WO2024017884A1 - Process for the catalytic activation of n2o - Google Patents

Process for the catalytic activation of n2o Download PDF

Info

Publication number
WO2024017884A1
WO2024017884A1 PCT/EP2023/069905 EP2023069905W WO2024017884A1 WO 2024017884 A1 WO2024017884 A1 WO 2024017884A1 EP 2023069905 W EP2023069905 W EP 2023069905W WO 2024017884 A1 WO2024017884 A1 WO 2024017884A1
Authority
WO
WIPO (PCT)
Prior art keywords
zeolitic material
aei
framework structure
type framework
range
Prior art date
Application number
PCT/EP2023/069905
Other languages
French (fr)
Inventor
Trees Maria DE BAERDEMAEKER
Andrei-Nicolae PARVULESCU
Toshiyuki Yokoi
Original Assignee
Basf Se
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Basf Se filed Critical Basf Se
Publication of WO2024017884A1 publication Critical patent/WO2024017884A1/en

Links

Classifications

    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01DSEPARATION
    • B01D53/00Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
    • B01D53/34Chemical or biological purification of waste gases
    • B01D53/74General processes for purification of waste gases; Apparatus or devices specially adapted therefor
    • B01D53/86Catalytic processes
    • B01D53/8621Removing nitrogen compounds
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01JCHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J29/00Catalysts comprising molecular sieves
    • B01J29/04Catalysts comprising molecular sieves having base-exchange properties, e.g. crystalline zeolites
    • B01J29/06Crystalline aluminosilicate zeolites; Isomorphous compounds thereof
    • B01J29/70Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of types characterised by their specific structure not provided for in groups B01J29/08 - B01J29/65
    • B01J29/72Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of types characterised by their specific structure not provided for in groups B01J29/08 - B01J29/65 containing iron group metals, noble metals or copper
    • B01J29/76Iron group metals or copper
    • CCHEMISTRY; METALLURGY
    • C01INORGANIC CHEMISTRY
    • C01BNON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B39/00Compounds having molecular sieve and base-exchange properties, e.g. crystalline zeolites; Their preparation; After-treatment, e.g. ion-exchange or dealumination
    • C01B39/02Crystalline aluminosilicate zeolites; Isomorphous compounds thereof; Direct preparation thereof; Preparation thereof starting from a reaction mixture containing a crystalline zeolite of another type, or from preformed reactants; After-treatment thereof
    • C01B39/026After-treatment
    • CCHEMISTRY; METALLURGY
    • C01INORGANIC CHEMISTRY
    • C01BNON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B39/00Compounds having molecular sieve and base-exchange properties, e.g. crystalline zeolites; Their preparation; After-treatment, e.g. ion-exchange or dealumination
    • C01B39/02Crystalline aluminosilicate zeolites; Isomorphous compounds thereof; Direct preparation thereof; Preparation thereof starting from a reaction mixture containing a crystalline zeolite of another type, or from preformed reactants; After-treatment thereof
    • C01B39/46Other types characterised by their X-ray diffraction pattern and their defined composition
    • C01B39/48Other types characterised by their X-ray diffraction pattern and their defined composition using at least one organic template directing agent
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01DSEPARATION
    • B01D2251/00Reactants
    • B01D2251/20Reductants
    • B01D2251/208Hydrocarbons
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01DSEPARATION
    • B01D2255/00Catalysts
    • B01D2255/20Metals or compounds thereof
    • B01D2255/207Transition metals
    • B01D2255/20761Copper
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01DSEPARATION
    • B01D2255/00Catalysts
    • B01D2255/50Zeolites
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01DSEPARATION
    • B01D2257/00Components to be removed
    • B01D2257/40Nitrogen compounds
    • B01D2257/402Dinitrogen oxide

