TECHNICAL FIELD

The present invention relates to a process for the activation of N ₂ O in the presence of a zeolitic material having the AEl-type framework structure, wherein the ²⁹ Si MAS NMR of the zeolitic material comprises three specific peaks P1, P2, and P3 and optionally a fourth peak P4, wherein the integration of said peaks in the ²⁹ Si MAS NMR of the zeolitic material offers a specific ratio of the integration values P1 : P2 : P3 : P4.

INTRODUCTION

N2O is a well-known greenhouse gas, that reguires to be decomposed/removed from off-gas emissions of chemical processes. N ₂ O activation, particularly at lower temperature is difficult.

Separately, the selective direct oxidation of methane to methanol is a long standing challenge for which Cu containing zeolites have often been investigated. Typically, only low levels of conversion can be reached until over-oxidation to CO and CO ₂ . N ₂ O can be used as a selective oxidant in this reaction. This N ₂ O is hereby decomposed resulting in the effective removal of N ₂ O from the gas stream.

R. Xu et al. disclose a study on “H ₂ O-Built Proton Transfer Bridge Enhances Continuous Methane Oxidation to Methanol over Cu-BEA Zeolite” in Angew. Chem. Int. Ed. 2021 , 60, 16634- 16640. B. Ipek et al. disclose a study on “Catalytic conversion of methane to methanol on Cu- SSZ-13 using N ₂ O as oxidant” in Chem Commun (Camb) 2016, 52 (91), 13401-13404. B. Ipek et al. disclose a study on “A potential catalyst for continuous methane partial oxidation to methanol using N ₂ O: Cu-SSZ-39” in Chem. Commun. 2021 , (57), 1364. In particular, a high methanol yield of 8.3 pmol-g- ¹ min- ¹ with 34 % selectivity on Cu/AEI zeolite at 300 °C is disclosed therein.

K. Narsimhan et al. disclose a study on “Catalytic Oxidation of Methane into Methanol over Copper-Exchanged Zeolites with Oxygen at Low Temperature” in ACS Cent Sci 2016, 2 (6), 424-9.

K. T. Dinh et al. disclose a study on “Continuous Partial Oxidation of Methane to Methanol Catalyzed by Diffusion-Paired Cu Dimers in Copper-Exchanged Zeolites” in J. Am. Chem. Soc.

2019, 141 , 11641 -11650.

Further, 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 example for converting nitrogen oxides (NO _X ) in an exhaust gas stream. Synthetic AEI zeolitic materials are generally produced by precipitating crystals of the zeolitic material from a synthesis mixture 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. The process for the activation of N ₂ O according to the present invention involves presence of a specific zeolitic material having the AEl-type framework structure. The preparation of said zeo- litic material is conducted via zeolitic framework conversion according to which a starting material which is a suitable zeolitic material comprising SiO ₂ and AI ₂ O ₃ in its framework structure and having an FER-type framework structure is suitably reacted to obtain the zeolitic material having framework type AEI. The ²⁹ Si MAS NMR of the resulting zeolitic material comprises three specific peaks P1 , P2, and P3, and optionally a fourth peak P4, wherein the integration of the first, second, third, and fourth peaks in the ²⁹ Si MAS NMR of the zeolitic material offers a specific ratio of the integration values P1 : P2 : P3 : P4.

WO 2017/134007 A1 relates to a method for the removal of nitrous oxide from off gas in presence of a catalyst comprising an Fe-AEI zeolite material. 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 presence of tetraethylphosphonium cations. Martin, 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 oxides 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 tetraethylphosphonium cations. US 2015/0118150 A1 describes zeolite synthesis methods involving the use of N,N-dimethyl-3,5-dimethylpiperidinium and N,N-dimethyl-2,6-dimethylpiperi- dinium cations, respectively. WO 2016/149234 A1 and Ransom, R. et al. in Ind. Eng. Chem. Res. 2017, 56, 4350-4356 respectively relate to the synthesis of SSZ-39 via interzeolitic conversion of faujasite using N,N-dimethyl-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-dimethylpiperidinium cations is described. WO 2016/149234 A1 and Ransom, R. et al. in Ind. Eng. Chem. Res. 2017, 56, 4350-4356 respectively relate to the synthesis of SSZ-39 using different isomer ratios of the c/sand trans isomers of the N,N-dimethyl- 3,5-dimethylpiperidinium cation. WO 2020/098796 A1 , on the other hand, concerns the production of an AEl-type zeolitic material via solvent-free interzeolitic conversion, wherein N,N-dime- thyl-3,5-dimethylpiperidinium having a specific ratio of c/sand trans isomers was employed. WO 2019/242618 A1 discloses a process for the preparation of a zeolitic material via interzeolitic conversion, wherein in Example 3 synthesis of an AEl-type zeolitic material is disclosed starting from a FER-type zeolitic material. WO 2021/122533 A1 discloses a continuous process for the preparation of a zeolitic material via interzeolitic conversion, wherein the examples disclose inter alia the synthesis of a zeolitic material having AEl-type framework structure starting from a FAU-type zeolitic material.

Despite the zeolitic materials having the AEl-type framework structure of the prior art, which can be used for several reactions as catalysts, there remains the need for a zeolitic material with unique physical and chemical characteristics of this highly specific framework structure type, in particular with respect to the use thereof as a catalyst for the activation of N ₂ O. DETAILED DESCRIPTION

It was therefore the object of the present invention to provide an improved process for the activation of N2O involving the presence of a zeolitic material having the AEl-type framework structure. In particular, it was an object to provide a process for the activation of N ₂ O, especially for the selective oxidation of methane, at lower temperatures. Thus, it has surprisingly been found that a novel process for the activation of N ₂ O can be provided involving a zeolitic material having the AEl-type framework structure, wherein the framework structure of the zeolitic material comprises SiO ₂ and AI ₂ Os, and wherein the ²⁹ Si MAS NMR of the zeolitic material comprises specific peaks P1 , P2, and P3, and optionally a fourth peak P4, wherein the integration of the said peaks in the ²⁹ Si MAS NMR of the zeolitic material offers a specific ratio of the integration values P1 : P2 : P3 : P4. Further, it was found that such a zeolitic material can be prepared by a preparation process particularly comprising an interzeolitic conversion of a zeolitic material comprising SiO ₂ and AI ₂ C>3 in its framework structure and having an FER-type framework structure. In addition thereto, it was found that the zeolitic material of the present invention is suitable as catalyst for the selective conversion of methane to methanol with N ₂ O.

