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WO2025021701A1 - Procédé de capture d'un métal noble, en particulier du rhodium et/ou du platine, perdu par volatilisation d'un catalyseur en un flux gazeux fortement chauffé à l'aide d'un oxyde de formule a2o3 - Google Patents

Procédé de capture d'un métal noble, en particulier du rhodium et/ou du platine, perdu par volatilisation d'un catalyseur en un flux gazeux fortement chauffé à l'aide d'un oxyde de formule a2o3 Download PDF

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Publication number
WO2025021701A1
WO2025021701A1 PCT/EP2024/070600 EP2024070600W WO2025021701A1 WO 2025021701 A1 WO2025021701 A1 WO 2025021701A1 EP 2024070600 W EP2024070600 W EP 2024070600W WO 2025021701 A1 WO2025021701 A1 WO 2025021701A1
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WIPO (PCT)
Prior art keywords
oxide
platinum
noble metal
rhodium
capture
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Pending
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PCT/EP2024/070600
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English (en)
Inventor
Anja Olafsen SJÅSTAD
Helmer FJELLVÅG
Asbjørn Slagtern FJELLVÅG
Julie HESSEVIK
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
KARasmussen
Oslo Uio, University of
Yara International ASA
Original Assignee
KARasmussen
Oslo Uio, University of
Yara International ASA
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Publication of WO2025021701A1 publication Critical patent/WO2025021701A1/fr
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Anticipated expiration legal-status Critical

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Classifications

    • C—CHEMISTRY; METALLURGY
    • C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22B—PRODUCTION AND REFINING OF METALS; PRETREATMENT OF RAW MATERIALS
    • C22B11/00—Obtaining noble metals
    • C22B11/02—Obtaining noble metals by dry processes
    • 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
    • B01J23/38—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals
    • B01J23/40—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals of the platinum group metals
    • 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
    • B01J23/90—Regeneration or reactivation
    • B01J23/96—Regeneration or reactivation of catalysts comprising metals, oxides or hydroxides of the noble metals
    • 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
    • B01J38/00—Regeneration or reactivation of catalysts, in general
    • B01J38/02—Heat treatment
    • 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
    • B01J38/00—Regeneration or reactivation of catalysts, in general
    • B01J38/48—Liquid treating or treating in liquid phase, e.g. dissolved or suspended
    • B01J38/64—Liquid treating or treating in liquid phase, e.g. dissolved or suspended using alkaline material; using salts
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B21/00—Nitrogen; Compounds thereof
    • C01B21/20—Nitrogen oxides; Oxyacids of nitrogen; Salts thereof
    • C01B21/24—Nitric oxide (NO)
    • C01B21/26—Preparation by catalytic or non-catalytic oxidation of ammonia
    • C—CHEMISTRY; METALLURGY
    • C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22B—PRODUCTION AND REFINING OF METALS; PRETREATMENT OF RAW MATERIALS
    • C22B11/00—Obtaining noble metals
    • C22B11/02—Obtaining noble metals by dry processes
    • C22B11/021—Recovery of noble metals from waste materials
    • C22B11/026—Recovery of noble metals from waste materials from spent catalysts
    • C22B11/028—Recovery of noble metals from waste materials from spent catalysts using solid sorbents, e.g. getters or catchment gauzes
    • C—CHEMISTRY; METALLURGY
    • C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22B—PRODUCTION AND REFINING OF METALS; PRETREATMENT OF RAW MATERIALS
    • C22B7/00—Working up raw materials other than ores, e.g. scrap, to produce non-ferrous metals and compounds thereof; Methods of a general interest or applied to the winning of more than two metals
    • C22B7/009—General processes for recovering metals or metallic compounds from spent catalysts

Definitions

  • the present invention relates to a process for the capture of a noble metal, especially of rhodium and/or platinum, lost by volatilization from a catalyst to a high heated gas stream (including local heating due to a highly exothermic reaction) by contacting the highly heated gas stream containing the volatilized noble metal with a first oxide element comprising an oxide of formula A2O3, especially Nd20s, as well as the use of an oxide of formula A2O3, especially Nd20s for capture of such a noble metal or catchment devices comprising an oxide of formula A2O3, especially Nd2Os.