Definitions

  • the present invention relates to a process for the activation of N 2 O comprising contacting a gas stream containing N 2 O with a catalyst comprising a zeolitic material having the AEI-type frame- work structure, wherein the zeolitic material contains copper.
  • a catalyst comprising a zeolitic material having the AEI-type frame- work structure, wherein the zeolitic material contains copper.
  • INTRODUCTION Zeolitic materials having framework type AEI are known to be potentially effective as catalysts or catalyst components for treating combustion exhaust gas in industrial applications, for exam- ple for converting nitrogen oxides (NOx) in an exhaust gas stream.
  • Synthetic AEI zeolitic materi- als are generally produced by precipitating crystals of the zeolitic material from a synthesis mix- ture which contains the sources of the elements from which the zeolitic framework is built, such as a source of silicon and a source of aluminum.
  • An alternative approach may be the prepara- tion via zeolitic framework conversion according to which a starting material which is a suitable zeolitic material having a framework type other than AEI is suitably reacted to obtain the zeolitic material having framework type AEI.
  • US 5,958,370 relates to SSZ-39 and to its preparation using cyclic or polycyclic quater- nary ammonium cations as templating agent. Moliner, M. et al.
  • Commun.2015, 51, 11030- 11033 concerns the synthesis of Cu-SSZ-39 and its use as a catalyst in the SCR of nitrogen ox- ides NOx.
  • these include the use of N,N-dimethyl-3,5-dimethylpiperidinium cations as well as of tetrae- thylphosphonium cations.
  • Dusselier, M. et al. in ACS Catal.2015, 5, 10, 6078-6085 describe methanol to olefin catalysis using hydrothermally treated SSZ-39.
  • US 2015/0118150 A1 describes zeolite synthesis methods involving the use of N,N-dimethyl- 3,5-dimethylpiperidinium and N,N-dimethyl-2,6-dimethylpiperidinium cations, respectively.
  • WO 2016/149234 A1 and Ransom, R. et al. in Ind. Eng. Chem. Res.2017, 56, 4350 ⁇ 4356 respec- tively relate to the synthesis of SSZ-39 via interzeolitic conversion of faujasite using N,N-dime- thyl-3,5-dimethylpiperidinium cations as the organotemplate.
  • WO 2018/113566 A1 relates to the synthesis of zeolites via solvent-free interzeolitic conversion, wherein the synthesis of SSZ-39 from interzeolitic conversion of zeolite Y using N,N-dimethyl-2,6-dimethylpi- peridinium cations is described.
  • WO 2016/149234 A1 and Ransom, R. et al. in Ind. Eng. Chem. Res.2017, 56, 4350-4356 re- spectively relate to the synthesis of SSZ-39 using different isomer ratios of the cis and trans iso- mers of the N,N-dimethyl-3,5-dimethylpiperidinium cation.
  • WO 2020/098796 A1 concerns the production of an AEI-type zeolitic material via solvent-free interzeolitic con- version, wherein N,N-dimethyl-3,5-dimethylpiperidinium having a specific ratio of cis and trans isomers was employed.
  • WO 2018/234044 A1 relates to a process for the oxidation of lower alkanes in the presence of ammonia over a copper loaded zeolite catalyst.
  • WO 2017/134007 A1 concerns a method for the removal of nitrous oxide from an off gas over an iron loaded zeolite having the AEI-type framework structure.
  • US 2016/264428 A1 discloses the production of zeolites by selective use of the trans isomer of 3,5-dimethyl-N,N-dimethylpiperidinium hydroxide, or of a mixture of cis and trans isomers with an enhanced content of the trans isomer.
  • the present invention therefore relates to a process for the activation of N 2 O comprising (i) providing a gas stream comprising N 2 O; (ii) contacting the gas stream provided in (i) with a catalyst at a temperature in the range of from 300 to 600 °C, wherein the catalyst comprises a zeolitic material having the AEI-type framework structure, wherein the framework structure of the zeolitic material comprises SiO 2 and Al 2 O 3 , and wherein the zeolitic material contains copper.
  • the gas stream in (i) contains N 2 O in an amount ranging from 1 to 100 vol.-%, more preferably from 5 to 90 vol.-%, more preferably from 10 to 80 vol.-%, more preferably from 15 to 70 vol.-%, more preferably from 20 to 60 vol.-%, more preferably from 25 to 55 vol.-%, more preferably from 30 to 50 vol.-%, more preferably from 35 to 45 vol.-%, and more prefera- bly from 38 to 42 vol.-%. It is preferred that the gas stream in (i) further comprises a reducing agent.
  • the reducing agent is selected from the group consisting of hydrocarbons, more preferably from the group consisting of (C 1 -C 8 )alkanes, more preferably from the group consisting of (C 1 -C 7 )alkanes, including mixtures of two or more thereof, more preferably from the group consisting of (C 1 -C 6 )alkanes, including mixtures of two or more thereof, more prefera- bly from the group consisting of (C 1 -C 5 )alkanes, including mixtures of two or more thereof, more preferably from the group consisting of (C 1 -C 4 )alkanes, including mixtures of two or more thereof, more preferably from the group consisting of (C 1 -C 3 )alkanes, including mixtures of two or more thereof, more preferably from the group consisting of (C 1 -C 2 )alkanes, including mixtures of two or more thereof, more preferably from the group consisting of methane and ethan
  • contacting in (ii) of the gas stream provided in (i) with a catalyst is conducted at a temperature in the range of from 350 to 550 °C, more preferably of from 400 to 550 °C, and more preferably of from 450 to 500 °C.
  • the SiO 2 : Al 2 O 3 molar ratio of the zeolitic material having the AEI-type frame- work structure is in the range of from 4 to 200, more preferably of from 6 to 120, more prefera- bly of from 8 to 80, more preferably of from 10 to 50, more preferably of from 12 to 35, more preferably of from 14 to 30, more preferably of from 16 to 25, more preferably of from 18 to 22, and more preferably of from 19.5 to 20.5.
  • the zeolitic material having the AEI-type framework structure is ion ex- changed with copper. It is preferred that the zeolitic material having the AEI-type framework structure contains copper in an amount in the range of from 0.1 to 12 wt.-% based on 100 wt.-% of the zeolitic material having the AEI-type framework structure, wherein copper is calculated as the element, wherein more preferably the zeolitic material having the AEI-type framework structure contains copper in an amount in the range of from 0.3 to 10 wt.-%, more preferably of from 0.5 to 8 wt.-%, more preferably of from 0.7 to 6 wt.-%, more preferably of from 0.9 to 4 wt.-%, more preferably of from 1.1 to 3 wt.-%, more preferably of from 1.3 to 2.5 wt.-%, more preferably of from 1.5 to 2.3 wt.- %, more preferably of from 1.7 to 2 wt.
  • the zeolitic material having the AEI-type framework structure comprised in the catalyst is prepared by a process comprising (1) preparing a mixture comprising one or more sources of SiO 2 , a first zeolitic material com- prising SiO 2 and Al 2 O 3 in its framework structure and having an FAU-type framework structure, one or more cationic structure directing agents, and water; (2) heating the mixture obtained in (1) for obtaining a second zeolitic material comprising SiO 2 and Al 2 O 3 in its framework structure and having an AEI-type framework structure.
  • the one or more cationic structure directing agents are selected from the group consisting of N,N-di(C 1 -C 4 )alkyl-3,5-di(C 1 -C 4 )alkylpyrrolidinium, N,N-di(C 1 -C 4 )alkyl-3,5-di(C 1 -C 4 )alkylpiperi- dinium, N,N-di(C 1 -C 4 )alkyl-3,5-di(C 1 -C 4 )alkylhexahydroazepinium, and mixtures of two or more thereof, more preferably from the group consisting of N,N-di(C 1 -C 3 )alkyl-3,5-di(C 1 -C 3 )alkylpyrrolidinium
  • the one or more cationic structure directing agents are selected from the group consisting of N,N-di(C 1 -C 4 )alkyl-3,5-di(C 1 -C 4 )alkylpyrrolidinium, N,N-di(C 1 -C 4 )alkyl-3,5- di(C 1 -C 4 )alkylpiperidinium, N,N-di(C 1 -C 4 )alkyl-3,5-di(C 1 -C 4 )alkylhexahydroazepinium, and mix- tures of two or more thereof, it is preferred according to a first alternative that the cis : trans mo- lar ratio of the cis isomer to the trans isomer in the one or more cationic structure directing agents relative to the alkyl groups at the 3 and 5 positions of the heterocyclic amine ring is in the range of from 0.01:1 to 0.95:1, more preferably of from 0.03:
  • the one or more cationic structure directing agents are selected from the group consisting of N,N-di(C 1 -C 4 )alkyl-3,5-di(C 1 -C 4 )alkylpyrrolidinium, N,N-di(C 1 -C 4 )alkyl-3,5- di(C 1 -C 4 )alkylpiperidinium, N,N-di(C 1 -C 4 )alkyl-3,5-di(C 1 -C 4 )alkylhexahydroazepinium, and mix- tures of two or more thereof, it is preferred according to a second alternative that the trans : cis molar ratio of the trans isomer to the cis isomer in the one or more cationic structure directing agents relative to the alkyl groups at the 3 and 5 positions of the heterocyclic amine ring is in the range of from 1:1 to 0:1, more preferably of from 0.8:1 to 0
  • the one or more cationic structure directing agents are provided as salts, pref- erably as one or more salts selected from the group consisting of halides, sulfate, nitrate, phos- phate, acetate, and mixtures of two or more thereof, more preferably from the group consisting of bromide, chloride, hydroxide, sulfate, and mixtures of two or more thereof, wherein more pref- erably the one or more cationic structure directing agents are provided as hydroxides and/or bromides, and more preferably as hydroxides.
  • the framework structure of the first zeolitic material displays a SiO 2 : Al 2 O 3 mo- lar ratio ranging from 1.5 to 100, more preferably of from 2 to 50, more preferably of from 2.5 to 25, more preferably of from 3 to 15, more preferably of from 3.5 to 10, more preferably of from 4 to 7, and more preferably of from 4.5 to 5.
  • the mixture prepared in (1) and heated in (2) displays an SDA : Si molar ratio of the one or more cationic structure directing agents (SDA) to Si contained in the mixture in the range of from 0.01 to 1.5, more preferably of from 0.05 to 1.2, more preferably of from 0.1 to 0.8, more preferably of from 0.3 to 0.6, more preferably of from 0.5 to 0.45, more preferably of from 0.8 to 0.35, more preferably of from 0.1 to 0.3, more preferably of from 0.13 to 0.25, and more preferably of from 0.15 to 0.2.
  • SDA cationic structure directing agents
  • the one or more sources of SiO 2 is selected from the group consisting of fumed silica, silica hydrosols, reactive amorphous solid silicas, silica gel, silicic acid, water glass, so- dium metasilicate hydrate, sesquisilicate, disilicate, colloidal silica, silicic acid esters, and mix- tures of two or more thereof, more preferably from the group consisting of fumed silica, silica hy- drosols, reactive amorphous solid silicas, silica gel, silicic acid, colloidal silica, silicic acid esters, and mixtures of two or more thereof, more preferably from the group consisting of fumed silica, silica hydrosols, reactive amorphous solid silicas, silica gel
  • the first zeolitic material having an FAU-type framework structure is selected from the group consisting of ZSM-3, Faujasite, [Al-Ge-O]-FAU, CSZ-1, ECR-30, Zeolite X, Zeo- lite Y, LZ-210, SAPO-37, ZSM-20, Na-X, US-Y, Na-Y, [Ga-Ge-O]-FAU, Li-LSX, [Ga-Al-Si-O]- FAU, and [Ga-Si-O]-FAU, including mixtures of two or more thereof, more preferably from the group consisting of ZSM-3, Faujasite, CSZ-1, ECR-30, Zeolite X, Zeo- lite Y, LZ-210, ZSM-20, Na-X,
  • the mixture prepared in (1) further comprises OH-.
  • the OH- : Si molar ratio of hydroxide to Si contained in the mixture prepared in (1) is in the range of from 0.01 to 5, more preferably from 0.05 to 3, more preferably from 0.1 to 1.5, more preferably from 0.2 to 1, more preferably from 0.3 to 0.8, and more preferably from 0.5 to 0.7, and more prefera- bly from 0.6 to 0.65.
  • the mixture prepared in (1) further comprises one or more alkali metals M, more preferably one or more alkali metals M selected from the group consisting of Na, K, and mix- tures thereof, wherein more preferably the mixture prepared in (1) further comprises Na as the alkali metal M.
  • the M : Si atomic ratio of the one or more alkali metals M to Si contained in the mixture prepared in (1) is in the range of from 0.01 to 2.5, more preferably of from 0.05 to 1.5, more preferably of from 0.1 to 1.0, more preferably of from 0.3 to 0.7, more preferably of from 0.4 to 0.5, and more preferably of from 0.45 to 0.47.
  • the mixture prepared in (1) further comprises one or more alkali met- als M
  • the one or more alkali metals M are comprised in the mixture prepared in (1) as hydroxide.
  • the mixture prepared in (1) contains water at an H 2 O : Si molar ratio in the range of from 1 to 60, more preferably of from 5 to 40, more preferably of from 10 to 30, more preferably of from 15 to 25, and more preferably of from 18 to 22.
  • heating in (2) is conducted at a temperature in the range of from 80 to 250 °C, more preferably from 100 to 230 °C, more preferably from 110 to 220 °C, more preferably from 115 to 210 °C, more preferably from 120 to 200 °C, more preferably from 125 to 190 °C, more preferably from 130 to 180 °C, more preferably from 135 to 170 °C, more preferably from 140 to 160 °C, and more preferably from 145 to 155 °C.
  • the zeolitic material having the AEI-type framework structure com- prised in the catalyst is prepared by a process comprising (1) and (2) as defined hereinabove, it is preferred that heating in (2) is conducted under autogenous pressure, more preferably under hydrothermal conditions. Further in the case where the zeolitic material having the AEI-type framework structure com- prised in the catalyst is prepared by a process comprising (1) and (2) as defined hereinabove, it is preferred that the heating in (2) is performed in a pressure tight vessel, more preferably in an autoclave.
  • heating in (2) is conducted for a duration in the range of from 3 h to 10 d, more preferably from 6 h to 8 d, more preferably from 12 h to 6 d, more preferably from 1 to 5 d, more preferably from 1.5 to 4.5 d, more preferably from 2 to 4 d, and more preferably from 2.5 to 3.5 d.
  • the second zeolitic material obtained in (2) having an AEI-type framework struc- ture is selected from the group consisting of SSZ-39, SAPO-18, SIZ-8, including mixtures of two or more thereof, wherein more preferably the second zeolitic material obtained in (2) comprises SSZ-39, and wherein more preferably the second zeolitic material obtained in (2) is SSZ-39.
  • the process further comprises (3) calcining the second zeolitic material obtained in (2).