Therefore the present invention relates to a process for the activation of N ₂ O, the process comprising

(i) providing a zeolitic material comprising one or more transition metals, wherein the zeolitic material has the AEl-type framework structure, wherein the framework structure of the zeolitic material comprises SiO ₂ and AI ₂ O ₃ , wherein the ²⁹ Si MAS NMR of the zeolitic material comprises: a first peak (P1) having a maximum in the range of from -107.0 to -114.0 ppm, a second peak (P2) having a maximum in the range of from -101.0 to -108.0 ppm, a third peak (P3) having a maximum in the range of from -97.0 to -105.0 ppm, and optionally a fourth peak (P4) having a maximum in the range of from -93.0 to -101.0 ppm, wherein the integration of the first, second, third, and optional fourth peaks in the ²⁹ Si MAS NMR of the zeolitic material offers a ratio of the integration values P1 : P2 : P3 : P4 comprised in the range of from (50-100) : (5-35) : (1-10) : (0-15), preferably in the range of from (50-100) : (5-30) : (1-10) : (0-15), more preferably in the range of from (50-100) : (5- 29) : (1-10) : (0-15), more preferably in the range of from (50-100) : (5-27) : (1-10) : (0-15), more preferably in the range of from (50-100) : (5-26) : (1-10) : (0-15), more preferably in the range of from (50-100) : (5-20) : (1-10) : (0-15), wherein the ²⁹ Si MAS NMR of the zeolitic material is determined on the zeolitic material which is devoid of transition metals, preferably according to Reference example 1 ;

(ii) providing a gas stream comprising N ₂ O;

(iii) contacting the gas stream provided in (ii) with the zeolitic material provided in (i) at a temperature in the range of from 300 to 600 °C. It is preferred that the ²⁹ Si MAS NMR of the zeolitic material is determined on the H-form of the zeolitic material, i.e. on the zeolitic material consisting only of the framework elements and H ⁺ as the counterions.

It is preferred that the gas stream provided in (ii) 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 preferably from 38 to 42 vol.-%.

It is preferred that the gas stream provided in (ii) further comprises one or more alkanes, more preferably one or more (C1-C6)alkanes, more preferably one or more (C1-C5)alkanes, more preferably one or more (C1-C4)alkanes, more preferably one or more (C1-C3)alkanes, wherein more preferably the gas stream provided in (ii) further comprises one or more alkanes selected from the group consisting of methane, ethane, and propane, including mixtures of two or more thereof, wherein more preferably the one or more alkanes comprise methane and/or propane, preferably methane, wherein more preferably the one or more alkanes are methane and/or propane, preferably methane, and wherein the gas stream provided in (ii) more preferably has a volume ratio of N ₂ O to methane in the range of from 0.1 :1 to 1 :0.1 , more preferably in the range of from 0.5:1 to 1 :0.5, more preferably in the range of from 0.9:1 to 1 :0.9.

In the context of the present invention, the one or more alkanes may be branched or unbranched, and may be optionally substituted with one or more functional groups. Preferably, the one or more alkanes are unbranched and are not substituted with functional groups.

It is preferred that the gas stream provided in (ii) further comprises H ₂ O.

In the case where the gas stream provided in (ii) further comprises H ₂ O, it is preferred that the gas stream in provided (ii) has a volume ratio of N ₂ O to H ₂ O in the range of from 1.0:1 to 10.0:1 , more preferably in the range of from 4.0:1 to 6.0:1 , more preferably in the range of from 4.9:1 to 5.1 :1.

It is preferred that the gas stream provided in (ii) further comprises an inert gas, wherein the inert gas is more preferably selected from the group consisting of N ₂ , Ar, and a mixture thereof.

It is preferred that the gas stream provided in (ii) has a weight hourly space velocity in the range of from 7,000 to 23,000 ml/(g(catalyst)*h), more preferably in the range of from 12,000 to 18,000 ml/(g(catalyst)*h), more preferably in the range of from 14,000 to 16,000 ml/(g(catalyst)*h).

It is preferred that contacting in (iii) of the gas stream provided in (ii) with the zeolitic material is conducted at a temperature in the range of from 330 to 600 °C, more preferably of from 350 to 550 °C, more preferably of from 200 to 550 °C, more preferably of from 250 to 500 °C, and more preferably of from 300 to 450 °C.

It is preferred that the ²⁹ Si MAS NMR of the zeolitic material provided in (I) comprises: a first peak (P1) having a maximum in the range of from -109.0 to -113.0 ppm, more preferably of from -110.0 to -112.0 ppm, and more preferably of from -110.5 to -111 .5 ppm; a second peak (P2) having a maximum in the range of from -103.0 to -107.0 ppm, more preferably of from -104.0 to -106.0 ppm, and more preferably of from -104.5 to -105.5 ppm; a third peak (P3) having a maximum in the range of from -99.0 to -103.0 ppm, more preferably of from -100.0 to -102.0 ppm, and more preferably of from -100.5 to -101.5 ppm; and optionally a fourth peak (P4) having a maximum in the range of from -95.0 to -99.0 ppm, more preferably of from -96.0 to -98.0 ppm, and more preferably of from -96.5 to -97.5 ppm.

It is preferred that the integration of the first, second, third, and optional fourth peaks in the ²⁹ Si MAS NMR of the zeolitic material provided in (i) offers a ratio of the integration values P1 : P2 : P3 : P4 comprised in the range of from (62-86) : (9-29) : (1-6) : (0-8), more preferably in the range of from (64-84) : (11-27) : (2-5) : (0-7), and more preferably in the range of from (65-83) : (12-26) : (3-4) : (0-6).

It is preferred that the ²⁹ Si MAS NMR of the zeolitic material provided in (i) comprises only three peaks P1 , P2, and P3 or only four peaks P1 , P2, P3, and P4 in the range of from -90 to -120 ppm.

It is preferred that the ²⁹ Si MAS NMR of the zeolitic material provided in (I) comprises four peaks, wherein the integration of the first, second, third, and optional fourth peaks in the ²⁹ Si MAS NMR of the zeolitic material provided in (i) offers a ratio of the integration values P1 : P2 : P3 : P4 comprised in the range of from (62-86) : (9-29) : (1-6) : (greater than 0-8), more preferably in the range of from (64-84) : (11 -27) : (2-5) : (greater than 0-7), and more preferably in the range of from (65-83) : (12-26) : (3-4) : (greater than 0-6).