  • This process is especially useful in relation to the industrial processes like the Ostwald process (showing a highly exothermic reaction) where a catalyst containing rhodium and platinum is used. In selected circumstances these oxides may also act on the decomposition of unwanted N2O arising in said Ostwald process.
  • N2O nitrous oxide
  • Pt and Rh are lost as PtO2 and RhO2 into the gas phase, with Pt being the dominating loss.
  • metal loss causes the largest costs in the production of nitric acid. Capturing and recycling of the precious metals is therefore a key problem that needs to be solved.
  • the most common technology used today is woven Pd-Ni (95:5 wt%) catchment gauzes installed downstream of the Pt-Rh catalyst gauzes; capturing the formed gaseous PtO2 and incorporate Pt into the Pd based alloy.
  • Pd-Ni catchment system Complete reconstruction of the Pd-Ni wire give rise to swelling and significant blockage of the gauzes; which in turn creates an undesired pressure drop.
  • Pd is lost into gas phase, affecting the cost-benefit of the process.
  • the present invention discloses a process for the capture of a noble metal, selected from rhodium or platinum or both, lost by volatilization from a catalyst to a high heated gas stream by contacting the highly heated gas stream containing the volatilized noble metal with a first oxide element comprising an oxide of formula A2O3, especially Nd20s, as well as the use of an oxide of formula A2O3, especially Nd20s, for capture of such a noble metal or catchment devices comprising an oxide of formula A2O3, especially Nd20s,.
  • the invention is directed in a main aspect to a process for the capture of at least one noble metal being selected from rhodium and platinum lost by volatilization from a catalyst comprising the at least one noble metal to a high heater gas stream contacted therewith in a high temperature gas reaction carried out at temperatures of at least 700°C which comprises contacting such highly heated gas stream, after its contact with such catalyst, which contains the volatilized at least one noble metal while such volatilized noble metal is still essentially in the vapor phase and at a temperature of at least 700 °C with a first oxide element comprising at least one oxide selected from an oxide of formula A2O3 with A being selected from rare earth elements/lanthanoids, optionally with one or more elements on A position in form of a solid solution.
  • the invention is based on the surprising effect that the oxides of formula A2O3, especially Nd2C>3, are/is able to highly effectively capture platinum or rhodium, especially both, if these noble metals are mobilized/volatilized by the high temperature gas reaction from a catalyst.
  • the inventors have seen this in their experiments showing a clear advantage over CaO - known from the art to capture platinum.
  • the inventors have found that the use of Nd2C>3 in this process was able to capture both platinum and rhodium and furthermore especially platinum to a much larger extent than seen in the art (CaO).
  • FIGURES are a diagrammatic representation of FIGURES.
  • Fig. 1 shows the result of a 26 days experiment for the catchment of platinum and rhodium (starting with 10 wt.% Rh) in a 5- zone furnace at 700, 800 and 900°C with CaO, showing the respective relations of the detected metals Ca, Pt, and Rh at the various temperatures (see Example 1 ).
  • Fig. 2 shows 2 different views of the results of a 26 days experiment for the catchment of platinum and rhodium (starting with 10 wt.% Rh) in a 5- zone furnace at 700, 800 and 900°C with Nd2C>3, showing the respective relations of the detected metals Nd, Pt, and Rh at the various temperatures (see Example 1 ).
  • Fig. 3 shows the results of two 26 days experiment for the catchment of a) platinum and rhodium and b) platinum alone in a 5- zone furnace at 700, 800 and 900°C with Nd2Os, showing the respective relations of the detected metals Nd, Pt (and Rh) at the various temperatures (see Example 4).