  • the process further comprises (4) subjecting the zeolitic material obtained in (2) or (3) to an ion-exchange procedure, wherein one or more ionic extra-framework elements contained in the zeolite framework is ion- exchanged against H + and/or NH 4 + , more preferably against NH 4 + .
  • the process further comprises (5) subjecting the zeolitic material obtained in (2), (3), or (4) to an ion-exchange procedure, wherein one or more ionic extra-framework elements contained in the zeolite framework is ion- exchanged against copper.
  • the process further comprises (6) calcining the zeolitic material obtained in (5).
  • the temperature of calcination in (3) and/or (6) is in the range of from 300 to 900 °C, more preferably of from 400 to 700 °C, more preferably of from 450 to 650 °C, and more preferably of from 500 to 600 °C.
  • calcining in (3) and/or (6) is conducted for a period in the range of from 0.5 to 10 h, more preferably from 1 to 15 h, more preferably from 2 to 12 h, more preferably from 3 to 9 h, more preferably from 4 to 7 h, more preferably from 4.5 to 6.5 h, and more preferably from 5 to 6 h.
  • the mixture in (1) further comprises seed crystals, wherein the seed crystals more preferably comprise a zeolitic material having an AEI-type framework structure, wherein more preferably the zeolitic material consists of a zeolitic material having an AEI-type framework structure.
  • the mixture in (1) further comprises seed crystals
  • the zeo- litic material having an AEI-type framework structure comprised in the seed crystals is selected from the group consisting of SSZ-39, SAPO-18, SIZ-8, including mixtures of two or more thereof, wherein more preferably the zeolitic material having an AEI-type framework structure comprised in the seed crystals is SSZ-39.
  • the amount of seed crystals in the mixture prepared in (1) and heated in (2) ranges from 3 to 12 wt.-% based on 100 wt.-% of Si in the mixture prepared in (1) calculated as the element, more preferably from 3.5 to 10 wt.-%, more preferably from 4 to 9 wt.-%, more preferably from 4.5 to 7 wt.-%, and more preferably from 5 to 6 wt.-% based on 100 wt.-% of Si in the mixture prepared in (1) calculated as the element.
  • the present invention is further illustrated by the following set of embodiments and combina- tions of embodiments resulting from the dependencies and back-references as indicated.
  • a process for the activation of N 2 O comprising (i) providing a gas stream comprising N 2 O; (ii) contacting the gas stream provided in (i) with a catalyst at a temperature in the range of from 300 to 600 °C, wherein the catalyst comprises a zeolitic material having the AEI-type framework structure, wherein the framework structure of the zeolitic material comprises SiO 2 and Al 2 O 3 , and wherein the zeolitic material contains copper.
  • the gas stream in (i) contains N 2 O in an amount ranging from 1 to 100 vol.-%, preferably from 5 to 90 vol.-%, more preferably from 10 to 80 vol.-%, more preferably from 15 to 70 vol.-%, more preferably from 20 to 60 vol.-%, more preferably from 25 to 55 vol.-%, more preferably from 30 to 50 vol.-%, more prefera- bly from 35 to 45 vol.-%, and more preferably from 38 to 42 vol.-%. 3.
  • the gas stream in (i) further comprises a re- ducing agent. 4.
  • any of embodiments 1 to 5 wherein the SiO 2 : Al 2 O 3 molar ratio of the zeo- litic material having the AEI-type framework structure is in the range of from 4 to 200, pref- erably of from 6 to 120, more preferably of from 8 to 80, more preferably of from 10 to 50, more preferably of from 12 to 35, more preferably of from 14 to 30, more preferably of from 16 to 25, more preferably of from 18 to 22, and more preferably of from 19.5 to 20.5. 7.
  • the zeolitic material having the AEI- type framework structure contains copper in an amount in the range of from 0.1 to 12 wt.- % based on 100 wt.-% of the zeolitic material having the AEI-type framework structure, wherein copper is calculated as the element, wherein preferably the zeolitic material hav- ing the AEI-type framework structure contains copper in an amount in the range of from 0.3 to 10 wt.-%, more preferably of from 0.5 to 8 wt.-%, more preferably of from 0.7 to 6 wt.-%, more preferably of from 0.9 to 4 wt.-%, more preferably of from 1.1 to 3 wt.-%, more preferably of from 1.3 to 2.5 wt.-%, more preferably of from 1.5 to 2.3 wt.-%, more preferably of from 1.7 to 2 wt.-%, and more preferably of from 1.8 to 1.9 wt.
  • the zeolitic material having the AEI- type framework structure comprised in the catalyst is prepared by a process comprising (1) preparing a mixture comprising one or more sources of SiO 2 , a first zeolitic material comprising SiO 2 and Al 2 O 3 in its framework structure and having an FAU-type framework structure, one or more cationic structure directing agents, and water; (2) heating the mixture obtained in (1) for obtaining a second zeolitic material compris- ing SiO 2 and Al 2 O 3 in its framework structure and having an AEI-type framework structure. 10.
  • the one or more cationic structure directing agents are selected from the group consisting of N,N-di(C 1 -C 4 )alkyl-3,5-di(C 1 -C 4 )alkylpyrroli- dinium, N,N-di(C 1 -C 4 )alkyl-3,5-di(C 1 -C 4 )alkylpiperidinium, N,N-di(C 1 -C 4 )alkyl-3,5-di(C 1 - C 4 )alkylhexahydroazepinium, and mixtures of two or more thereof, preferably from the group consisting of N,N-di(C 1 -C 3 )alkyl-3,5-di(C 1 -C 3 )alkylpyrrolidinium, N,N-di(C 1 -C 3 )alkyl-3,5-di(C 1 -C 3 )alkylpiperidinium
  • trans : cis molar ratio of the trans isomer to the cis isomer in the one or more cationic structure directing agents relative to the alkyl groups at the 3 and 5 positions of the heterocyclic amine ring is in the range of from 1:1 to 0:1, preferably of from 0.8:1 to 0:1, more preferably of from 0.5:1 to 0:1, more preferably of from 0.4:1 to 0:1, more preferably of from 0.3:1 to 0:1, more preferably of from 0.2:1 to 0:1, more preferably of from 0.1:1 to 0:1, more preferably of from 0.05:1 to 0:1, and more preferably of from 0.01:1 to 0:1. 13.
  • the one or more cationic structure directing agents are provided as salts, preferably as one or more salts selected from the group consisting of halides, sulfate, nitrate, phosphate, acetate, and mixtures of two or more thereof, more preferably from the group consisting of bromide, chloride, hydroxide, sulfate, and mixtures of two or more thereof, wherein more preferably the one or more cat- ionic structure directing agents are provided as hydroxides and/or bromides, and more preferably as hydroxides. 14.
  • SDA cationic structure direct- ing agents
  • any of embodiments 9 to 15, wherein the one or more sources of SiO 2 is selected from the group consisting of fumed silica, silica hydrosols, reactive amorphous solid silicas, silica gel, silicic acid, water glass, sodium metasilicate hydrate, sesquisilicate, disilicate, colloidal silica, silicic acid esters, and mixtures of two or more thereof, preferably from the group consisting of fumed silica, silica hydrosols, reactive amorphous solid sili- cas, silica gel, silicic acid, colloidal silica, silicic acid esters, and mixtures of two or more thereof, more preferably from the group consisting of fumed silica, silica hydrosols, reac- tive amorphous solid silicas, silica gel, colloidal silica, and mixtures of two or more thereof, wherein even more preferably the one or more sources for YO 2 comprises fumed silica and/or colloidal siliclica
  • the first zeolitic material having an FAU-type framework structure is selected from the group consisting of ZSM-3, Faujasite, [Al-Ge-O]-FAU, CSZ-1, ECR-30, Zeolite X, Zeolite Y, LZ-210, SAPO-37, ZSM-20, Na-X, US-Y, Na-Y, [Ga-Ge-O]-FAU, Li-LSX, [Ga-Al-Si-O]-FAU, and [Ga-Si-O]-FAU, including mixtures of two or more thereof, preferably from the group consisting of ZSM-3, Faujasite, CSZ-1, ECR-30, Zeolite X, Zeo- lite Y, LZ-210, ZSM-20, Na-X, US-Y, Na-Y, and Li-LSX, including mixtures of two or more thereof, more preferably from the group consisting of Faujasite, Zeolite
  • the mixture prepared in (1) further comprises one or more alkali metals M, preferably one or more alkali metals M selected from the group consisting of Na, K, and mixtures thereof, wherein more preferably the mixture prepared in (1) further comprises Na as the alkali metal M.
  • the M : Si atomic ratio of the one or more alkali metals M to Si contained in the mixture prepared in (1) is in the range of from 0.01 to 2.5, preferably of from 0.05 to 1.5, more preferably of from 0.1 to 1.0, more preferably of from 0.3 to 0.7, more preferably of from 0.4 to 0.5, and more preferably of from 0.45 to 0.47. 22.
  • heating in (2) is conducted at a tem- perature in the range of from 80 to 250 °C, preferably from 100 to 230 °C, more preferably from 110 to 220 °C, more preferably from 115 to 210 °C, more preferably from 120 to 200 °C, more preferably from 125 to 190 °C, more preferably from 130 to 180 °C, more prefer- ably from 135 to 170 °C, more preferably from 140 to 160 °C, and more preferably from 145 to 155 °C. 25.
  • the second zeolitic material obtained in (2) having an AEI-type framework structure is selected from the group consisting of SSZ-39, SAPO-18, SIZ-8, including mixtures of two or more thereof, wherein more prefer- ably the second zeolitic material obtained in (2) comprises SSZ-39, and wherein more preferably the second zeolitic material obtained in (2) is SSZ-39. 29.
  • any of embodiments 29 to 33 wherein calcining in (3) and/or (6) is con- ducted for a period in the range of from 0.5 to 10 h, preferably from 1 to 15 h, more prefer- ably from 2 to 12 h, more preferably from 3 to 9 h, more preferably from 4 to 7 h, more preferably from 4.5 to 6.5 h, and more preferably from 5 to 6 h. 35.
  • the mixture in (1) further comprises seed crystals, wherein the seed crystals preferably comprise a zeolitic material having an AEI-type framework structure, wherein more preferably the zeolitic material consists of a zeolitic material having an AEI-type framework structure.
  • FIG.1 displays the cis (chemical structure on the left hand side) and trans (chemical struc- ture on the right hand side) isomers of N,N-dimethyl-3,5-dimethylpiperidinium hy- droxide.
  • Fig.2 displays the results from catalyst testing using the AEI(100) zeolite samples from Reference Example 1 respectively loaded with different amounts of copper, wherein the N 2 O conversion in % is plotted along the ordinate, and the temperature in °C is plotted along the abscissa.
  • Fig.3 displays the results from catalyst testing using the AEI(20) zeolite samples from Ref- erence Example 1 respectively loaded with different amounts of copper, wherein the N 2 O conversion in % is plotted along the ordinate, and the temperature in °C is plot- ted along the abscissa.
  • EXPERIMENTAL SECTION Characterization methods XRD patterns were collected on a Rint-Ultima III (Rigaku) using a Cu K ⁇ X-ray source (40 kV, 20 mA). Elemental analyses of the samples were performed on an inductively coupled plasma-atomic emission spectrometer (ICP-AES, Shimadzu ICPE-9000).
  • Reference Example 1 Cu/AEI zeolite catalysts preparation
  • the AEI-type aluminosilicate zeolites were prepared by using N,N-dimethyl-3,5-dimethylpiperi- dinium hydroxide with different cis :trans isomer (see Figure 1) ratios (SACHEM, Inc.) as or- ganic structure directing agent (OSDA).
  • Fumed silica (Cab-O-Sil M5, Cabot) was added into the solution containing N,N-dimethyl-3,5-dimethylpiperidinium hydroxide, NaOH (8M, Wako) and ze- olite Y having an Si/Al atomic ratio of 2.4 (JRC-Z-HY4.8, JGC Catalysts and Chemicals Ltd).
  • the suspension with the molar composition of 1 SiO 2 : 0.017 Al 2 O 3 : 0.17 OSDA: 0.46 NaOH: 20 H 2 O was transferred to a Teflon-lined stainless-steel autoclave and crystallized at 150 °C for 3 days under tumbling condition.
  • the as-synthesized samples were recovered after filtering, washing and drying at 100 °C overnight.
  • the framework structure type of the zeolitic material obtained was verified by X-ray diffraction.
  • the samples prepared using the OSDA with 20% cis and 100% cis isomer (both obtained from SACHEM, Inc.) were designated as AEI(20) and AEI(100), respectively.
  • the OSDA was re- moved by calcination at 600 °C in air for 6 h. Then, the calcined samples were exchanged with 2.5 M NH 4 NO 3 aqueous solution at 80 °C for 3 h to obtain the NH4-form ones.
  • Example 1 Catalytic testing The continuous oxidation of methane reaction was performed in a fixed-bed flow reactor. In each run, 100 mg of catalyst in a granular form (particle size 500 ⁇ 1000 ⁇ m) was charged into a quartz tube (inner diameter 4 mm), which was placed in an electric tube furnace. The catalyst was pretreated at 500 °C for 1 h in an Ar and steam flow.
  • the reaction was conducted at the temperature ranging from 300 to 450 °C in a flowing gas mixture of CH4, N 2 O, H 2 O and Ar with flow rates of 10, 10, 2 and 3 mL ⁇ min ⁇ 1 .
  • the outlet gas, containing the products, unreacted CH 4 and N 2 O were analyzed using two on-line gas chromatographs (GC; GC-2014, Shimadzu).
  • GC on-line gas chromatographs
  • One of the GCs was used with a Shincarbon ST 50/80 packed column (3 mm ⁇ 6 m) and a TCD de- tector.
  • GC-TCD with a methanizer was used to detect H 2 , N 2 O, CO, CO 2 and CH 4 .
  • the AEI(100) zeo- lite samples i.e. the AEI-type zeolite obtained using the cis isomer of N,N-dimethyl-3,5-dime- thylpiperidinium hydroxide
  • the AEI(100) zeo- lite samples respectively loaded with different amounts of copper afford a comparatively low conversion of N 2 O with methane up to a tempera- ture of about 350 °C.
  • a substantial increase in the N 2 O conversion rate is observed, wherein said increase is particularly apparent for the sam- ples having a higher copper loading.
  • the intermediate sample with regard to copper loading displays a somewhat higher N 2 O conversion rate at 400 °C, yet a far lower N 2 O conversion rate at 450 °C compared to the results displayed in Figure 2 for the corresponding copper loaded AEI(100) ze- olite sample.
  • the sample with the highest copper loading displays a far higher N 2 O conversion rate at 400°C comparted to the result obtained at that temperature for the corresponding copper loaded AEI(100) zeolite sample. Accordingly, it has surprisingly been found that the inventive process allows for the activation of N 2 O to unprecedented levels for its controlled catalytic conversion.
  • the catalyst may display completely different N 2 O activation degrees at comparable loading of copper, such that catalytic conversion may be fine-tuned depending on the required activity for a given reac- tion at a given temperature, thus affording not only a highly effective, but also a highly versatile process for the activation of N 2 O for chemical conversion.
  • Cited Literature - US 5,958,370 - Moliner, M. et al. in Chem.