It is preferred that the zeolitic material provided in (I) has a Si : Al molar ratio in the range of from 2 to 100, more preferably of from 4 to 50, more preferably of from 6 to 20, more preferably of from 8 to 15, more preferably of from 9 to 14, more preferably of from 9.5 to 13.0, more preferably of from 10.2 to 12.2, and more preferably of from 10.7 to 11.7.

It is preferred that the zeolitic material provided in (I) is selected from the group consisting of SSZ-39, SAPO-18, SIZ-8, including mixtures of two or more thereof, wherein the zeolitic material more preferably comprises, more preferably consist of, SSZ-39.

It is preferred that the one or more transition metals are selected from the group consisting of Fe, Cu, and mixtures thereof, wherein the one or more transition metals more preferably are Cu. It is preferred that the zeolitic material provided in (i) is ion exchanged with the one or more transition metals.

It is preferred that the zeolitic material provided in (i) comprises the one or more transition metals, calculated as sum of the weights of the transition metals as elements, in an amount in the range of from 0.1 to 12 wt.-% based on 100 wt-% of the zeolitic material, more preferably of from 0.4 to 8.0 wt.-%, more preferably of from 0.7 to 5.5 wt.-%, more preferably of from 0.9 to 4.0 wt.-%, more preferably of from 1 .1 to 2.5 wt.-%, more preferably of from 1 .3 to 2.3 wt.-%, more preferably of from 1 .5 to 2.1 wt.-%, and more preferably of from 1 .7 to 1.9 wt-% based on 100 wt.-% of the zeolitic material.

It is preferred that the zeolitic material provided in (i) has a molar ratio of the one or more transition metals comprised in the zeolitic material to the Al comprised in the framework structure of the zeolitic material in the range of from 0.01 :1 to 0.45:1 , more preferably in the range of from 0.04:1 to 0.42:1 , more preferably in the range of from 0.07:1 to 0.38:1 , more preferably in the range of from 0.10:1 to 0.34:1 , more preferably in the range of from 0.13:1 to 0.31 :1 , more preferably in the range of from 0.15:1 to 0.29:1 , more preferably in the range of from 0.17:1 to 0.27:1 , more preferably in the range of from 0.19:1 to 0.25:1 , more preferably in the range of from 0.21 :1 to 0.23:1.

It is preferred that the temperature programmed desorption of ammonia (NH3-TPD) profile of the zeolitic material displays one or more desorption peaks having maxima in the temperature range of from 80 to 230 °C, preferably of from 90 to 220 °C, more preferably of from 100 to 210 °C, more preferably of from 110 to 200 °C, more preferably of from 120 to 190 °C, more preferably of from 130 to 180 °C, more preferably of from 135 to 170 °C, and more preferably of from 140 to 160 °C, wherein the integration of said one or more desorption peaks affords a total value of 0.60 mmol/g or less, more preferably in the range of from 0.02 to 0.55 mmol/g, more preferably in the range of from 0.04 to 0.50 mmol/g, more preferably in the range of from 0.06 to 0.45 mmol/g, more preferably in the range of from 0.08 to 0.40 mmol/g, more preferably in the range of from 0.09 to 0.37 mmol/g, more preferably in the range of from 0.10 to 0.34 mmol/g, more preferably in the range of from 0.14 to 0.26 mmol/g, more preferably in the range of from 0.17 to 0.21 mmol/g, wherein the NH3-TPD profile is preferably determined according to Reference Example 5.

It is preferred that the temperature programmed desorption of ammonia (NH3-TPD) profile of the zeolitic material displays one or more desorption peaks having maxima in the temperature range of from greater than 230 to 370 °C, preferably of from 240 to 360 °C, preferably of from 250 to 350 °C, more preferably of from 260 to 340 °C, more preferably of from 270 to 330 °C, more preferably of from 280 to 320 °C, more preferably of from 285 to 315 °C, and more preferably of from 290 to 310 °C, wherein the integration of said one or more desorption peaks affords a total value of 1 .00 mmol/g or less, preferably in the range of from 0.05 to 0.95 mmol/g, more preferably in the range of from 0.10 to 0.90 mmol/g, more preferably in the range of from 0.30 to 0.85 mmol/g, more preferably in the range of from 0.50 to 0.80 mmol/g, more preferably in the range of from 0.67 to 0.77 mmol/g, more preferably in the range of from 0.71 to 0.75 mmol/g, wherein the NH ₃ -TPD profile is preferably determined according to Reference Example 5.

It is preferred that the temperature programmed desorption of ammonia (NH3-TPD) profile of the zeolitic material displays one or more desorption peaks having maxima in the temperature range of from greater than 370 to 520 °C, more preferably of from 380 to 510 °C, more preferably of from 390 to 510 °C, more preferably of from 400 to 500 °C, more preferably of from 410 to 490 °C, more preferably of from 420 to 480 °C, more preferably of from 430 to 470 °C, more preferably of from 435 to 465 °C, and more preferably of from 440 to 460 °C, wherein the integration of said one or more desorption peaks affords a total value of 0.80 mmol/g or less, more preferably in the range of from 0.10 to 0.75 mmol/g, more preferably in the range of from 0.15 to 0.70 mmol/g, more preferably in the range of from 0.20 to 0.65 mmol/g, more preferably in the range of from 0.25 to 0.60 mmol/g, more preferably in the range of from 0.30 to 0.55 mmol/g, more preferably in the range of from 0.35 to 0.52 mmol/g, more preferably in the range of from 0.39 to 0.48 mmol/g, more preferably in the range of from 0.42 to 0.46 mmol/g, wherein the NH3-TPD profile is preferably determined according to Reference Example 5.

It is preferred that the integration of the desorption peaks in the NH3-TPD profile of the zeolitic material having maxima in the temperature range of from 50 to 800 °C, more preferably of from 80 to 520 °C, more preferably of from 90 to 510 °C, more preferably of from 100 to 500 °C, more preferably of from 110 to 490 °C, more preferably of from 120 to 480 °C, more preferably of from 130 to 470 °C, and more preferably of from 140 to 460 °C, affords a total value of 1.70 mmol/g or less, more preferably in the range of from 0.45 to 1.60 mmol/g, more preferably in the range of from 0.60 to 1.55 mmol/g, more preferably in the range of from 0.75 to 1.50 mmol/g, more preferably in the range of from 0.90 to 1.45 mmol/g, more preferably in the range of from 1.10 to 1 .40 mmol/g, more preferably in the range of from 1.30 to 1.38 mmol/g, wherein the NH3-TPD profile is preferably determined according to Reference Example 5.

