal alloy, wherein further components not listed in the tables may be included:
  • the metal alloy is selected from the group consisting of metal alloys K1 to K12, LI to L17, M1 to M17, NI to N17, or 01 to 017, which each contain the following content of chromium, nickel and optionally cobalt in wt.% based on the total weight of the metal alloy, wherein further components not listed in the tables may be included:
  • the metal alloy is selected from the group consisting of metal alloys PI to P12, Ql to Q17, RI to R17, S1 to S17, or TI to T17, which each contain the following content of optionally iron, chromium, nickel and optionally cobalt in wt.% based on the total weight of the metal alloy, wherein in each case further constituents not listed in the tables may be included:
  • the metal alloy is selected from the group consisting of metal alloys Ul to Ul 2, VI to VI 7, W1 to W 17, XI to XI 7, or Y1 to Y17, which each contain the following content of iron, chromium, nickel, cobalt, aluminum and titanium in % by weight based on the total weight of the metal alloy, wherein further components not listed in the tables may be included:
  • the metal alloy according to the invention is selected from the group consisting of materials according to DIN/EN X9CrNiSiNCe21-1 l-2, X8CrNiNbl6-13, X12CrNi25-21, X10NiCrAlTi32-20, X5NiCrAlTi31-20, X12NiCrSi35-16, 35Ni25Crl.5SiCeN, NiFe30Cr21Mo3, NiCr23Col2Mo, NiMol6Crl5Fe6W4, NiCr22W14Mo, NiCr23Fel5Al, NiCr25FeAlY,
  • NiCr22Mo9Nb, and NiCrl5Fe are NiCr22Mo9Nb, and NiCrl5Fe.
  • the metal alloy according to the invention is selected from the group consisting of materials according to material class DIN No. 1.4820, 1.4821, 1.4822, 1.4823, 1.4824, 1.4825, 1.4826, 1.4827, 1.4828, 1.4829, 1.4830, 1.4831, 1.4832, 1.4833, 1.4834, 1.4835, 1.4836, 1.4837, 1.4838,
  • the metal alloy according to the invention is selected from the group consisting of materials according to material class DIN No. 1.4948, 1.4949, 1.4950, 1.4951, 1.4952, 1.4953, 1.4954, 1.4955, 1.4956, 1.4957, 1.4958, 1.4959, 1.4960, 1.4961, 1.4962, 1.4963, 1.4964, 1.4965, 1.4966, 1.4967, 1.4968, 1.4969, 1.4970, and 1.4971.
  • the metal alloy according to the invention is selected from the group consisting of materials according to material class DIN No. 2.4630, 2.4633, 2.4650, 2.4653, 2.4654, 2.4655, 2.4656, 2.4657, 2.4658, 2.4659, 2.4660, 2.4661, 2.4662, 2.4663, 2.4664, 2.4665, 2.4666, 2.4667, 2.4668, 2.4669, 2.4670, 2.4671, 2.4672, and 2.4673.
  • the metal alloy according to the invention is selected from the group consisting of materials according to material class DIN No. 2.4723, 2.4724, 2.4725, 2.4726, 2.4727, 2.4728, 2.4729, 2.4730, 2.4731, 2.4732, 2.4733, 2.4734, 2.4735, 2.4736, 2.4737, 2.4738, 2.4739, 2.4740, 2.4741, 2.4742, and 2.4743.
  • the metal alloy according to the invention is selected from the group consisting of materials according to material class DIN No. 2.4806, 2.4807, 2.4808, 2.4809, 2.4810, 2.4811, 2.4812, 2.4813, 2.4814, 2.4815, 2.4816, 2.4817, 2.4818, 2.4819, 2.4820, 2.4821, 2.4822, 2.4823, 2.4824,
  • the metal alloy comes into direct contact with gaseous NH;.
  • the metal alloy does not come into direct contact with NH; in the supercritical state.
  • a further aspect of the invention relates to a process for the catalytic decomposition of NH3 to N2 and H2 in a plant according to the invention as described above, wherein the NH3 is introduced into the reactor at a temperature of at least 500°C, more preferably at least 530°C, even more preferably at least 560°C, most preferably at least 590°C, and in particular at least 620°C.
  • the component is exposed to a temperature of at least 500°C, more preferably at least 530°C, even more preferably at least 560°C, most preferably at least 590°C, and in particular at least 620°C.
  • the component is exposed to a temperature of at least 650°C, more preferably at least 680°C, even more preferably at least 710°C, most preferably at least 740°C, and in particular at least 770°C.
  • the component is exposed to a temperature of at least 800°C, more preferably at least 830°C, even more preferably at least 860°C, most preferably at least 890°C, and in particular at least 920°C.
  • the NH3 is present in the reactor in gaseous state.
  • the NH3 in the reactor is not in a supercritical state.
  • FIG. 1 schematically illustrates a preferred embodiment of a reactor 1 according to the invention, which comprises, for example, four tubular reaction chambers 2, each of which contains NH3 decomposition catalyst.
  • the reactor 1 forms a combustion chamber 3 in its interior, in which the four tubular reaction chambers 2 are arranged in parallel as a bundle.
  • NH3 reactant gas
  • the product gas which comprises N2 and H2, is discharged from the reaction chambers 2 and the reactor 1 via discharge system 5.
  • combustion gas is fed via feed line 6 into the combustion chamber 3, where it is burned to form flame 7.
  • Combustion heat generated during combustion flows from the interior of the combustion chamber 3 through the walls of the reaction chambers 2 to the NFfi decomposition catalyst.
  • the flue gas generated during combustion is discharged from the combustion chamber 3 and the reactor 1 via discharge line 8.

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Abstract

L'invention concerne des réacteurs et des éléments de réacteurs qui présentent une bonne résistance vis-à-vis des composés NH3 et N2 et éventuellement H2O à des températures élevées et à une pression moyenne, de sorte qu'ils puissent être utilisés pour la décomposition catalytique de NH3 en N2 et H2 à l'échelle industrielle.
PCT/EP2024/065354 2023-06-05 2024-06-04 Réacteurs servant à la décomposition de nh3 à hautes températures Ceased WO2024251744A1 (fr)

Priority Applications (4)

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JP2025570650A JP2026524761A (ja) 2023-06-05 2024-06-04 高温でｎｈ３を分解するための反応器
KR1020257040274A KR20260005380A (ko) 2023-06-05 2024-06-04 고온에서 nh3를 분해하기 위한 반응기
EP24731874.4A EP4719640A1 (fr) 2023-06-05 2024-06-04 Réacteurs servant à la décomposition de nhà hautes températures
CN202480038060.4A CN121335750A (zh) 2023-06-05 2024-06-04 用于在高温下分解nh3的反应器

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LU103141A LU103141B1 (de) 2023-06-05 2023-06-05 Reaktoren und Reaktorbauteile zur Zersetzung von NH3 bei hohen Temperaturen
LULU103141 2023-06-05
DE102023114700.5 2023-06-05
DE102023114700.5A DE102023114700A1 (de) 2023-06-05 2023-06-05 Reaktoren und Reaktorbauteile zur Zersetzung von NH3 bei hohen Temperaturen

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CN121335750A (zh) 2026-01-13

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