  • the invention relates to a process for the capture of at least one noble metal being selected from rhodium and platinum lost by volatilization from a catalyst comprising the at least one noble metal to a high heater gas stream contacted therewith in a high temperature gas reaction carried out at temperatures of at least 700°C which comprises contacting such highly heated gas stream, after its contact with such catalyst, which contains the volatilized at least one noble metal while such volatilized noble metal is still essentially in the vapor phase and at a temperature of at least 700 °C with a first oxide element comprising at least one oxide selected from
  • the invention is based on the surprising effect that these oxides (of formula A2O3), especially Nd20s, are/is highly effective in capturing platinum - if mobilized by the high temperature gas reaction from a catalyst - but that it is also able to highly effectively capture rhodium. This is especially true if seen on the experiments of EXAMPLE 1.
  • said oxide is an oxide of formula A2O3 with A being selected from La, Ce, Pr, Nd, Pm, Sm, Eu and Gd; or from La, Nd, Pm, Sm, Eu and Gd; or from La, Ce, Pr, Nd, Pm, Sm, Eu and Gd; preferably from La, Nd and Gd, more preferably from La and Nd; especially wherein said oxide is selected from Nd20s, La2Os, and Gd2Os, preferably from Nd20s and Gd2Os; most preferably wherein said oxide is Nd20s.
  • the invention relates to a process for the capture of at least one noble metal being selected from rhodium and platinum lost by volatilization from a catalyst comprising the at least one noble metal to a high heater gas stream contacted therewith in a high temperature gas reaction carried out at temperatures of at least 700°C, wherein the catalytic reaction of the high temperature gas reaction is a catalytic ammonia oxidation or catalytic ammonia combustion, which comprises contacting such highly heated gas stream, after its contact with such catalyst, which contains the volatilized at least one noble metal while such volatilized noble metal is still essentially in the vapor phase and at a temperature of at least 700 °C with a first oxide element comprising at least one oxide selected from an oxide of formula A2O3 with A being selected from Nd and Gd.
  • a SUB-ASPECT A1) of ASPECT A) it is preferred if the at least one oxide is selected from an oxide of formula A2O3 with A being Nd.
  • SUB-ASPECT A2) of ASPECT A) it is preferred if the at least one oxide is selected from an oxide of formula A2O3 with A being Gd.
  • the invention relates to a process for the capture of at least one noble metal being selected from rhodium and platinum lost by volatilization from a catalyst comprising the at least one noble metal to a high heater gas stream contacted therewith in a high temperature gas reaction carried out at temperatures of at least 700°C, wherein the catalytic reaction of the high temperature gas reaction is a catalytic ammonia oxidation or catalytic ammonia combustion, which comprises contacting such highly heated gas stream, after its contact with such catalyst, which contains the volatilized at least one noble metal while such volatilized noble metal is still essentially in the vapor phase and at a temperature of at least 700 °C with a first oxide element comprising at least one oxide selected from an oxide of formula A2O3 with A being selected from Pm, Sm and Eu.
  • the at least one oxide is selected from an oxide of formula A2O3 with A being Pm.
  • the at least one oxide is selected from an oxide of formula A2O3 with A being Sm.
  • the at least one oxide is selected from an oxide of formula A2O3 with A being Eu.
  • the invention relates to a process for the capture of at least one noble metal being selected from rhodium and platinum lost by volatilization from a catalyst comprising the at least one noble metal to a high heater gas stream contacted therewith in a high temperature gas reaction carried out at temperatures of at least 700°C, wherein the catalytic reaction of the high temperature gas reaction is a catalytic ammonia oxidation or catalytic ammonia combustion, which comprises contacting such highly heated gas stream, after its contact with such catalyst, which contains the volatilized at least one noble metal while such volatilized noble metal is still essentially in the vapor phase and at a temperature of at least 700 °C with a first oxide element comprising at least one oxide selected from an oxide of formula A2O3 with A being La.
  • said highly heated gas stream in addition to contacting said first oxide element is further also contacting a metallic element comprising a metallic material selected from the group consisting of palladium, and palladium alloys, more specifically palladium-nickel alloys and palladiumgold alloys.
  • This preferred embodiment of the invention carries the additional advantage that it is based on the selection of combining a metal element such as the Pd/Ni catchment device and the oxide This is a very advantageous combination as the Pd/Ni catchment device captures platinum and the first oxide element with Nd20s helps capturing also rhodium.