It is preferred that the NH3-TPD profile of the zeolitic material is a deconvoluted NH3-TPD profile, wherein the one or more desorption peaks of the NH3-TPD profile are the one or more deconvoluted desorption peaks of the NH3-TPD profile, wherein deconvolution of the desorption peaks is more preferably achieved according to Reference Example 5.

It is preferred that the zeolitic material provided in (i) further comprises an alkali metal selected from the group consisting of Li, Na, K, Rb, Cs, and mixtures of two or more thereof, more preferably from the group consisting of Li, Na, K, and mixtures of two or more thereof, wherein the zeolitic material more preferably further comprises Na, wherein the zeolitic material more preferably is ion exchanged with the alkali metal, preferably with Na. In the case where the zeolitic material provided in (i) further comprises an alkali metal selected from the group consisting of Li, Na, K, Rb, Cs, and mixtures of two or more thereof, it is preferred that the zeolitic material has a Na:AI molar ratio of the Na comprised in the zeolitic material to the Al comprised in the framework structure of the zeolitic material in the range of from 0.002:1 to 2.00:1 , more preferably in the range of from 0.004:1 to 1.60:1 , more preferably in the range of from 0.006:1 to 1.50:1 , more preferably in the range of from 0.007:1 to 1.40:1.

It is preferred that the zeolitic material provided in (i) has a BET specific surface area in the range of from 200 to 650 m ² /g, more preferably from 360 to 560 m ² /g, more preferably from 410 to 510 m ² /g, and more preferably from 430 to 490 m ² /g, wherein the BET surface area is preferably determined according to Reference Example 4.

It is preferred that the zeolitic material provided in (i) has a total micropore volume in the range of from 0.10 to 0.35 cm ³ /g, more preferably from 0.15 to 0.27 cm ³ /g, more preferably from 0.17 to 0.25 cm ³ /g, and more preferably from 0.19 to 0.23 cm ³ /g, wherein the total micropore volume is preferably determined according to Reference Example 4.

It is preferred that the zeolitic material provided in (i) has a particle size in the range of from 100 to 1200 nm, more preferably in the range of from 250 to 1100 nm, more preferably in the range of from 500 to 1000 nm.

It is preferred that providing a zeolitic material according to (i) comprises, more preferably consists of,

(1 ) preparing a mixture comprising a zeolitic material comprising SiO ₂ and AI ₂ O ₃ in its framework structure and having an FER-type framework structure, one or more cationic structure directing agents, and water;

(2) heating the mixture obtained in (1 ) for obtaining the zeolitic material having the AEl-type framework structure and comprising SiO ₂ and AI ₂ O ₃ in its framework structure.

In the case where providing a zeolitic material according to (i) comprises (1 ) and (2), it is preferred that the one or more cationic structure directing agents are selected from the group consisting of /V,/V-di(Ci-C ₄ )alkyl-3,5-di(Ci-C4)alkylpyrrolidinium, A/, di(Ci-C ₄ )alkyl-3,5-di(Ci-C4)al- kylpiperidinium, A/,A ^L di(Ci-C4)alkyl-3,5-di(Ci-C4)alkylhexahydroazepinium, and mixtures of two or more thereof, more preferably from the group consisting of /,/V-di(Ci-C ₃ )alkyl-3,5-di(Ci-C ₃ )alkylpyrrolidinium, /V,A/-di(Ci-C ₃ )alkyl-3,5-di(Ci-C ₃ )alkylpiperidinium, A/,A/-di(Ci-C ₃ )alkyl-3,5-di(Ci-C ₃ )alkylhexahy- droazepinium, and mixtures of two or more thereof, more preferably from the group consisting of /V,/V-di(Ci-C ₂ )alkyl-3,5-di(Ci-C ₂ )alkylpyrrolidinium, /V,/V-di(Ci-C ₂ )alkyl-3,5-di(Ci-C ₂ )alkylpiperidinium, /V,A/-di(Ci-C ₂ )alkyl-3,5-di(Ci-C ₂ )alkylhexahy- droazepinium, and mixtures of two or more thereof, more preferably from the group consisting of /V,/V-di(Ci-C ₂ )alkyl-3,5-di(Ci-C ₂ )alkylpiperidinium, and mixtures of two or more thereof, wherein more preferably the one or more cationic structure directing agents comprises /V,A/-dimethyl-3,5-dimethylpiperidinium, wherein more preferably the one or more cationic structure directing agents consists of /V,A/-dimethyl-3,5-dimethylpiperi- dinium.

Further in the case where providing a zeolitic material according to (i) comprises (1 ) and (2), it is preferred that 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 cationic structure directing agents are provided as hydroxides and/or bromides, and more preferably as hydroxides.

Further in the case where providing a zeolitic material according to (i) comprises (1 ) and (2), it is preferred that the framework structure of the zeolitic material having an FER-type framework structure displays a SiO ₂ : AI ₂ O ₃ molar ratio ranging from 5 to 100, preferably of from 10 to 50, more preferably of from 15 to 41 , more preferably of from 20 to 36, more preferably of from 23 to 33, more preferably of from 25 to 31 , and more preferably of from 27 to 29.

Further in the case where providing a zeolitic material according to (i) comprises (1 ) and (2), 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, 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 providing a zeolitic material according to (i) comprises (1 ) and (2), it is preferred that the zeolitic material having an FER-type framework structure is selected from the group consisting of ferrierite, ZSM-35, NU-23, FU-23, ISI-6, [Si-O]-FER, [Ga-Si-O]-FER, [B-Si- O]-FER, and mixtures of two or more thereof, more preferably from the group consisting of ferrierite, ZSM-35, NU-23, FU-23, ISI-6, [Si-O]-FER, and mixtures of two or more thereof, wherein more preferably the zeolitic material having an FER-type framework structure comprises ferrierite, wherein more preferably the zeolitic material having an FER-type framework structure is ferrierite.