Landscapes

  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Organic Chemistry (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Geology (AREA)
  • General Life Sciences & Earth Sciences (AREA)
  • Materials Engineering (AREA)
  • Environmental & Geological Engineering (AREA)
  • Inorganic Chemistry (AREA)
  • Health & Medical Sciences (AREA)
  • Crystallography & Structural Chemistry (AREA)
  • Biomedical Technology (AREA)
  • Oil, Petroleum & Natural Gas (AREA)
  • General Chemical & Material Sciences (AREA)
  • Analytical Chemistry (AREA)
  • Catalysts (AREA)

Abstract

The present invention relates to a process for the activation of N2O comprising (i) providing a gas stream comprising N2O; (ii) contacting the gas stream provided in (i) with a catalyst at a temperature in the range of from 300 to 600 °C, wherein the catalyst comprises a zeolitic material having the AEI-type framework structure, wherein the framework structure of the zeolitic material comprises SiO2 and Al2O3, and wherein the zeolitic material contains copper.

Description

Process for the catalytic activation of N2O TECHNICAL FIELD The present invention relates to a process for the activation of N2O comprising contacting a gas stream containing N2O with a catalyst comprising a zeolitic material having the AEI-type frame- work structure, wherein the zeolitic material contains copper. INTRODUCTION Zeolitic materials having framework type AEI are known to be potentially effective as catalysts or catalyst components for treating combustion exhaust gas in industrial applications, for exam- ple for converting nitrogen oxides (NOx) in an exhaust gas stream. Synthetic AEI zeolitic materi- als are generally produced by precipitating crystals of the zeolitic material from a synthesis mix- ture which contains the sources of the elements from which the zeolitic framework is built, such as a source of silicon and a source of aluminum. An alternative approach may be the prepara- tion via zeolitic framework conversion according to which a starting material which is a suitable zeolitic material having a framework type other than AEI is suitably reacted to obtain the zeolitic material having framework type AEI. Thus, US 5,958,370 relates to SSZ-39 and to its preparation using cyclic or polycyclic quater- nary ammonium cations as templating agent. Moliner, M. et al. in Chem. Commun.2012, 48, pages 8264-8266, on the other hand, concerns Cu-SSZ-39 and its use for the SCR of nitrogen oxides NOx, wherein the SSZ-39 is produced with the use of N,N-dimethyl-3,5-dimethylpiperi- dinium cations as the organotemplate. Maruo, T. et al. in Chem. Lett.2014, 43, page 302-304 relates to the synthesis of AEI zeolites by hydrothermal conversion of FAU zeolites in the pres- ence of tetraethylphosphonium cations. Martín, N. et al. in Chem. Commun.2015, 51, 11030- 11033 concerns the synthesis of Cu-SSZ-39 and its use as a catalyst in the SCR of nitrogen ox- ides NOx. As regards the methods of synthesis of the SSZ-39 zeolite in said document, these include the use of N,N-dimethyl-3,5-dimethylpiperidinium cations as well as of tetrae- thylphosphonium cations. Dusselier, M. et al. in ACS Catal.2015, 5, 10, 6078-6085, on the other hand, describe methanol to olefin catalysis using hydrothermally treated SSZ-39. US 2015/0118150 A1 describes zeolite synthesis methods involving the use of N,N-dimethyl- 3,5-dimethylpiperidinium and N,N-dimethyl-2,6-dimethylpiperidinium cations, respectively. WO 2016/149234 A1 and Ransom, R. et al. in Ind. Eng. Chem. Res.2017, 56, 4350−4356 respec- tively relate to the synthesis of SSZ-39 via interzeolitic conversion of faujasite using N,N-dime- thyl-3,5-dimethylpiperidinium cations as the organotemplate. WO 2018/113566 A1, on the other hand, relates to the synthesis of zeolites via solvent-free interzeolitic conversion, wherein the synthesis of SSZ-39 from interzeolitic conversion of zeolite Y using N,N-dimethyl-2,6-dimethylpi- peridinium cations is described. WO 2016/149234 A1 and Ransom, R. et al. in Ind. Eng. Chem. Res.2017, 56, 4350-4356 re- spectively relate to the synthesis of SSZ-39 using different isomer ratios of the cis and trans iso- mers of the N,N-dimethyl-3,5-dimethylpiperidinium cation. WO 2020/098796 A1, on the other hand, concerns the production of an AEI-type zeolitic material via solvent-free interzeolitic con- version, wherein N,N-dimethyl-3,5-dimethylpiperidinium having a specific ratio of cis and trans isomers was employed. WO 2018/234044 A1 relates to a process for the oxidation of lower alkanes in the presence of ammonia over a copper loaded zeolite catalyst. Memioglu, O. et al., “A potential catalyst for continuous methane partial oxidation to methanol using N2O : Cu-SSZ-39”, Chem. Comm. 2021, 57, 1364-1367, on the other hand, describes the use of Cu-SSZ-39 as a catalyst for con- tinuous methane partial oxidation to methanol, wherein conversions are performed at 573 and 598 K (300 and 325 °C), respectively. WO 2017/134007 A1 concerns a method for the removal of nitrous oxide from an off gas over an iron loaded zeolite having the AEI-type framework structure. US 2016/264428 A1 discloses the production of zeolites by selective use of the trans isomer of 3,5-dimethyl-N,N-dimethylpiperidinium hydroxide, or of a mixture of cis and trans isomers with an enhanced content of the trans isomer. Despite the current applications involving the use of zeolitic material of the AEI-type framework structure, there remains the need for new applications which may further exploit the unique physical and chemical characteristics of this highly specific framework structure type among ze- olitic materials, in particular as a catalyst when used in conjunction with catalytically active tran- sition metals. DETAILED DESCRIPTION It was therefore the object of the present invention to provide novel applications for zeolitic ma- terials of the AEI-type framework structure when employed in conjunction with copper. Thus, it has surprisingly been found that at elevated temperatures, zeolitic materials of the AEI-type framework structure loaded with copper are able to activate N2O to the effect that it may react with reducing agents such as hydrocarbons to a substantial extent. In particular, it has unex- pectedly been found that activation of N2O with zeolitic materials of the AEI-type framework structure loaded with copper may even allow for near total to total conversion thereof in the presence of hydrocarbons such as methane as a reducing agent. Accordingly, it has surpris- ingly been found that AEI-type zeolitic materials loaded with copper may allow for the controlled conversion of N2O at elevated temperatures in chemical conversions such as the oxidation of hydrocarbons. Furthermore, it has unexpectedly been found that the use of specific isomer ra- tios among the chiral structure directing agents used in the synthesis of the AEI-type framework structure leads to striking differences in the rate of N2O activation, in particular in the intermedi- ate temperature ranges. The present invention therefore relates to a process for the activation of N2O comprising (i) providing a gas stream comprising N2O; (ii) contacting the gas stream provided in (i) with a catalyst at a temperature in the range of from 300 to 600 °C, wherein the catalyst comprises a zeolitic material having the AEI-type framework structure, wherein the framework structure of the zeolitic material comprises SiO2 and Al2O3, and wherein the zeolitic material contains copper. It is preferred that the gas stream in (i) contains N2O in an amount ranging from 1 to 100 vol.-%, more preferably from 5 to 90 vol.-%, more preferably from 10 to 80 vol.-%, more preferably from 15 to 70 vol.-%, more preferably from 20 to 60 vol.-%, more preferably from 25 to 55 vol.-%, more preferably from 30 to 50 vol.-%, more preferably from 35 to 45 vol.-%, and more prefera- bly from 38 to 42 vol.-%. It is preferred that the gas stream in (i) further comprises a reducing agent. It is preferred that the reducing agent is selected from the group consisting of hydrocarbons, more preferably from the group consisting of (C1-C8)alkanes, more preferably from the group consisting of (C1-C7)alkanes, including mixtures of two or more thereof, more preferably from the group consisting of (C1-C6)alkanes, including mixtures of two or more thereof, more prefera- bly from the group consisting of (C1-C5)alkanes, including mixtures of two or more thereof, more preferably from the group consisting of (C1-C4)alkanes, including mixtures of two or more thereof, more preferably from the group consisting of (C1-C3)alkanes, including mixtures of two or more thereof, more preferably from the group consisting of (C1-C2)alkanes, including mixtures of two or more thereof, more preferably from the group consisting of methane and ethane, in- cluding mixtures thereof, wherein more preferably the reducing agent comprises methane, wherein more preferably the reducing agent is methane. It is preferred that contacting in (ii) of the gas stream provided in (i) with a catalyst is conducted at a temperature in the range of from 350 to 550 °C, more preferably of from 400 to 550 °C, and more preferably of from 450 to 500 °C. It is preferred that the SiO2 : Al2O3 molar ratio of the zeolitic material having the AEI-type frame- work structure is in the range of from 4 to 200, more preferably of from 6 to 120, more prefera- bly of from 8 to 80, more preferably of from 10 to 50, more preferably of from 12 to 35, more preferably of from 14 to 30, more preferably of from 16 to 25, more preferably of from 18 to 22, and more preferably of from 19.5 to 20.5. It is preferred that the zeolitic material having the AEI-type framework structure is ion ex- changed with copper. It is preferred that the zeolitic material having the AEI-type framework structure contains copper in an amount in the range of from 0.1 to 12 wt.-% based on 100 wt.-% of the zeolitic material having the AEI-type framework structure, wherein copper is calculated as the element, wherein more preferably the zeolitic material having the AEI-type framework structure contains copper in an amount in the range of from 0.3 to 10 wt.-%, more preferably of from 0.5 to 8 wt.-%, more preferably of from 0.7 to 6 wt.-%, more preferably of from 0.9 to 4 wt.-%, more preferably of from 1.1 to 3 wt.-%, more preferably of from 1.3 to 2.5 wt.-%, more preferably of from 1.5 to 2.3 wt.- %, more preferably of from 1.7 to 2 wt.-%, and more preferably of from 1.8 to 1.9 wt.-% based on 100 wt.-% of the zeolitic material having the AEI-type framework structure. It is preferred that the zeolitic material having the AEI-type framework structure comprised in the catalyst is prepared by a process comprising (1) preparing a mixture comprising one or more sources of SiO2, a first zeolitic material com- prising SiO2 and Al2O3 in its framework structure and having an FAU-type framework structure, one or more cationic structure directing agents, and water; (2) heating the mixture obtained in (1) for obtaining a second zeolitic material comprising SiO2 and Al2O3 in its framework structure and having an AEI-type framework structure. In the case where the zeolitic material having the AEI-type framework structure comprised in the catalyst is prepared by a process comprising (1) and (2) as defined hereinabove, it is preferred that the one or more cationic structure directing agents are selected from the group consisting of N,N-di(C1-C4)alkyl-3,5-di(C1-C4)alkylpyrrolidinium, N,N-di(C1-C4)alkyl-3,5-di(C1-C4)alkylpiperi- dinium, N,N-di(C1-C4)alkyl-3,5-di(C1-C4)alkylhexahydroazepinium, and mixtures of two or more thereof, more preferably from the group consisting of N,N-di(C1-C3)alkyl-3,5-di(C1-C3)alkylpyrrolidinium, N,N-di(C1-C3)alkyl-3,5-di(C1-C3)alkylpiperidinium, N,N-di(C1-C3)alkyl-3,5-di(C1-C3)alkylhexahy- droazepinium, and mixtures of two or more thereof, more preferably from the group consisting of N,N-di(C1-C2)alkyl-3,5-di(C1-C2)alkylpyrrolidinium , N,N-di(C1-C2)alkyl-3,5-di(C1-C2)alkylpiperidinium, N,N-di(C1-C2)alkyl-3,5-di(C1-C2)alkylhexahy- droazepinium, and mixtures of two or more thereof, more preferably from the group consisting of N,N-di(C1-C2)alkyl-3,5-di(C1-C2)alkylpiperidinium, and mixtures of two or more thereof, wherein more preferably the one or more cationic structure directing agents comprises N,N-dimethyl-3,5-dimethylpiperidinium, wherein more preferably the one or more cationic structure directing agents consists of N,N-dimethyl-3,5-dimethylpiperi- dinium. In the case where the one or more cationic structure directing agents are selected from the group consisting of