  • the highly heated gas stream after its contact with said catalyst is contacted with said first oxide element at a temperature at around or above 900 °C (or at 850°C to 950°C).
  • This specific embodiment of the invention is further based on the surprising finding that a higher rhodium capture on the oxide of formula A2O3, especially Nd20s, seems to be connected to a higher temperature. This more pronounced capture of rhodium with these higher temperatures at around 900°C can be seen in Example 1. Thus, the Nd20s does more pronouncedly capture the rhodium, while the metal element would capture the platinum.
  • the process of the invention (especially according to ASPECT A) and its SUB-ASPECTS, but also ASPECTS B) and C ⁇ ) there is no further oxide element, comprising metal oxides, and/or no further N2O-decomposition catalyst used in the process; and/or the first oxide element comprises only one metal oxide.
  • this feature applies especially (as one example) if the at least one oxide is selected from an oxide of formula A2O3 with A being Gd.
  • the process according to the invention involves only one oxide element, which comprises metal oxides. Again, this feature applies especially (as one example) if the at least one oxide is selected from an oxide of formula A2O3 with A being Gd.
  • the highly heated gas stream also contains N2O
  • this is decomposed/converted upon contact with said first oxide element, (preferably wherein the N2O is decomposed/converted to NO, NO X , N2 and/or O2)
  • said first oxide element could (also) take the role of an (additional/further) codecomposition catalyst.
  • the first oxide element comprises only one metal oxide (or at least 95, 97, 98 or 99% w/w of the metal oxides comprised). This feature applies especially (as one example) if the at least one oxide is selected from an oxide of formula A2O3 with A being Nd
  • said highly heated gas stream in addition to contacting said first oxide element is further also contacting a second oxide element comprising at least one further oxide being different from said at least one oxide, wherein said at least one further oxide is selected from
  • A being selected from alkaline earth and rare earth elements/lanthanoids, preferably with A being selected from La, Ce, Pr, Nd, Pm, Sm, Eu and Gd, Sr, Ca and Ba, and with B being selected from 3-5d elements, and p-block elements, preferably with B being selected from Ti, V, Cr, Mn, Fe, Co, Ni, Mg, Al, Ga; optionally with one or more elements on A position in form of a solid solution or in an ordered arrangement and/or optionally with one or more elements in B-position in form of a solid solution or in an ordered arrangement and/or optionally in its respective RP phases; or
  • the second oxide element comprises as the at least one further oxide LaNiOs.
  • the second oxide element comprises as the at least one further oxide an oxide as described above for - but different from - said at least one oxide of the first oxide element especially according to ASPECT A) and its SUB-ASPECTS, but also ASPECTS B) and
  • said at least one further oxide comprised in the second oxide element is selected from LaNIOs, La2NIO4, La4Ni30io, NdNIOs, Nd2NiO4, Nd4Ni30io, LaFeOs, and LaCoOs.
  • said at least one further oxide comprised in the second oxide element is selected from LaNIOs, La2NIO4, La4Ni30io, NdNIOs, Nd2NiO4, Nd4Ni30io, and LaFeOs.
  • said at least one further oxide comprised in the second oxide element is selected from LaNIOs, La2NIO4, La4Ni30io, LaFeOs, LaCoOs.
  • said at least one further oxide comprised in the second oxide element is selected from LaNIOs, La2NIO4, La4Ni30io, NdNIOs and LaFeOs.
  • said at least one further oxide comprised in the second oxide element is selected from LaNIOs, La2NIO4, La4Ni30io, NdNIOs and LaFeOs.
  • said at least one further oxide comprised in the second oxide element is selected from LaNIOs, La2NIO4, and La4Ni30 .
  • said at least one further oxide comprised in the second oxide element is selected from NdNIOs, Nd2NIO4, Nd4Ni30io, and LaFeOs.
  • said at least one further oxide comprised in the second oxide element is selected from NdNIOs, Nd2NIO4, Nd4Ni30io, and LaFeOs.