Further in the case where providing a zeolitic material according to (i) comprises (1 ) and (2), 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 0.25 to 1 , more preferably from 0.35 to 0.70, and more preferably from 0.45 to 0.59, and more preferably from 0.51 to 0.52. Further in the case where providing a zeolitic material according to (i) comprises (1 ) and (2), 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 mixtures 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 5, more preferably from 0.05 to 3, more preferably from 0.1 to 1 .5, more preferably from 0.15 to 1 , more preferably from 0.2 to 0.5, and more preferably from 0.27 to 0.45, and more preferably from 0.32 to 0.40.

Further in the case where the mixture prepared in (1) further comprises one or more alkali metals 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 providing a zeolitic material according to (i) comprises (1 ) and (2), 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, 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 providing a zeolitic material according to (i) comprises (1 ) and (2), 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 providing a zeolitic material according to (I) comprises (1 ) and (2), it is preferred that heating in (2) is conducted under autogenous pressure, more preferably under hydrothermal conditions.

Further in the case where providing a zeolitic material according to (i) comprises (1 ) and (2), it is preferred that heating in (2) is performed in a pressure tight vessel, more preferably in an autoclave.

Further in the case where providing a zeolitic material according to (i) comprises (1 ) and (2), 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 8 h to 6 d, more preferably from 10 h to 3 d, more preferably from 15 h to 1 .5 d, more preferably from 21 to 27, and more preferably from 23 to 25 h. Further in the case where providing a zeolitic material according to (i) comprises (1 ) and (2), it is preferred that the zeolitic material obtained in (2) 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 obtained in (2) comprises SSZ-39, and wherein more preferably the zeolitic material obtained in (2) is SSZ-39.

Further in the case where providing a zeolitic material according to (i) comprises (1 ) and (2), it is preferred that the process further comprises

(3) calcining the zeolitic material obtained in (2).

Further in the case where providing a zeolitic material according to (i) comprises (1), (2), and optionally (3), 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 framework structure of the zeolitic material is ion-exchanged against one or more of H ⁺ , NH ₄ ⁺ , and Na, more preferably against NH ₄ ⁺ or Na.

Further in the case where providing a zeolitic material according to (i) comprises (1), (2), optionally (3), and optionally (4), 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 framework structure of the zeolitic material is ion-exchanged against one or more transition metals, preferably against one or more transition metals selected from the group consisting of Fe, Cu, and mixtures thereof, more preferably against copper.

In the case where the process further comprises (5), it is preferred that the process further comprises

(6) subjecting the zeolitic material obtained in (5) to an ion-exchange procedure, wherein one or more ionic extra-framework elements contained in the framework structure of the zeolitic material is ion-exchanged against Na.

In the case where the process further comprises (5) and optionally (6), it is preferred that the process further comprises

(7) calcining the zeolitic material obtained in (5) or (6).

In the case where the process further comprises (3), it is preferred that the temperature of calcination in (3) is in the range of from 300 to 1000°C, more preferably of from 400 to 800°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), it is preferred that calcining in (3) is conducted for a period in the range of from 0.5 to 20 h, 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, and more preferably from 4.5 to 6.5 h. In the case where the process further comprises (6), it is preferred that the temperature of calcination in (6) is in the range of from 300 to 1000°C, more preferably of from 400 to 800°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 (6), it is preferred that calcining in (6) is conducted for a period in the range of from 0.5 to 20 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, and more preferably from 4.5 to 6.5 h.

Further in the case where providing a zeolitic material according to (i) comprises (1 ) and (2), it is preferred that the mixture in (1) further comprises seed crystals, wherein the seed crystals more preferably comprise a zeolitic material having an AEl-type framework structure, wherein more preferably the zeolitic material consists of a zeolitic material having an AEl-type framework structure.

In the case where the mixture in (1) further comprises seed crystals, it is preferred that the zeolitic material having an AEl-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 AEl-type framework structure comprised in the seed crystals is SSZ-39, preferably calcined 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 SiO ₂ in the mixture prepared in (1), 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 SiO ₂ in the mixture prepared in (1) calculated as SiO ₂ .

The unit bar(abs) refers to an absolute pressure wherein 1 bar equals 10 ⁵ Pa.

The present invention is further illustrated by the following set of embodiments and combinations of embodiments resulting from the dependencies and back-references as indicated. In particular, it is noted that in each instance where a range of embodiments is mentioned, for example in the context of a term such as "The catalyst 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 catalyst 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, the process comprising (i) providing a zeolitic material comprising one or more transition metals, wherein the zeolitic material has the AEl-type framework structure, wherein the framework structure of the zeolitic material comprises SiC>2 and AI2O3, wherein the ²⁹ Si MAS NMR of the zeolitic material comprises: a first peak (P1) having a maximum in the range of from -107.0 to -114.0 ppm, a second peak (P2) having a maximum in the range of from -101.0 to -108.0 ppm, a third peak (P3) having a maximum in the range of from -97.0 to -105.0 ppm, and optionally a fourth peak (P4) having a maximum in the range of from -93.0 to -101.0 ppm, wherein the integration of the first, second, third, and optional fourth peaks in the 2 ⁹ Si MAS NMR of the zeolitic material offers a ratio of the integration values P1 : P2 : P3 : P4 comprised in the range of from (50-100) : (5-35) : (1-10) : (0-15), preferably in the range of from (50-100) : (5-30) : (1-10) : (0-15), more preferably in the range of from (50-100) : (5-29) : (1-10) : (0-15), more preferably in the range of from (50- 100) : (5-27) : (1-10) : (0-15), more preferably in the range of from (50-100) : (5-26) : (1-10) : (0-15), more preferably in the range of from (50-100) : (5-20) : (1-10) : (0- 15), wherein the ²⁹ Si MAS NMR of the zeolitic material is determined on the zeolitic material which is devoid of transition metals, preferably according to Reference example 1 ;

(ii) providing a gas stream comprising N2O;

(iii) contacting the gas stream provided in (ii) with the zeolitic material provided in (i) at a temperature in the range of from 300 to 600 °C.