N,N-di(C1-C4)alkyl-3,5-di(C1-C4)alkylpyrrolidinium, N,N-di(C1-C4)alkyl-3,5- di(C1-C4)alkylpiperidinium, N,N-di(C1-C4)alkyl-3,5-di(C1-C4)alkylhexahydroazepinium, and mix- tures of two or more thereof, it is preferred according to a first alternative that the cis : trans mo- lar ratio of the cis isomer to the trans isomer in the one or more cationic structure directing agents relative to the alkyl groups at the 3 and 5 positions of the heterocyclic amine ring is in the range of from 0.01:1 to 0.95:1, more preferably of from 0.03:1 to 0.9:1, more preferably of from 0.05:1 to 0.7:1, more preferably of from 0.07:1 to 0.5:1, more preferably of from 0.1:1 to 0.45:1, more preferably of from 0.13:1 to 0.4:1, more preferably of from 0.15:1 to 0.35:1, more preferably of from 0.18:1 to 0.33:1, more preferably of from 0.2:1 to 0.3:1, and more preferably of from 0.23:1 to 0.27:1. In the case where the one or more cationic structure directing agents are selected from the group consisting of N,N-di(C1-C4)alkyl-3,5-di(C1-C4)alkylpyrrolidinium, N,N-di(C1-C4)alkyl-3,5- di(C1-C4)alkylpiperidinium, N,N-di(C1-C4)alkyl-3,5-di(C1-C4)alkylhexahydroazepinium, and mix- tures of two or more thereof, it is preferred according to a second alternative that the trans : cis molar ratio of the trans isomer to the cis isomer in the one or more cationic structure directing agents relative to the alkyl groups at the 3 and 5 positions of the heterocyclic amine ring is in the range of from 1:1 to 0:1, more preferably of from 0.8:1 to 0:1, more preferably of from 0.5:1 to 0:1, more preferably of from 0.4:1 to 0:1, more preferably of from 0.3:1 to 0:1, more prefera- bly of from 0.2:1 to 0:1, more preferably of from 0.1:1 to 0:1, more preferably of from 0.05:1 to 0:1, and more preferably of from 0.01:1 to 0:1. Further in the case where the zeolitic material having the AEI-type framework structure com- prised in the catalyst is prepared by a process comprising (1) and (2) as defined hereinabove, it is preferred that the one or more cationic structure directing agents are provided as salts, pref- erably as one or more salts selected from the group consisting of halides, sulfate, nitrate, phos- phate, acetate, and mixtures of two or more thereof, more preferably from the group consisting of bromide, chloride, hydroxide, sulfate, and mixtures of two or more thereof, wherein more pref- erably the one or more cationic structure directing agents are provided as hydroxides and/or bromides, and more preferably as hydroxides. Further in the case where the zeolitic material having the AEI-type framework structure com- prised in the catalyst is prepared by a process comprising (1) and (2) as defined hereinabove, it is preferred that the framework structure of the first zeolitic material displays a SiO2 : Al2O3 mo- lar ratio ranging from 1.5 to 100, more preferably of from 2 to 50, more preferably of from 2.5 to 25, more preferably of from 3 to 15, more preferably of from 3.5 to 10, more preferably of from 4 to 7, and more preferably of from 4.5 to 5. Further in the case where the zeolitic material having the AEI-type framework structure com- prised in the catalyst is prepared by a process comprising (1) and (2) as defined hereinabove, it is preferred that the mixture prepared in (1) and heated in (2) displays an SDA : Si molar ratio of the one or more cationic structure directing agents (SDA) to Si contained in the mixture in the range of from 0.01 to 1.5, more preferably of from 0.05 to 1.2, more preferably of from 0.1 to 0.8, more preferably of from 0.3 to 0.6, more preferably of from 0.5 to 0.45, more preferably of from 0.8 to 0.35, more preferably of from 0.1 to 0.3, more preferably of from 0.13 to 0.25, and more preferably of from 0.15 to 0.2. Further in the case where the zeolitic material having the AEI-type framework structure com- prised in the catalyst is prepared by a process comprising (1) and (2) as defined hereinabove, it is preferred that the one or more sources of SiO2 is selected from the group consisting of fumed silica, silica hydrosols, reactive amorphous solid silicas, silica gel, silicic acid, water glass, so- dium metasilicate hydrate, sesquisilicate, disilicate, colloidal silica, silicic acid esters, and mix- tures of two or more thereof, more preferably from the group consisting of fumed silica, silica hy- drosols, reactive amorphous solid silicas, silica gel, silicic acid, colloidal silica, silicic acid esters, and mixtures of two or more thereof, more preferably from the group consisting of fumed silica, silica hydrosols, reactive amorphous solid silicas, silica gel, colloidal silica, and mixtures of two or more thereof, wherein even more preferably the one or more sources for YO2 comprises fumed silica and/or colloidal silica, preferably fumed silica. Further in the case where the zeolitic material having the AEI-type framework structure com- prised in the catalyst is prepared by a process comprising (1) and (2) as defined hereinabove, it is preferred that the first zeolitic material having an FAU-type framework structure is selected from the group consisting of ZSM-3, Faujasite, [Al-Ge-O]-FAU, CSZ-1, ECR-30, Zeolite X, Zeo- lite Y, LZ-210, SAPO-37, ZSM-20, Na-X, US-Y, Na-Y, [Ga-Ge-O]-FAU, Li-LSX, [Ga-Al-Si-O]- FAU, and [Ga-Si-O]-FAU, including mixtures of two or more thereof, more preferably from the group consisting of ZSM-3, Faujasite, CSZ-1, ECR-30, Zeolite X, Zeo- lite Y, LZ-210, ZSM-20, Na-X, US-Y, Na-Y, and Li-LSX, including mixtures of two or more thereof, more preferably from the group consisting of Faujasite, Zeolite X, Zeolite Y, Na-X, US-Y, and Na-Y, including mixtures of two or more thereof, more preferably from the group consisting of Faujasite, Zeolite X, and Zeolite Y, including mix- tures of two or more thereof, wherein more preferably the first zeolitic material having an FAU-type framework structure com- prises zeolite X and/or zeolite Y, preferably zeolite Y, wherein more preferably the first zeolitic material having an FAU-type framework structure is ze- olite X and/or zeolite Y, preferably zeolite Y. Further in the case where the zeolitic material having the AEI-type framework structure com- prised in the catalyst is prepared by a process comprising (1) and (2) as defined hereinabove, it is preferred that the mixture prepared in (1) further comprises OH-. In the case where the mixture prepared in (1) further comprises OH-, it is preferred that the OH- : Si molar ratio of hydroxide to Si contained in the mixture prepared in (1) is in the range of from 0.01 to 5, more preferably from 0.05 to 3, more preferably from 0.1 to 1.5, more preferably from 0.2 to 1, more preferably from 0.3 to 0.8, and more preferably from 0.5 to 0.7, and more prefera- bly from 0.6 to 0.65. Further in the case where the zeolitic material having the AEI-type framework structure com- prised in the catalyst is prepared by a process comprising (1) and (2) as defined hereinabove, it is preferred that the mixture prepared in (1) further comprises one or more alkali metals M, more preferably one or more alkali metals M selected from the group consisting of Na, K, and mix- tures thereof, wherein more preferably the mixture prepared in (1) further comprises Na as the alkali metal M. In the case where the mixture prepared in (1) further comprises one or more alkali metals M, it is preferred that the M : Si atomic ratio of the one or more alkali metals M to Si contained in the mixture prepared in (1) is in the range of from 0.01 to 2.5, more preferably of from 0.05 to 1.5, more preferably of from 0.1 to 1.0, more preferably of from 0.3 to 0.7, more preferably of from 0.4 to 0.5, and more preferably of from 0.45 to 0.47. Further in the case where the mixture prepared in (1) further comprises one or more alkali met- als M, it is preferred that the one or more alkali metals M are comprised in the mixture prepared in (1) as hydroxide. Further in the case where the zeolitic material having the AEI-type framework structure com- prised in the catalyst is prepared by a process comprising (1) and (2) as defined hereinabove, it is preferred that the mixture prepared in (1) contains water at an H2O : Si molar ratio in the range of from 1 to 60, more preferably of from 5 to 40, more preferably of from 10 to 30, more preferably of from 15 to 25, and more preferably of from 18 to 22. Further in the case where the zeolitic material having the AEI-type framework structure com- prised in the catalyst is prepared by a process comprising (1) and (2) as defined hereinabove, it is preferred that heating in (2) is conducted at a temperature in the range of from 80 to 250 °C, more preferably from 100 to 230 °C, more preferably from 110 to 220 °C, more preferably from 115 to 210 °C, more preferably from 120 to 200 °C, more preferably from 125 to 190 °C, more preferably from 130 to 180 °C, more preferably from 135 to 170 °C, more preferably from 140 to 160 °C, and more preferably from 145 to 155 °C. Further in the case where the zeolitic material having the AEI-type framework structure com- prised in the catalyst is prepared by a process comprising (1) and (2) as defined hereinabove, it is preferred that heating in (2) is conducted under autogenous pressure, more preferably under hydrothermal conditions. Further in the case where the zeolitic material having the AEI-type framework structure com- prised in the catalyst is prepared by a process comprising (1) and (2) as defined hereinabove, it is preferred that the heating in (2) is performed in a pressure tight vessel, more preferably in an autoclave. Further in the case where the zeolitic material having the AEI-type framework structure com- prised in the catalyst is prepared by a process comprising (1) and (2) as defined hereinabove, it is preferred that heating in (2) is conducted for a duration in the range of from 3 h to 10 d, more preferably from 6 h to 8 d, more preferably from 12 h to 6 d, more preferably from 1 to 5 d, more preferably from 1.5 to 4.5 d, more preferably from 2 to 4 d, and more preferably from 2.5 to 3.5 d. Further in the case where the zeolitic material having the AEI-type framework structure com- prised in the catalyst is prepared by a process comprising (1) and (2) as defined hereinabove, it is preferred that the second zeolitic material obtained in (2) having an AEI-type framework struc- ture is selected from the group consisting of SSZ-39, SAPO-18, SIZ-8, including mixtures of two or more thereof, wherein more preferably the second zeolitic material obtained in (2) comprises SSZ-39, and wherein more preferably the second zeolitic material obtained in (2) is SSZ-39. Further in the case where the zeolitic material having the AEI-type framework structure com- prised in the catalyst is prepared by a process comprising (1) and (2) as defined hereinabove, it is preferred that the process further comprises (3) calcining the second zeolitic material obtained in (2). Further in the case where the zeolitic material having the AEI-type framework structure com- prised in the catalyst is prepared by a process comprising (1) and (2) as defined hereinabove, it is preferred that the process further comprises (4) subjecting the zeolitic material obtained in (2) or (3) to an ion-exchange procedure, wherein one or more ionic extra-framework elements contained in the zeolite framework is ion- exchanged against H+ and/or NH4 +, more preferably against NH4 +. Further in the case where the zeolitic material having the AEI-type framework structure com- prised in the catalyst is prepared by a process comprising (1) and (2) as defined hereinabove, it is preferred that the process further comprises (5) subjecting the zeolitic material obtained in (2), (3), or (4) to an ion-exchange procedure, wherein one or more ionic extra-framework elements contained in the zeolite framework is ion- exchanged against copper. In the case where the process further comprises (5) as defined hereinabove, it is preferred that the process further comprises (6) calcining the zeolitic material obtained in (5). In the case where the process further comprises (3) and/or (6) as defined herein above, it is preferred that the temperature of calcination in (3) and/or (6) is in the range of from 300 to 900 °C, more preferably of from 400 to 700 °C, more preferably of from 450 to 650 °C, and more preferably of from 500 to 600 °C. Further in the case where the process further comprises (3) and/or (6) as defined herein above, it is preferred that calcining in (3) and/or (6) is conducted for a period in the range of from 0.5 to 10 h, more preferably from 1 to 15 h, more preferably from 2 to 12 h, more preferably from 3 to 9 h, more preferably from 4 to 7 h, more preferably from 4.5 to 6.5 h, and more preferably from 5 to 6 h. Further in the case where the zeolitic material having the AEI-type framework structure com- prised in the catalyst is prepared by a process comprising (1) and (2) as defined hereinabove, it is preferred that the mixture in (1) further comprises seed crystals, wherein the seed crystals more preferably comprise a zeolitic material having an AEI-type framework structure, wherein more preferably the zeolitic material consists of a zeolitic material having an AEI-type framework structure. In the case where the mixture in (1) further comprises seed crystals, it is preferred that the zeo- litic material having an AEI-type framework structure comprised in the seed crystals is selected from the group consisting of SSZ-39, SAPO-18, SIZ-8, including mixtures of two or more thereof, wherein more preferably the zeolitic material having an AEI-type framework structure comprised in the seed crystals is SSZ-39. Further in the case where the mixture in (1) further comprises seed crystals, it is preferred that the amount of seed crystals in the mixture prepared in (1) and heated in (2) ranges from 3 to 12 wt.