  • said at least one further oxide comprised in the second oxide element is selected from LaNIOs, La2NIO4, La4Ni30io, NdNIOs, Nd2NIO4 and Nd4Ni30io.
  • said at least one further oxide comprised in the second oxide element is selected from LaNIOs, NdNIOs, and LaFeOs.
  • said at least one further oxide comprised in the second oxide element is selected from LaNIOs and NdNIOs.
  • said at least one further oxide comprised in the second oxide element is selected from NdNIOs, and LaFeOs.
  • said at least one further oxide comprised in the second oxide element is LaFeOs.
  • said at least one further oxide comprised in the second oxide element is NdNiOs.
  • said at least one further oxide comprised in the second oxide element is LaNiOs.
  • the second oxide element comprises at least one further oxide being LaNiOs.
  • This embodiment carries the additional advantage that this combination could e.g. allow that the second oxide element can be chosen to be better suited to capture platinum while the first (e.g. comprising the oxide of formula A2O3, especially Nd20s) oxide element helps more effectively capture rhodium or vice versa (maybe also relying on different temperatures of around 800° or around 900° C depending on which noble metal to capture).
  • the first oxide element e.g. comprising the oxide of formula A2O3, especially Nd20s
  • the first oxide element e.g. comprising the oxide of formula A2O3, especially Nd20s oxide element helps more effectively capture rhodium or vice versa (maybe also relying on different temperatures of around 800° or around 900° C depending on which noble metal to capture).
  • This embodiment is based on the surprising effect that it was found that catchment behavior appears to be different depending on whether Pt is collected alone or together with another element as seen in the example with Rh.
  • the oxide of formula A2O3, especially Nd20s when tested on capture of platinum alone seems to show a different behavior if compared to the situation when both platinum and rhodium are present (see Example 4 and Fig. 3).
  • the temperature conditions can be adapted depending on the relative presence of the respective noble metal.
  • the highly heated gas stream after its contact with said catalyst is contacted with said first oxide element at a temperature at around or above 800°C (or at 750°C to 900°C or at 750°C to 850°C or at 800°C to 900°C), preferably at around or above 900 °C (or at 850°C to 950°C), preferably wherein said high temperature gas reaction is carried out at temperatures of at around or above 800°C, preferably at around 900°C or above.
  • the highly heated gas stream after its contact with said catalyst is contacted with said first oxide element at a temperature at around or above 800°C (or at 750°C to 900°C or at 750°C to 850°C or at 800°C to 900°C), or at a temperature at around or above 900 °C (or at 850°C to 950°C).
  • said high temperature gas reaction is carried out at the same temperature, e.g. of at around or above 800°C, or at around 900°C or above.
  • This preferred broader embodiment of the invention is further based on the surprising finding that rhodium capture on the oxide of formula A2O3, especially Nd20s seems to be connected to a higher temperature. This more pronounced capture of rhodium with these higher temperatures at around 900°C can be seen in Example 1 . It can be seen there as well, that at around 800 °C Platinum capture seems optimized and dominates. The art is completely silent on this influence of temperature on rhodium or platinum capture.
  • the highly heated gas stream also contains N2O, which is decomposed/converted upon contact with said first oxide element, preferably wherein the N2O is decomposed/converted to NO, NO X , N2 and/or O2.
  • the catalytic reaction of the high temperature gas reaction is a catalytic ammonia oxidation or catalytic ammonia combustion.
  • the invention relates to a use of an oxide element comprising at least one oxide selected from an oxide of formula A2O3 with A being selected from rare earth elements/lanthanoids, optionally with one or more elements on A position in form of a solid solution for the capture of at least one noble metal being selected from rhodium and platinum, especially from a highly heated gas stream (at a temperature of at least 700 °C), which contains the volatilized at least one noble metal while such volatilized noble metal is still essentially in the vapor phase.
  • the at least one oxide comprised by said oxide element used according to the invention is selected from an oxide of formula A2O3 with A as defined above for ASPECT A) and its SUB-ASPECTS, but also - alternatively - ASPECTS B) and C)).