2. The process of embodiment 1 , wherein the gas stream provided in (ii) 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 preferably 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 provided in (ii) further comprises one or more alkanes, preferably one or more (C1-C6)alkanes, more preferably one or more (C1-C5)alkanes, more preferably one or more (C1-C4)alkanes, more preferably one or more (C1-C3)alkanes, wherein more preferably the gas stream provided in (ii) further comprises one or more alkanes selected from the group consisting of methane, ethane, and propane, including mixtures of two or more thereof, wherein more preferably the one or more alkanes comprise methane and/or propane, preferably methane, wherein more preferably the one or more alkanes are methane and/or propane, preferably methane, and wherein the gas stream provided in (ii) preferably has a volume ratio of N2O to methane in the range of from 0.1 :1 to 1 :0.1 , more preferably in the range of from 0.5:1 to 1 :0.5, more preferably in the range of from 0.9:1 to 1 :0.9. The process of any one of embodiments 1 to 3, wherein the gas stream provided in (ii) further comprises H ₂ O. The process of embodiment 4, wherein the gas stream in provided (ii) has a volume ratio of N ₂ O to H ₂ O in the range of from 1.0:1 to 10.0:1 , preferably in the range of from 4.0:1 to 6.0:1 , more preferably in the range of from 4.9:1 to 5.1 :1. The process of any one of embodiments 1 to 5, wherein the gas stream provided in (ii) further comprises an inert gas, wherein the inert gas is preferably selected from the group consisting of N ₂ , Ar, and a mixture thereof. The process of any one of embodiments 1 to 6, wherein the gas stream provided in (ii) has a weight hourly space velocity in the range of from 7,000 to 23,000 ml/(g(catalyst)*h), preferably in the range of from 12,000 to 18,000 ml/(g(catalyst)*h), more preferably in the range of from 14,000 to 16,000 ml/(g(catalyst)*h). The process of any one of embodiments 1 to 7, wherein contacting in (iii) of the gas stream provided in (ii) with the zeolitic material is conducted at a temperature in the range of from 330 to 600 °C, more preferably of from 350 to 550 °C, more preferably of from 200 to 550 °C, preferably of from 250 to 500 °C, and more preferably of from 300 to 450 °C. The process of any one of embodiments 1 to 8, wherein the ²⁹ Si MAS NMR of the zeolitic material provided in (i) comprises: a first peak (P1) having a maximum in the range of from -109.0 to -113.0 ppm, preferably of from -110.0 to -112.0 ppm, and more preferably of from -110.5 to -111.5 ppm; a second peak (P2) having a maximum in the range of from -103.0 to -107.0 ppm, preferably of from -104.0 to -106.0 ppm, and more preferably of from -104.5 to -105.5 ppm; a third peak (P3) having a maximum in the range of from -99.0 to -103.0 ppm, preferably of from -100.0 to -102.0 ppm, and more preferably of from -100.5 to -101.5 ppm; and optionally a fourth peak (P4) having a maximum in the range of from -95.0 to -99.0 ppm, more preferably of from -96.0 to -98.0 ppm, and more preferably of from -96.5 to - 97.5 ppm. The process of any one of embodiments 1 to 9, wherein the integration of the first, second, third, and optional fourth peaks in the ²⁹ Si MAS NMR of the zeolitic material provided in (i) offers a ratio of the integration values P1 : P2 : P3 : P4 comprised in the range of from (62-86) : (9-29) : (1-6) : (0-8), preferably in the range of from (64-84) : (11-27) : (2-5) : (0-7), and more preferably in the range of from (65-83) : (12-26) : (3-4) : (0-6). 11 . The process of any one of embodiments 1 to 10, wherein the ²⁹ Si MAS NMR of the zeolitic material provided in (i) comprises only three peaks P1 , P2, and P3 or only four peaks P1 , P2, P3, and P4 in the range of from -90 to -120 ppm.

12. The process of any one of embodiments 1 to 11 , wherein the ²⁹ Si MAS NMR of the zeolitic material provided in (i) comprises four peaks, wherein the integration of the first, second, third, and optional fourth peaks in the ²⁹ Si MAS NMR of the zeolitic material provided in (i) offers a ratio of the integration values P1 : P2 : P3 : P4 comprised in the range of from (62-86) : (9-29) : (1-6) : (greater than 0-8), preferably in the range of from (64-84) : (11-27) : (2-5) : (greater than 0-7), and more preferably in the range of from (65-83) : (12-26) : (3- 4) : (greater than 0-6).

13. The process of any one of embodiments 1 to 12, wherein the zeolitic material provided in (I) has a Si : Al molar ratio in the range of from 2 to 100, preferably of from 4 to 50, more preferably of from 6 to 20, more preferably of from 8 to 15, more preferably of from 9 to 14, more preferably of from 9.5 to 13.0, more preferably of from 10.2 to 12.2, and more preferably of from 10.7 to 11 .7.

14. The process of any one of embodiments 1 to 13, wherein the zeolitic material provided in (i) is selected from the group consisting of SSZ-39, SAPO-18, SIZ-8, including mixtures of two or more thereof, wherein the zeolitic material preferably comprises, more preferably consist of, SSZ-39.

15. The process of any one of embodiments 1 to 14, wherein the one or more transition metals are selected from the group consisting of Fe, Cu, and mixtures thereof, wherein the one or more transition metals more preferably are Cu.

16. The process of any one of embodiments 1 to 15, wherein the zeolitic material provided in (I) is ion exchanged with the one or more transition metals.

17. The process of any one of embodiments 1 to 16, wherein the zeolitic material provided in (i) comprises the one or more transition metals, calculated as sum of the weights of the transition metals as elements, in an amount in the range of from 0.1 to 12 wt.-% based on 100 wt.-% of the zeolitic material, preferably of from 0.4 to 8.0 wt.-%, more preferably of from 0.7 to 5.5 wt.-%, more preferably of from 0.9 to 4.0 wt.-%, more preferably of from

1 .1 to 2.5 wt.-%, more preferably of from 1 .3 to 2.3 wt.-%, more preferably of from 1 .5 to

2.1 wt.-%, and more preferably of from 1.7 to 1.9 wt.-% based on 100 wt.-% of the zeolitic material.