-% based on 100 wt.-% of Si in the mixture prepared in (1) calculated as the element, more preferably from 3.5 to 10 wt.-%, more preferably from 4 to 9 wt.-%, more preferably from 4.5 to 7 wt.-%, and more preferably from 5 to 6 wt.-% based on 100 wt.-% of Si in the mixture prepared in (1) calculated as the element. The present invention is further illustrated by the following set of embodiments and combina- tions of embodiments resulting from the dependencies and back-references as indicated. In par- ticular, it is noted that in each instance where a range of embodiments is mentioned, for exam- ple in the context of a term such as "The composite oxide of any one of embodiments 1 to 4", every embodiment in this range is meant to be explicitly disclosed for the skilled person, i.e. the wording of this term is to be understood by the skilled person as being synonymous to "The composite oxide of any one of embodiments 1, 2, 3, and 4". Further, it is explicitly noted that the following set of embodiments is not the set of claims determining the extent of protection, but represents a suitably structured part of the description directed to general and preferred aspects of the present invention. 1. A process for the activation of N2O comprising (i) providing a gas stream comprising N2O; (ii) contacting the gas stream provided in (i) with a catalyst at a temperature in the range of from 300 to 600 °C, wherein the catalyst comprises a zeolitic material having the AEI-type framework structure, wherein the framework structure of the zeolitic material comprises SiO2 and Al2O3, and wherein the zeolitic material contains copper. 2. The process of embodiment 1, wherein the gas stream in (i) contains N2O in an amount ranging from 1 to 100 vol.-%, preferably from 5 to 90 vol.-%, more preferably from 10 to 80 vol.-%, more preferably from 15 to 70 vol.-%, more preferably from 20 to 60 vol.-%, more preferably from 25 to 55 vol.-%, more preferably from 30 to 50 vol.-%, more prefera- bly from 35 to 45 vol.-%, and more preferably from 38 to 42 vol.-%. 3. The process of embodiment 1 or 2, wherein the gas stream in (i) further comprises a re- ducing agent. 4. The process of any of embodiments 1 to 3, wherein the reducing agent is selected from the group consisting of hydrocarbons, preferably from the group consisting of (C1-C8)al- kanes, more preferably from the group consisting of (C1-C7)alkanes, including mixtures of two or more thereof, more preferably from the group consisting of (C1-C6)alkanes, includ- ing mixtures of two or more thereof, more preferably from the group consisting of (C1- C5)alkanes, including mixtures of two or more thereof, more preferably from the group consisting of (C1-C4)alkanes, including mixtures of two or more thereof, more preferably from the group consisting of (C1-C3)alkanes, including mixtures of two or more thereof, more preferably from the group consisting of (C1-C2)alkanes, including mixtures of two or more thereof, more preferably from the group consisting of methane and ethane, including mixtures thereof, wherein more preferably the reducing agent comprises methane, wherein more preferably the reducing agent is methane. 5. The process of any of embodiments 1 to 4, wherein contacting in (ii) of the gas stream provided in (i) with a catalyst is conducted at a temperature in the range of from 350 to 550 °C, preferably of from 400 to 550 °C, and more preferably of from 450 to 500 °C. 6. The process of any of embodiments 1 to 5, wherein the SiO2 : Al2O3 molar ratio of the zeo- litic material having the AEI-type framework structure is in the range of from 4 to 200, pref- erably of from 6 to 120, more preferably of from 8 to 80, more preferably of from 10 to 50, more preferably of from 12 to 35, more preferably of from 14 to 30, more preferably of from 16 to 25, more preferably of from 18 to 22, and more preferably of from 19.5 to 20.5. 7. The process of any of embodiments 1 to 6, wherein the zeolitic material having the AEI- type framework structure is ion exchanged with copper. 8. The process of any of embodiments 1 to 7, wherein the zeolitic material having the AEI- type framework structure contains copper in an amount in the range of from 0.1 to 12 wt.- % based on 100 wt.-% of the zeolitic material having the AEI-type framework structure, wherein copper is calculated as the element, wherein preferably the zeolitic material hav- ing the AEI-type framework structure contains copper in an amount in the range of from 0.3 to 10 wt.-%, more preferably of from 0.5 to 8 wt.-%, more preferably of from 0.7 to 6 wt.-%, more preferably of from 0.9 to 4 wt.-%, more preferably of from 1.1 to 3 wt.-%, more preferably of from 1.3 to 2.5 wt.-%, more preferably of from 1.5 to 2.3 wt.-%, more preferably of from 1.7 to 2 wt.-%, and more preferably of from 1.8 to 1.9 wt.-% based on 100 wt.-% of the zeolitic material having the AEI-type framework structure. 9. The process of any of embodiments 1 to 8, wherein the zeolitic material having the AEI- type framework structure comprised in the catalyst is prepared by a process comprising (1) preparing a mixture comprising one or more sources of SiO2, a first zeolitic material comprising SiO2 and Al2O3 in its framework structure and having an FAU-type framework structure, one or more cationic structure directing agents, and water; (2) heating the mixture obtained in (1) for obtaining a second zeolitic material compris- ing SiO2 and Al2O3 in its framework structure and having an AEI-type framework structure. 10. The process of embodiment 9, wherein the one or more cationic structure directing agents are selected from the group consisting of N,N-di(C1-C4)alkyl-3,5-di(C1-C4)alkylpyrroli- dinium, N,N-di(C1-C4)alkyl-3,5-di(C1-C4)alkylpiperidinium, N,N-di(C1-C4)alkyl-3,5-di(C1- C4)alkylhexahydroazepinium, and mixtures of two or more thereof, preferably from the group consisting of N,N-di(C1-C3)alkyl-3,5-di(C1-C3)alkylpyrrolidinium, N,N-di(C1-C3)alkyl-3,5-di(C1-C3)alkylpiperidinium, N,N-di(C1-C3)alkyl-3,5-di(C1-C3)alkylhex- ahydroazepinium, and mixtures of two or more thereof, more preferably from the group consisting of N,N-di(C1-C2)alkyl-3,5-di(C1-C2)alkylpyrroli- dinium, N,N-di(C1-C2)alkyl-3,5-di(C1-C2)alkylpiperidinium, N,N-di(C1-C2)alkyl-3,5-di(C1- C2)alkylhexahydroazepinium, and mixtures of two or more thereof, more preferably from the group consisting of N,N-di(C1-C2)alkyl-3,5-di(C1-C2)alkylpiperi- dinium, and mixtures of two or more thereof, wherein more preferably the one or more cat- ionic structure directing agents comprises N,N-dimethyl-3,5-dimethylpiperidinium, wherein more preferably the one or more cationic structure directing agents consists of N,N-dime- thyl-3,5-dimethylpiperidinium. 11. The process of embodiment 10, wherein the cis : trans molar ratio of the cis isomer to the trans isomer in the one or more cationic structure directing agents relative to the alkyl groups at the 3 and 5 positions of the heterocyclic amine ring is in the range of from 0.01:1 to 0.95:1, preferably of from 0.03:1 to 0.9:1, more preferably of from 0.05:1 to 0.7:1, more preferably of from 0.07:1 to 0.5:1, more preferably of from 0.1:1 to 0.45:1, more pref- erably of from 0.13:1 to 0.4:1, more preferably of from 0.15:1 to 0.35:1, more preferably of from 0.18:1 to 0.33:1, more preferably of from 0.2:1 to 0.3:1, and more preferably of from 0.23:1 to 0.27:1. 12. The process of embodiment 10, wherein the trans : cis molar ratio of the trans isomer to the cis isomer in the one or more cationic structure directing agents relative to the alkyl groups at the 3 and 5 positions of the heterocyclic amine ring is in the range of from 1:1 to 0:1, preferably of from 0.8:1 to 0:1, more preferably of from 0.5:1 to 0:1, more preferably of from 0.4:1 to 0:1, more preferably of from 0.3:1 to 0:1, more preferably of from 0.2:1 to 0:1, more preferably of from 0.1:1 to 0:1, more preferably of from 0.05:1 to 0:1, and more preferably of from 0.01:1 to 0:1. 13. The process of any of embodiments 9 to 12, wherein the one or more cationic structure directing agents are provided as salts, preferably as one or more salts selected from the group consisting of halides, sulfate, nitrate, phosphate, acetate, and mixtures of two or more thereof, more preferably from the group consisting of bromide, chloride, hydroxide, sulfate, and mixtures of two or more thereof, wherein more preferably the one or more cat- ionic structure directing agents are provided as hydroxides and/or bromides, and more preferably as hydroxides. 14. The process of any of embodiments 9 to 13, wherein the framework structure of the first zeolitic material displays a SiO2 : Al2O3 molar ratio ranging from 1.5 to 100, preferably of from 2 to 50, more preferably of from 2.5 to 25, more preferably of from 3 to 15, more pref- erably of from 3.5 to 10, more preferably of from 4 to 7, and more preferably of from 4.5 to 5. 15. The process of any of embodiments 9 to 14, wherein the mixture prepared in (1) and heated in (2) displays an SDA : Si molar ratio of the one or more cationic structure direct- ing agents (SDA) to Si contained in the mixture in the range of from 0.01 to 1.5, preferably of from 0.05 to 1.2, more preferably of from 0.1 to 0.8, more preferably of from 0.3 to 0.6, more preferably of from 0.5 to 0.45, more preferably of from 0.8 to 0.35, more preferably of from 0.1 to 0.3, more preferably of from 0.13 to 0.25, and more preferably of from 0.15 to 0.2. 16. The process of any of embodiments 9 to 15, wherein the one or more sources of SiO2 is selected from the group consisting of fumed silica, silica hydrosols, reactive amorphous solid silicas, silica gel, silicic acid, water glass, sodium metasilicate hydrate, sesquisilicate, disilicate, colloidal silica, silicic acid esters, and mixtures of two or more thereof, preferably from the group consisting of fumed silica, silica hydrosols, reactive amorphous solid sili- cas, silica gel, silicic acid, colloidal silica, silicic acid esters, and mixtures of two or more thereof, more preferably from the group consisting of fumed silica, silica hydrosols, reac- tive amorphous solid silicas, silica gel, colloidal silica, and mixtures of two or more thereof, wherein even more preferably the one or more sources for YO2 comprises fumed silica and/or colloidal silica, preferably fumed silica. 17. The process of any of embodiments 9 to 16, wherein the first zeolitic material having an FAU-type framework structure is selected from the group consisting of ZSM-3, Faujasite, [Al-Ge-O]-FAU, CSZ-1, ECR-30, Zeolite X, Zeolite Y, LZ-210, SAPO-37, ZSM-20, Na-X, US-Y, Na-Y, [Ga-Ge-O]-FAU, Li-LSX, [Ga-Al-Si-O]-FAU, and [Ga-Si-O]-FAU, including mixtures of two or more thereof, preferably from the group consisting of ZSM-3, Faujasite, CSZ-1, ECR-30, Zeolite X, Zeo- lite Y, LZ-210, ZSM-20, Na-X, US-Y, Na-Y, and Li-LSX, including mixtures of two or more thereof, more preferably from the group consisting of Faujasite, Zeolite X, Zeolite Y, Na-X, US-Y, and Na-Y, including mixtures of two or more thereof, more preferably from the group consisting of Faujasite, Zeolite X, and Zeolite Y, including mixtures of two or more thereof, wherein more preferably the first zeolitic material having an FAU-type framework structure comprises zeolite X and/or zeolite Y, preferably zeolite Y, wherein more preferably the first zeolitic material having an FAU-type framework structure is zeolite X and/or zeolite Y, preferably zeolite Y. 18. The process of any of embodiments 9 to 17, wherein the mixture prepared in (1) further comprises OH-. 