  • the at least one oxide comprised by said oxide element used according to the invention is selected from an oxide of formula A2O3 with A being selected from Nd and Gd (or - alternatively - as defined in the other ASPECTS).
  • the highly heated gas stream is at a temperature of at least 700 °C and/or the use is for the capture of rhodium and platinum.
  • the use is for the capture of rhodium and platinum.
  • the use is for the capture of platinum and rhodium, especially in the same process.
  • the use further encompasses the decomposition/conversion of N2O, especially in the same process, preferably wherein the N2O is decomposed/converted upon contact with said oxide element, most preferably wherein the N2O is decomposed/converted to NO, NO X , N2 and/or O2.
  • the invention in another different aspect, relates to a device for the capture of at least one noble metal being selected from rhodium and platinum from a combustion furnace of the type having a noble metal gauze arranged across the furnace in a direction transverse to the flow of gas therethrough, said device being an oxide element comprising or consisting of at least one oxide selected from an oxide of formula A2O3 with A being selected from rare earth elements/lanthanoids, optionally with one or more elements on A position in form of a solid solution.
  • the invention relates to a catchment device for the capture of at least one noble metal being selected from rhodium and platinum, in an ammonia oxidation reaction, comprising an oxide element comprising or consisting of at least one oxide selected from an oxide of formula A2O3 with A being selected from rare earth elements/lanthanoids, optionally with one or more elements on A position in form of a solid solution.
  • the at least one oxide comprised by said oxide element comprised by the device or catchment device according to the invention is selected from an oxide of formula A2O3 with A as defined above for ASPECT A) and its SUB-ASPECTS, but also - alternatively - ASPECTS B) and C ⁇ ).
  • the at least one oxide comprised by said oxide element comprised by the device or catchment device according to the invention is selected from an oxide of formula A2O3 with A being selected from Nd and Gd (or - alternatively - as defined in the other ASPECTS).
  • the use of the device or catchment device is for the capture of rhodium and platinum.
  • the device according to the invention or catchment device according to the invention said oxide is an oxide of formula A2O3 with A being selected from La, Ce, Pr, Nd, Pm, Sm, Eu and Gd; or from La, Nd, Pm, Sm, Eu and Gd; or from La, Ce, Pr, Nd, Pm, Sm, Eu and Gd; preferably from La, Nd and Gd, more preferably from La and Nd; especially said oxide is selected from Nd20s, La2O3, and Gd2O3, preferably from Nd20s and Gd2Os; most preferably said oxide is Nd20s.
  • lanthanoid is to be understood as meaning a series of chemical elements of atomic numbers 57-71 , from lanthanum through lutetium.
  • lanthanoids in the context of the invention are selected from La, Ce, Pr, Nd, Pm, Sm, Eu and Gd.
  • transition metal is to be understood as meaning a chemical element in d-block od the periodic table, including groups 3 to 12.
  • the “transition metals” in the context of the invention are selected from Fe, Co, Ni and Zn ....
  • alkaline earth metal is to be understood as meaning the chemical elements Be, Mg, Ca, Sr, Ba and Rd from Group 2 of the periodic table.
  • alkali metal is to be understood as meaning the chemical elements Li, Na, K, Rb, Cs and Fr from Group 1 of the periodic table.
  • capture is to be understood as meaning the fixation of the noble metal that was volatilized before on e.g. an oxide element, the oxide or the metal element or a metal of the metal element.
  • “decompose” and/or “convert” is to be understood as meaning the conversion/decomposition, especially of N2O, especially to NO, NOx, N2 and/or O2. This happens upon contact with an element, e.g. the “first oxide element”, (or the oxide comprised therein) and thus for example leads to an abatement of the laughing gas.
  • volatilization (from a catalyst) is to be understood as meaning the removal of the noble metal like rhodium or platinum from e.g. the solid metal structure of e.g. the catalyst and putting this noble metal or any derivative in its “vapor phase”, including taking it up in this vapor phase e.g. in a gas stream. This volatilization usually happens at “high temperatures”.
  • high temperature is to be understood as meaning at a temperature of or above 700°C.