18. The process of any one of embodiments 1 to 17, wherein the zeolitic material provided in (I) has a molar ratio of the one or more transition metals comprised in the zeolitic material to the Al comprised in the framework structure of the zeolitic material in the range of from 0.01 :1 to 0.45:1 , preferably in the range of from 0.04:1 to 0.42:1 , more preferably in the range of from 0.07:1 to 0.38:1 , more preferably in the range of from 0.10:1 to 0.34:1 , more preferably in the range of from 0.13:1 to 0.31 :1 , more preferably in the range of from 0.15:1 to 0.29:1 , more preferably in the range of from 0.17:1 to 0.27:1 , more preferably in the range of from 0.19:1 to 0.25:1 , more preferably in the range of from 0.21 :1 to 0.23:1. The process of any one of embodiments 1 to 18, wherein the temperature programmed desorption of ammonia (NH ₃ -TPD) profile of the zeolitic material displays one or more desorption peaks having maxima in the temperature range of from 80 to 230 °C, preferably of from 90 to 220 °C, more preferably of from 100 to 210 °C, more preferably of from 110 to 200 °C, more preferably of from 120 to 190 °C, more preferably of from 130 to 180 °C, more preferably of from 135 to 170 °C, and more preferably of from 140 to 160 °C, wherein the integration of said one or more desorption peaks affords a total value of 0.60 mmol/g or less, preferably in the range of from 0.02 to 0.55 mmol/g, more preferably in the range of from 0.04 to 0.50 mmol/g, more preferably in the range of from 0.06 to 0.45 mmol/g, more preferably in the range of from 0.08 to 0.40 mmol/g, more preferably in the range of from 0.09 to 0.37 mmol/g, more preferably in the range of from 0.10 to 0.34 mmol/g, more preferably in the range of from 0.14 to 0.26 mmol/g, more preferably in the range of from 0.17 to 0.21 mmol/g, wherein the NH3-TPD profile is preferably determined according to Reference Example 5. The process of any one of embodiments 1 to 19, wherein the temperature programmed desorption of ammonia (NH3-TPD) profile of the zeolitic material displays one or more desorption peaks having maxima in the temperature range of from greater than 230 to 370 °C, preferably of from 240 to 360 °C, preferably of from 250 to 350 °C, more preferably of from 260 to 340 °C, more preferably of from 270 to 330 °C, more preferably of from 280 to 320 °C, more preferably of from 285 to 315 °C, and more preferably of from 290 to 310 °C, wherein the integration of said one or more desorption peaks affords a total value of 1 .00 mmol/g or less, preferably in the range of from 0.05 to 0.95 mmol/g, more preferably in the range of from 0.10 to 0.90 mmol/g, more preferably in the range of from 0.30 to 0.85 mmol/g, more preferably in the range of from 0.50 to 0.80 mmol/g, more preferably in the range of from 0.67 to 0.77 mmol/g, more preferably in the range of from 0.71 to 0.75 mmol/g, wherein the NH3-TPD profile is preferably determined according to Reference Example 5. The process of any one of embodiments 1 to 20, wherein the temperature programmed desorption of ammonia (NH3-TPD) profile of the zeolitic material displays one or more desorption peaks having maxima in the temperature range of from greater than 370 to 520 °C, preferably of from 380 to 510 °C, more preferably of from 390 to 510 °C, more preferably of from 400 to 500 °C, more preferably of from 410 to 490 °C, more preferably of from 420 to 480 °C, more preferably of from 430 to 470 °C, more preferably of from 435 to 465 °C, and more preferably of from 440 to 460 °C, wherein the integration of said one or more desorption peaks affords a total value of 0.80 mmol/g or less, preferably in the range of from 0.10 to 0.75 mmol/g, more preferably in the range of from 0.15 to 0.70 mmol/g, more preferably in the range of from 0.20 to 0.65 mmol/g, more preferably in the range of from 0.25 to 0.60 mmol/g, more preferably in the range of from 0.30 to 0.55 mmol/g, more preferably in the range of from 0.35 to 0.52 mmol/g, more preferably in the range of from 0.39 to 0.48 mmol/g, more preferably in the range of from 0.42 to 0.46 mmol/g, wherein the NH3-TPD profile is preferably determined according to Reference Example 5.

22. The process of any one of embodiments 1 to 21 , wherein the integration of the desorption peaks in the NH3-TPD profile of the zeolitic material having maxima in the temperature range of from 50 to 800 °C, preferably of from 80 to 520 °C, preferably of from 90 to 510 °C, more preferably of from 100 to 500 °C, more preferably of from 110 to 490 °C, more preferably of from 120 to 480 °C, more preferably of from 130 to 470 °C, and more preferably of from 140 to 460 °C, affords a total value of 1.70 mmol/g or less, preferably in the range of from 0.45 to 1.60 mmol/g, more preferably in the range of from 0.60 to 1.55 mmol/g, more preferably in the range of from 0.75 to 1 .50 mmol/g, more preferably in the range of from 0.90 to 1.45 mmol/g, more preferably in the range of from 1.10 to 1.40 mmol/g, more preferably in the range of from 1.30 to 1.38 mmol/g, wherein the NH3-TPD profile is preferably determined according to Reference Example 5.

23. The process of any one of embodiments 19 to 22, wherein the NH3-TPD profile is a de- convoluted NH3-TPD profile, and wherein the one or more desorption peaks of the NH ₃ - TPD profile are the one or more deconvoluted desorption peaks of the NH3-TPD profile, wherein deconvolution of the desorption peaks is preferably achieved according to Reference Example 5.

24. The process of any one of embodiments 1 to 23, wherein the zeolitic material provided in (i) further comprises an alkali metal selected from the group consisting of Li, Na, K, Rb, Cs, and mixtures of two or more thereof, preferably from the group consisting of Li, Na, K, and mixtures of two or more thereof, wherein the zeolitic material more preferably further comprises Na, wherein the zeolitic material more preferably is ion exchanged with the alkali metal, preferably with Na.

25. The process of embodiment 24, wherein the zeolitic material has a Na:AI molar ratio of the Na comprised in the zeolitic material to the Al comprised in the framework structure of the zeolitic material in the range of from 0.002:1 to 2.00:1 , preferably in the range of from 0.004:1 to 1.60:1 , more preferably in the range of from 0.006:1 to 1.50:1 , more preferably in the range of from 0.007:1 to 1 .40:1 .

26. The process of any one of embodiments 1 to 25, wherein the zeolitic material provided in (I) has a BET specific surface area in the range of from 200 to 650 m ² /g, preferably from 360 to 560 m ² /g, more preferably from 410 to 510 m ² /g, and more preferably from 430 to 490 m ² /g, wherein the BET surface area is preferably determined according to Reference Example 4.

27. The process of any one of embodiments 1 to 26, wherein the zeolitic material provided in (i) has a total micropore volume in the range of from 0.10 to 0.35 cm ³ /g, preferably from 0.15 to 0.27 cm ³ /g, more preferably from 0.17 to 0.25 cm ³ /g, and more preferably from 0.19 to 0.23 cm ³ /g, wherein the total micropore volume is preferably determined according to Reference Example 4.