19. The process of embodiment 18, wherein the OH- : Si molar ratio of hydroxide to Si con- tained in the mixture prepared in (1) is in the range of from 0.01 to 5, preferably from 0.05 to 3, more preferably from 0.1 to 1.5, more preferably from 0.2 to 1, more preferably from 0.3 to 0.8, and more preferably from 0.5 to 0.7, and more preferably from 0.6 to 0.65. 20. The process of any of embodiments 9 to 19, wherein the mixture prepared in (1) further comprises one or more alkali metals M, preferably one or more alkali metals M selected from the group consisting of Na, K, and mixtures thereof, wherein more preferably the mixture prepared in (1) further comprises Na as the alkali metal M. 21. The process of embodiment 20, wherein the M : Si atomic ratio of the one or more alkali metals M to Si contained in the mixture prepared in (1) is in the range of from 0.01 to 2.5, preferably of from 0.05 to 1.5, more preferably of from 0.1 to 1.0, more preferably of from 0.3 to 0.7, more preferably of from 0.4 to 0.5, and more preferably of from 0.45 to 0.47. 22. The process of embodiment 20 or 21, wherein the one or more alkali metals M are com- prised in the mixture prepared in (1) as hydroxide. 23. The process of any of embodiments 9 to 22, wherein the mixture prepared in (1) contains water at an H2O : Si molar ratio in the range of from 1 to 60, preferably of from 5 to 40, more preferably of from 10 to 30, more preferably of from 15 to 25, and more preferably of from 18 to 22. 24. The process of any of embodiments 9 to 23, wherein heating in (2) is conducted at a tem- perature in the range of from 80 to 250 °C, preferably from 100 to 230 °C, more preferably from 110 to 220 °C, more preferably from 115 to 210 °C, more preferably from 120 to 200 °C, more preferably from 125 to 190 °C, more preferably from 130 to 180 °C, more prefer- ably from 135 to 170 °C, more preferably from 140 to 160 °C, and more preferably from 145 to 155 °C. 25. The process of any of embodiments 9 to 24, wherein heating in (2) is conducted under au- togenous pressure, preferably under hydrothermal conditions. 26. The process of any of embodiments 9 to 25, wherein the heating in (2) is performed in a pressure tight vessel, preferably in an autoclave. 27. The process of any of embodiments 9 to 26, wherein heating in (2) is conducted for a du- ration in the range of from 3 h to 10 d, preferably from 6 h to 8 d, more preferably from 12 h to 6 d, more preferably from 1 to 5 d, more preferably from 1.5 to 4.5 d, more preferably from 2 to 4 d, and more preferably from 2.5 to 3.5 d. 28. The process of any of embodiments 9 to 27, wherein the second zeolitic material obtained in (2) having an AEI-type framework structure is selected from the group consisting of SSZ-39, SAPO-18, SIZ-8, including mixtures of two or more thereof, wherein more prefer- ably the second zeolitic material obtained in (2) comprises SSZ-39, and wherein more preferably the second zeolitic material obtained in (2) is SSZ-39. 29. The process of any of embodiments 9 to 28, further comprising (3) calcining the second zeolitic material obtained in (2). 30. The process of any of embodiments 9 to 29, further comprising (4) subjecting the zeolitic material obtained in (2) or (3) to an ion-exchange procedure, wherein one or more ionic extra-framework elements contained in the zeolite framework is ion-exchanged against H+ and/or NH4 +, more preferably against NH4 +. 31. The process of any of embodiments 9 to 30, further comprising (5) subjecting the zeolitic material obtained in (2), (3), or (4) to an ion-exchange proce- dure, wherein one or more ionic extra-framework elements contained in the zeolite frame- work is ion-exchanged against copper. 32. The process of embodiment 31, further comprising (6) calcining the zeolitic material obtained in (5). 33. The process of any of embodiments 29 to 32, wherein the temperature of calcination in (3) and/or (6) is in the range of from 300 to 900°C, preferably of from 400 to 700°C, more preferably of from 450 to 650°C, and more preferably of from 500 to 600°C. 34. The process of any of embodiments 29 to 33, wherein calcining in (3) and/or (6) is con- ducted for a period in the range of from 0.5 to 10 h, preferably from 1 to 15 h, more prefer- ably from 2 to 12 h, more preferably from 3 to 9 h, more preferably from 4 to 7 h, more preferably from 4.5 to 6.5 h, and more preferably from 5 to 6 h. 35. The process of any of embodiments 9 to 34, wherein the mixture in (1) further comprises seed crystals, wherein the seed crystals preferably comprise a zeolitic material having an AEI-type framework structure, wherein more preferably the zeolitic material consists of a zeolitic material having an AEI-type framework structure. 36. The process of embodiment 35, wherein the zeolitic material having an AEI-type frame- work structure comprised in the seed crystals is selected from the group consisting of SSZ-39, SAPO-18, SIZ-8, including mixtures of two or more thereof, wherein preferably the zeolitic material having an AEI-type framework structure comprised in the seed crystals is SSZ-39. 37. The process of embodiment 35 or 36, wherein the amount of seed crystals in the mixture prepared in (1) and heated in (2) ranges from 3 to 12 wt.-% based on 100 wt.-% of Si in the mixture prepared in (1) calculated as the element, preferably from 3.5 to 10 wt.-%, more preferably from 4 to 9 wt.-%, more preferably from 4.5 to 7 wt.-%, and more prefera- bly from 5 to 6 wt.-% based on 100 wt.-% of Si in the mixture prepared in (1) calculated as the element. DESCRIPTION OF THE FIGURES Fig.1 displays the cis (chemical structure on the left hand side) and trans (chemical struc- ture on the right hand side) isomers of N,N-dimethyl-3,5-dimethylpiperidinium hy- droxide. Fig.2 displays the results from catalyst testing using the AEI(100) zeolite samples from Reference Example 1 respectively loaded with different amounts of copper, wherein the N2O conversion in % is plotted along the ordinate, and the temperature in °C is plotted along the abscissa. Fig.3 displays the results from catalyst testing using the AEI(20) zeolite samples from Ref- erence Example 1 respectively loaded with different amounts of copper, wherein the N2O conversion in % is plotted along the ordinate, and the temperature in °C is plot- ted along the abscissa. EXPERIMENTAL SECTION Characterization methods XRD patterns were collected on a Rint-Ultima III (Rigaku) using a Cu Kα X-ray source (40 kV, 20 mA). Elemental analyses of the samples were performed on an inductively coupled plasma-atomic emission spectrometer (ICP-AES, Shimadzu ICPE-9000). Reference Example 1: Cu/AEI zeolite catalysts preparation The AEI-type aluminosilicate zeolites were prepared by using N,N-dimethyl-3,5-dimethylpiperi- dinium hydroxide with different cis :trans isomer (see Figure 1) ratios (SACHEM, Inc.) as or- ganic structure directing agent (OSDA). Fumed silica (Cab-O-Sil M5, Cabot) was added into the solution containing N,N-dimethyl-3,5-dimethylpiperidinium hydroxide, NaOH (8M, Wako) and ze- olite Y having an Si/Al atomic ratio of 2.4 (JRC-Z-HY4.8, JGC Catalysts and Chemicals Ltd). The suspension with the molar composition of 1 SiO2: 0.017 Al2O3: 0.17 OSDA: 0.46 NaOH: 20 H2O was transferred to a Teflon-lined stainless-steel autoclave and crystallized at 150 °C for 3 days under tumbling condition. The as-synthesized samples were recovered after filtering, washing and drying at 100 °C overnight. The framework structure type of the zeolitic material obtained was verified by X-ray diffraction. The samples prepared using the OSDA with 20% cis and 100% cis isomer (both obtained from SACHEM, Inc.) were designated as AEI(20) and AEI(100), respectively. The OSDA was re- moved by calcination at 600 °C in air for 6 h. Then, the calcined samples were exchanged with 2.5 M NH4NO3 aqueous solution at 80 °C for 3 h to obtain the NH4-form ones. To research the effect of Cu loading on the reaction performance, 1, 5 and 50 mmol/L Cu(NO3)2 solutions were used to exchange with the NH4-type AEI(20) and AEI(100) zeolites at a 100 mL/g liquid-to-solid ratio stirring at 80 °C for 24 h. The suspension was filtered, washed, dried and calcined in air at 550 °C for 5 h. The obtained samples were noted as xCu/AEI(20) and xCu/AEI(100), where x means the concentration of the Cu(NO3)2 solution. The Si : Al and Cu : Al molar ratios of the re- spective samples are displayed in Table 1 below, together with the copper loading values as de- termined by ICP-AES. Table 1: Chemical composition of the samples obtained according to Reference Example 1 as obtained from ICP-AES.
Figure imgf000017_0001
Example 1: Catalytic testing The continuous oxidation of methane reaction was performed in a fixed-bed flow reactor. In each run, 100 mg of catalyst in a granular form (particle size 500−1000 μm) was charged into a quartz tube (inner diameter 4 mm), which was placed in an electric tube furnace. The catalyst was pretreated at 500 °C for 1 h in an Ar and steam flow. The reaction was conducted at the temperature ranging from 300 to 450 °C in a flowing gas mixture of CH4, N2O, H2O and Ar with flow rates of 10, 10, 2 and 3 mL·min−1. The outlet gas, containing the products, unreacted CH4 and N2O were analyzed using two on-line gas chromatographs (GC; GC-2014, Shimadzu). One of the GCs was used with a Shincarbon ST 50/80 packed column (3 mm × 6 m) and a TCD de- tector. Specifically, GC-TCD with a methanizer was used to detect H2, N2O, CO, CO2 and CH4. As may be taken from the results from catalyst testing displayed in Figure 2, the AEI(100) zeo- lite samples (i.e. the AEI-type zeolite obtained using the cis isomer of N,N-dimethyl-3,5-dime- thylpiperidinium hydroxide) from reference Example 1 respectively loaded with different amounts of copper afford a comparatively low conversion of N2O with methane up to a tempera- ture of about 350 °C. When increasing the temperature up to 400 °C, a substantial increase in the N2O conversion rate is observed, wherein said increase is particularly apparent for the sam- ples having a higher copper loading. When further raising the temperature to 450 °C, said trend continues, wherein the samples with higher copper loadings lead to a significant increase in N2O conversion, in particular for the sample displaying the higher loading, which reaches com- plete conversion of N2O at 450 °C. On the other hand, the results from catalyst testing using the AEI(20) zeolite samples (i.e. the AEI-type zeolite obtained using the N,N-dimethyl-3,5-dimethylpiperidinium hydroxide at a cis : trans molar ratio of 0.25) from Reference Example 1 respectively loaded with different amounts of copper displayed in Figure 3 show distinctly different N2O conversion rates depending on the temperature and the degree of loading with copper. Thus, although results at the lowest copper loading levels are comparable, the intermediate sample with regard to copper loading displays a somewhat higher N2O conversion rate at 400 °C, yet a far lower N2O conversion rate at 450 °C compared to the results displayed in Figure 2 for the corresponding copper loaded AEI(100) ze- olite sample. On the other hand, the sample with the highest copper loading displays a far higher N2O conversion rate at 400°C comparted to the result obtained at that temperature for the corresponding copper loaded AEI(100) zeolite sample. Accordingly, it has surprisingly been found that the inventive process allows for the activation of N2O to unprecedented levels for its controlled catalytic conversion. Furthermore, it has quite un- expectedly been found that depending on the cis : trans ratio of the N,N-dimethyl-3,5-dime- thylpiperidinium hydroxide used as OSDA in the synthesis of the AEI-type zeolite, the catalyst may display completely different N2O activation degrees at comparable loading of copper, such that catalytic conversion may be fine-tuned depending on the required activity for a given reac- tion at a given temperature, thus affording not only a highly effective, but also a highly versatile process for the activation of N2O for chemical conversion. Cited Literature: - US 5,958,370 - Moliner, M. et al. in Chem. Commun.2012, 48, pages 8264-8266 - Maruo, T. et al. in Chem. Lett.2014, 43, page 302-304 - Martín, N. et al. in Chem. Commun.2015, 51, 11030-11033 - Dusselier, M. et al. in ACS Catal.2015, 5, 10, 6078-6085 - US 2015/0118150 A1 - WO 2016/149234 A1 - Ransom, R. et al. in Ind. Eng. Chem. Res.2017, 56, 4350−4356 - WO 2018/113566 A1 - WO 2020/098796 A1 - WO 2018/234044 A1 - Memioglu, O. et al. in Chem. Comm.2021, 57, 1364-1367 - WO 2017/134007 A1 - US 2016/264428 A1