  • contact is to be understood as meaning a physical contact or close contact e.g. coming within 1 cm or less, e.g. between the gas of a “high heated gas stream” or a volatilized noble metal (or a derivative, e.g. in said gas stream with an oxide element or the metal element.
  • high heated gas stream is to be understood as meaning as steam of gas like N2, NH3, air, O2, CO2 or any other gas at temperatures of or above 700°C.
  • perovskite is to be understood as meaning that a perovskite is a compound, ABX3, that belong to the class of compounds that take a perovskite type structure.
  • X O
  • the perovskite is an oxide ABO3.
  • the B-site cation is 6-coordinated to oxygen and A-site is 12- coordinated to oxygen.
  • a site cation is generally from (alkali earth) alkaline earth and rare earth elements whereas B site cation is generally selected from 3-5d elements, p-block elements.
  • the perovskite oxide can have lower symmetry, being distorted, and may have oxygen vacancies in random or ordered patterns.
  • RP-phase is to be understood as meaning that an RP phase is a phase that is described by the so-called Ruddlesden-Popper type structure.
  • the general formula is A n+i B n O3n+i or (ABO3)n(AO) whereof n is an integer.
  • the atomic arrangement in ABO3 (part of the structure) is the same as in the perovskite whereas AO is a structure fragment corresponding to half a rock salt layer.
  • a site cation is generally from alkaline earth and rare earth elements whereas B site cation is generally selected from 3-5d elements, p-block elements.
  • a solid solution in form of a solid solution is to be understood as meaning that a solid solution is a uniform mixture of two crystalline solids that share a common crystal lattice. Solid solutions often consist of two or more types of atoms that occupy the same crystallographic site in the crystal structure in a random manner.
  • an ordered arrangement is to be understood as meaning that an ordered arrangement occurs when two or more types of atoms are having the potential to occupy the same crystallographic site in a crystal structure, however, their distribution is not random in nature as for a solid solution, but rather systematically alternating in manner.
  • one or more elements on A position in form of a solid solution or in an ordered arrangement is to be understood as meaning that the compound has two or more types of category A-atoms that occupy the same crystallographic site in the structure in a random manner (solid solution) or in a systematic manner (ordered arrangement).
  • rare earth is to be understood as meaning a cation representing Sc, Y, La or the fourteen 4f-elements; i.e. elements with numbers 21 , 38, and 57 to 71 in the Periodic Table.
  • lanthanoids/rare earth elements is to be understood as meaning that the respective “A” is selected from both the lanthanoids or rare earth elements as defined herein. Thus, in a preferred embodiment it encompasses or is selected from Ce, Pr, Nd, Pm, Sm, Eu, Gd, or La, Sc, or Y.
  • 3-5d elements is to be understood as meaning that 3-5d elements refer to 3d, 4d and 5d elements in the periodic table, altogether 10, 10 and 10 elements, respectively
  • p-block elements is to be understood as meaning that p- block elements refer to the elements in groups 13, 14 and 15, in the periodic table.
  • a laboratory scale six-zone furnace (Entech Energiteknik AB, Sweden) was used in the Pt and Pt+Rh catchment experiments. All the experiments were run in dry air ( ⁇ 300 ppm H2O) with a flow of approximately 450 mL/min in quartz tubes of inner diameter 4 mm, giving a similar linear gas velocity as in the ammonia oxidation process. Rolled up nets of Pt or Pt-Rh were placed upstream of the oxide rectangular pellets in a zone set to 1000 °C to yield PtC /RhC in the gas phase. The duration of the catchment experiments were in the range from 1 to 26 days, and 3 parallel experiments were run at the same time by placing the oxide pellets in 3 parallel tubes in 3 different zones of different temperatures: 700, 800 and 900 °C.
  • CaO Gd2Os and Nd20s were tested in a lab scale for Pt and Rh catchment at 700, 800 and 900°C.