Claims

Claims 1. A process for the activation of N2O comprising (i) providing a gas stream comprising N2O; (ii) contacting the gas stream provided in (i) with a catalyst at a temperature in the range of from 300 to 600 °C, wherein the catalyst comprises a zeolitic material having the AEI-type framework structure, wherein the framework structure of the zeolitic material comprises SiO2 and Al2O3, and wherein the zeolitic material contains copper. 2. The process of claim 1, wherein the gas stream in (i) contains N2O in an amount ranging from 1 to 100 vol.-%. 3. The process of claim 1 or 2, wherein the gas stream in (i) further comprises a reducing agent, wherein the reducing agent is selected from the group consisting of hydrocarbons. 4. The process of any of claims 1 to 3, wherein in (ii), contacting the gas stream provided in (i) with a catalyst is carried out at a temperature in the range of from 350 to 550 °C. 5. The process of any of claims 1 to 4, wherein the zeolitic material having the AEI-type framework structure is ion exchanged with copper. 6. The process of any of claims 1 to 5, wherein the zeolitic material having the AEI-type framework structure contains copper in an amount in the range of from 0.1 to 12 wt.-% based on 100 wt.-% of the zeolitic material having the AEI-type framework structure, wherein copper is calculated as the element. 7. The process of any of claims 1 to 6, wherein the zeolitic material having the AEI-type framework structure comprised in the catalyst is prepared by a process comprising (1) preparing a mixture comprising one or more sources of SiO2, a first zeolitic material comprising SiO2 and Al2O3 in its framework structure and having an FAU-type framework structure, one or more cationic structure directing agents, and water; (2) heating the mixture obtained in (1) for obtaining a second zeolitic material compris- ing SiO2 and Al2O3 in its framework structure and having an AEI-type framework structure 8. The process of claim 7, wherein the one or more cationic structure directing agents are selected from the group consisting of N,N-di(C1-C4)alkyl-3,5-di(C1-C4)alkylpyrrolidinium , N,N-di(C1-C4)alkyl-3,5-di(C1-C4)alkylpiperidinium, N,N-di(C1-C4)alkyl-3,5-di(C1-C4)alkylhex- ahydroazepinium, and mixtures of two or more thereof. 9. The process of claim 8, wherein the cis : trans molar ratio of the cis isomer to the trans isomer in the one or more cationic structure directing agents relative to the alkyl groups at the 3 and 5 positions of the heterocyclic amine ring is in the range of from 0.01:1 to 0.95:1. 10. The process of claim 8, wherein the trans : cis molar ratio of the trans isomer to the cis isomer in the one or more cationic structure directing agents relative to the alkyl groups at the 3 and 5 positions of the heterocyclic amine ring is in the range of from 1:1 to 0:1. 11. The process of any of claims 7 to 10, wherein the one or more sources of SiO2 is selected from the group consisting of fumed silica, silica hydrosols, reactive amorphous solid sili- cas, silica gel, silicic acid, water glass, sodium metasilicate hydrate, sesquisilicate, disili- cate, colloidal silica, silicic acid esters, and mixtures of two or more thereof. 12. The process of any of claims 7 to 11, wherein the mixture prepared in (1) further com- prises OH-. 13. The process of claim 12, wherein the OH- : Si molar ratio of hydroxide to Si contained in the mixture prepared in (1) is in the range of from 0.01 to 5. 14. The process of any of claims 7 to 13, wherein the mixture prepared in (1) contains water at an H2O : Si molar ratio in the range of from 1 to 60. 15. The process of any of claims 7 to 14, wherein heating in (2) is conducted under autoge- nous pressure, preferably under hydrothermal conditions.
PCT/EP2023/069905 2022-07-19 2023-07-18 Process for the catalytic activation of n2o WO2024017884A1 (en)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
EP22185650 2022-07-19
EP22185650.3 2022-07-19

Publications (1)

Publication Number Publication Date
WO2024017884A1 true WO2024017884A1 (en) 2024-01-25

Family

ID=82655047

Family Applications (1)

Application Number Title Priority Date Filing Date
PCT/EP2023/069905 WO2024017884A1 (en) 2022-07-19 2023-07-18 Process for the catalytic activation of n2o

Country Status (1)

Country Link
WO (1) WO2024017884A1 (en)

Citations (7)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US5958370A (en) 1997-12-11 1999-09-28 Chevron U.S.A. Inc. Zeolite SSZ-39
US20150118150A1 (en) 2013-10-31 2015-04-30 Johnson Matthey Public Limited Company Aei zeolite synthesis
US20160264428A1 (en) 2015-03-15 2016-09-15 Sachem, Inc. Structure directing agent for improved synthesis of zeolites
WO2017134007A1 (en) 2016-02-01 2017-08-10 Haldor Topsøe A/S Method for the removal of nitrous oxide from off gas in presence of catalyst comprising an fe-aei zeolite material essentially free of alkali metal
WO2018113566A1 (en) 2016-12-21 2018-06-28 Basf Se Process for the production of a zeolitic material via solvent-free interzeolitic conversion
WO2018234044A1 (en) 2017-06-23 2018-12-27 Haldor Topsøe A/S A process for oxidation of a lower alkane at low temperatures in ammonia-containing gas mixtures
WO2020098796A1 (en) 2018-11-16 2020-05-22 Basf Se Process for the production of a zeolitic material having an aei-type framework structure via solvent-free interzeolitic conversion

Patent Citations (9)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US5958370A (en) 1997-12-11 1999-09-28 Chevron U.S.A. Inc. Zeolite SSZ-39
US20150118150A1 (en) 2013-10-31 2015-04-30 Johnson Matthey Public Limited Company Aei zeolite synthesis
US20160264428A1 (en) 2015-03-15 2016-09-15 Sachem, Inc. Structure directing agent for improved synthesis of zeolites
WO2016149234A1 (en) 2015-03-15 2016-09-22 Sachem, Inc. Structure directing agent for improved synthesis of zeolites
WO2017134007A1 (en) 2016-02-01 2017-08-10 Haldor Topsøe A/S Method for the removal of nitrous oxide from off gas in presence of catalyst comprising an fe-aei zeolite material essentially free of alkali metal
US20190275504A1 (en) * 2016-02-01 2019-09-12 Umicore Ag & Co. Kg Method for the Removal of Nitrous Oxide from Off Gas in Presence of Catalyst Comprising an Fe-AEI Zeolite Material Essentially Free of Alkali Metal
WO2018113566A1 (en) 2016-12-21 2018-06-28 Basf Se Process for the production of a zeolitic material via solvent-free interzeolitic conversion
WO2018234044A1 (en) 2017-06-23 2018-12-27 Haldor Topsøe A/S A process for oxidation of a lower alkane at low temperatures in ammonia-containing gas mixtures
WO2020098796A1 (en) 2018-11-16 2020-05-22 Basf Se Process for the production of a zeolitic material having an aei-type framework structure via solvent-free interzeolitic conversion

Non-Patent Citations (8)

* Cited by examiner, † Cited by third party
Title
DUSSELIER, M ET AL., ACS CATAL, vol. 5, no. 10, 2015, pages 6078 - 6085
MARTIN, N ET AL., CHEM. COMMUN., vol. 51, 2015, pages 11030 - 11033
MARUO, T ET AL., CHEM. LETT, vol. 43, 2014, pages 302 - 304
MEMIOGLU OZGUN ET AL: "A potential catalyst for continuous methane partial oxidation to methanol using N 2 O: Cu-SSZ-39", vol. 57, no. 11, 11 February 2021 (2021-02-11), UK, pages 1364 - 1367, XP093012326, ISSN: 1359-7345, Retrieved from the Internet <URL:https://pubs.rsc.org/en/content/articlepdf/2021/cc/d0cc06534j> [retrieved on 20230109], DOI: 10.1039/D0CC06534J *
MEMIOGLU, O ET AL., CHEM. COMM., vol. 57, 2021, pages 1364 - 1367
MEMIOGLU, O ET AL.: "A potential catalyst for continuous methane partial oxidation to methanol using N O : Cu-SSZ-39", CHEM. COMM., vol. 57, 2021, pages 1364 - 1367, XP093012326, DOI: 10.1039/D0CC06534J
MOLINER, M ET AL., CHEM. COMMUN., vol. 48, 2012, pages 8264 - 8266
RANSOM, R. ET AL., IND. ENG. CHEM. RES., vol. 56, 2017, pages 4350 - 4356

Similar Documents

Publication Publication Date Title
CA1283648C (en) Zeolite ssz-25
EP3097054B1 (en) Method for the production of a bimetal-exchanged zeolite beta from organotemplate-free synthesis
US20160271596A1 (en) One-pot method for the synthesis of cu-ssz-13, the compound obtained by the method and use thereof
EP3050847B1 (en) Mse-type zeolite, manufacturing method of the same, and catalytic cracking catalyst of paraffin
US10792614B2 (en) Process and apparatus for treatment of gas streams containing nitrogen oxides
JP6951343B2 (en) Methods for Direct Synthesis of Iron-Containing AEI Zeolite Catalysts
JPS63162521A (en) Novel synthesis of ferric silicate type zeolites, obtained substances and their uses
EP3313782A1 (en) Synthesis of aluminosilicate zeolite ssz-98
CN112055613A (en) Aluminum-rich zeolite material containing rare earth elements
EP2072128A1 (en) Catalyst for reducing nitrogen oxides and process for reducing nitrogen oxides
WO2015018815A1 (en) Process for the oxygen free conversion of methane to ethylene on zeolite catalysts
CN114007984A (en) Synthesis of chabazite using organic template
JP7251471B2 (en) Transition metal-supported zeolite, method for producing the same, catalyst for purifying nitrogen oxides, and method for using the same
Vergani et al. Isopropylation of biphenyl over dealuminated mordenite
Zhang et al. Synthesis and catalytic property of a Co2+-exchanged Beta/Y composite for the selective catalytic reduction of NO by CH4 in the presence of excess oxygen
WO2024017884A1 (en) Process for the catalytic activation of n2o
WO2020098796A1 (en) Process for the production of a zeolitic material having an aei-type framework structure via solvent-free interzeolitic conversion
JP4247504B2 (en) Dealuminated zeolite IM-5
CN105008047A (en) Hydrocarbon reforming/trapping material and method for removing hydrocarbon
US5583081A (en) Copper-containing zeolite catalysts
KR20230108315A (en) Synthesis of chabazite zeolites using combined organic templates
EP3458416B1 (en) Molecular sieve ssz-104, its synthesis and use
WO2020164545A1 (en) Aluminum-and Gallium Containing Zeolitic Material and Use Thereof in SCR
JP3211254B2 (en) Nitrogen oxide adsorbent
Price et al. Copper-containing zeolite catalysts

Legal Events

Date Code Title Description
121 Ep: the epo has been informed by wipo that ep was designated in this application

Ref document number: 23742103

Country of ref document: EP

Kind code of ref document: A1