  • a laboratory scale six-zone furnace (Entech Energiteknik AB, Sweden) was used in the Pt and Pt+Rh catchment experiments. All the experiments were run in dry air ( ⁇ 300 ppm H2O) with a flow of approximately 450 mL/min in quartz tubes of inner diameter 4 mm, giving a similar linear gas velocity as in the ammonia oxidation process. Rolled up nets of Pt or Pt-Rh were placed upstream of the oxide rectangular pellets in a zone set to 1000 °C to yield PtC /RhC in the gas phase. The duration of the catchment experiments were in the range from 1 to 26 days, and 3 parallel experiments were run at the same time by placing the oxide pellets in 3 parallel tubes in 3 different zones of different temperatures: 700, 800 and 900 °C.
  • Table 1 shows a summary of EDX results and crystal structure from XRD of surfaces of pellets of catchment oxides after reaction with PtO2(g) at 700, 800 and 900°C for 26 days.
  • the primary cation of each oxide is called A and EDX quantifications are given as Pt/(Pt+A) molar fraction.

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Abstract

La présente invention concerne un procédé de capture d'un métal noble, en particulier du rhodium et/ou du platine, perdu par volatilisation d'un catalyseur en un flux gazeux fortement chauffé (notamment un chauffage local dû à une réaction fortement exothermique) par mise en contact du flux gazeux fortement chauffé contenant le métal noble volatilisé avec un premier élément oxyde comprenant un oxyde de formule A2O3, en particulier du Nd2O3, ainsi que l'utilisation d'un oxyde de formule A2O3, en particulier du Nd2O3 aux fins de la capture d'un tel métal noble ou des dispositifs de captage comprenant un oxyde de formule A2O3, en particulier du Nd2O3. Le présent procédé est particulièrement utile pour les procédés industriels tels que le procédé Ostwald (montrant une réaction fortement exothermique) dans lequel un catalyseur contenant du rhodium et du platine est utilisé. Dans des circonstances choisies, ces oxydes peuvent également agir sur la décomposition du N2O indésirable survenant dans ledit procédé Ostwald.
PCT/EP2024/070600 2023-07-21 2024-07-19 Procédé de capture d'un métal noble, en particulier du rhodium et/ou du platine, perdu par volatilisation d'un catalyseur en un flux gazeux fortement chauffé à l'aide d'un oxyde de formule a2o3 Pending WO2025021701A1 (fr)

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Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US4774069A (en) * 1985-06-28 1988-09-27 Johnson Matthey Public Limited Company Process for the manufacture of nitric oxide
WO2004096703A2 (fr) * 2003-04-29 2004-11-11 Johnson Matthey Plc Procede d'oxydation de l'ammoniac
US20180043342A1 (en) * 2016-08-12 2018-02-15 Johnson Matthey Public Limited Company Exhaust system for a compression ignition engine having a capture region for volatilised platinum

Patent Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US4774069A (en) * 1985-06-28 1988-09-27 Johnson Matthey Public Limited Company Process for the manufacture of nitric oxide
WO2004096703A2 (fr) * 2003-04-29 2004-11-11 Johnson Matthey Plc Procede d'oxydation de l'ammoniac
US20180043342A1 (en) * 2016-08-12 2018-02-15 Johnson Matthey Public Limited Company Exhaust system for a compression ignition engine having a capture region for volatilised platinum

Non-Patent Citations (2)

* Cited by examiner, † Cited by third party
Title
FJELLVAG ASBJØRN SLAGTERN: "Platinum Catchment by Noble Metal Alloys and structural studies of Pt- and Rh-containing perovskites", SERIES OF DISSERTATIONS SUBMITTED TO THE FACULTY OF MATHEMATICS AND NATURAL SCIENCES, 6 October 2022 (2022-10-06), NO, pages 1 - 27, XP093124893, ISSN: 1501-7710, Retrieved from the Internet <URL:https://www.duo.uio.no/bitstream/handle/10852/97026/PhD-Fjellvaag-2022.pdf?sequence=1&isAllowed=y> [retrieved on 20240129] *
N.I. ZAKHARCHENKO: "Recovery of platinum with calcium oxide sorbent in ammonia oxidation", RUSS. J. APPL. CHEM., 2002, pages 402 - 407

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