28. The process of any one of embodiments 1 to 27, wherein the zeolitic material provided in (i) has a particle size in the range of from 100 to 1200 nm, preferably in the range of from 250 to 1100 nm, more preferably in the range of from 500 to 1000 nm.

29. The process of any one of embodiments 1 to 28, wherein providing a zeolitic material according to (i) comprises, preferably consists of,

(1 ) preparing a mixture comprising a zeolitic material comprising SiC>2 and AI2O3 in its framework structure and having an FER-type framework structure, one or more cationic structure directing agents, and water;

(2) heating the mixture obtained in (1 ) for obtaining the zeolitic material having the AEI- type framework structure and comprising SiO ₂ and AI ₂ O ₃ in its framework structure.

30. The process of embodiment 29, wherein the one or more cationic structure directing agents are selected from the group consisting of N, di(Ci-C ₄ )alkyl-3,5-di(Ci-C4)alkylpyr- rolidinium, /V,A/-di(Ci-C4)alkyl-3,5-di(Ci-C ₄ )alkylpiperidinium, /V,AAdi(Ci-C ₄ )alkyl-3,5-di(Ci- C ₄ )alkylhexahydroazepinium, and mixtures of two or more thereof, preferably from the group consisting of /V,/V-di(Ci-C3)alkyl-3,5-di(Ci-C3)alkylpyrrolidinium, /V,/V-di(Ci-C3)alkyl-3,5-di(Ci-C ₃ )alkylpiperidinium, /V,/V-di(Ci-C3)alkyl-3,5-di(Ci-C ₃ )alkylhex- ahydroazepinium, and mixtures of two or more thereof, more preferably from the group consisting of N, di(Ci-C ₂ )alkyl-3,5-di(Ci-C ₂ )alkylpyrroli- dinium, /V,A/-di(Ci-C ₂ )alkyl-3,5-di(Ci-C ₂ )alkylpiperidinium, /V,Mdi(Ci-C ₂ )alkyl-3,5-di(Ci- C ₂ )alkylhexahydroazepinium, and mixtures of two or more thereof, more preferably from the group consisting of N, di(Ci-C ₂ )alkyl-3,5-di(Ci-C ₂ )alkylpiperi- dinium, and mixtures of two or more thereof, wherein more preferably the one or more cationic structure directing agents comprises /V,/V-dimethyl-3,5-dimethylpiperidinium, wherein more preferably the one or more cationic structure directing agents consists of /,/V-dime- thyl-3,5-dimethylpiperidinium.

31 . The process of embodiment 29 or 30, 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 cationic structure directing agents are provided as hydroxides and/or bromides, and more preferably as hydroxides.

32. The process of any one of embodiments 29 to 31 , wherein the framework structure of the zeolitic material having an FER-type framework structure displays a SiC>2 : AI2O3 molar ratio ranging from 5 to 100, preferably of from 10 to 50, more preferably of from 15 to 41 , more preferably of from 20 to 36, more preferably of from 23 to 33, more preferably of from 25 to 31 , and more preferably of from 27 to 29.

33. The process of any one of embodiments 29 to 32, wherein 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, 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.

34. The process of any one of embodiments 29 to 33, wherein the zeolitic material having an FER-type framework structure is selected from the group consisting of ferrierite, ZSM-35, NU-23, FU-23, ISI-6, [Si-O]-FER, [Ga-Si-O]-FER, [B-Si-O]-FER, and mixtures of two or more thereof, preferably from the group consisting of ferrierite, ZSM-35, NU-23, FU-23, ISI-6, [Si-O]-FER, and mixtures of two or more thereof, wherein more preferably the zeolitic material having an FER-type framework structure comprises ferrierite, wherein more preferably the zeolitic material having an FER-type framework structure is ferrierite.

35. The process of any one of embodiments 29 to 34, wherein the mixture prepared in (1 ) further comprises OH-.

36. The process of embodiment 35, 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, preferably from 0.05 to 3, more preferably from 0.1 to 1.5, more preferably from 0.25 to 1 , more preferably from 0.35 to 0.70, and more preferably from 0.45 to 0.59, and more preferably from 0.51 to 0.52.

37. The process of any one of embodiments 29 to 36, 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.

38. The process of embodiment 37, 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 5, preferably from 0.05 to 3, more preferably from 0.1 to 1 .5, more preferably from 0.15 to 1 , more preferably from 0.2 to 0.5, and more preferably from 0.27 to 0.45, and more preferably from 0.32 to 0.40.

39. The process of embodiment 37 or 38, wherein the one or more alkali metals M are comprised in the mixture prepared in (1) as hydroxide.

40. The process of any one of embodiments 29 to 39, 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.

41 . The process of any one of embodiments 29 to 40, wherein heating in (2) is conducted at a temperature 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 preferably from 135 to 170 °C, more preferably from 140 to 160 °C, and more preferably from 145 to 155 °C.

42. The process of any one of embodiments 29 to 41 , wherein heating in (2) is conducted under autogenous pressure, preferably under hydrothermal conditions.

43. The process of any one of embodiments 29 to 42, wherein heating in (2) is performed in a pressure tight vessel, preferably in an autoclave.

44. The process of any one of embodiments 29 to 43, wherein heating in (2) is conducted for a duration in the range of from 3 h to 10 d, preferably from 6 h to 8 d, more preferably from 8 h to 6 d, more preferably from 10 h to 3 d, more preferably from 15 h to 1 .5 d, more preferably from 21 to 27, and more preferably from 23 to 25 h.

45. The process of any one of embodiments 29 to 44, wherein the zeolitic material obtained in

(2) 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 obtained in (2) comprises SSZ-39, and wherein more preferably the zeolitic material obtained in (2) is SSZ- 39.

46. The process of any one of embodiments 29 to 45, further comprising

(3) calcining the zeolitic material obtained in (2).

47. The process of any one of embodiments 29 to 46, 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 framework structure of the zeolitic material is ion-exchanged against one or more of H ⁺ , NH ₄ ⁺ , and Na, more preferably against NH Tor Na. The process of any one of embodiments 29 to 47, further comprising

(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 framework structure of the zeolitic material is ion-exchanged against one or more transition metals, preferably against one or more transition metals selected from the group consisting of Fe, Cu, and mixtures thereof, more preferably against copper. The process of embodiment 48, further comprising

(6) subjecting the zeolitic material obtained in (5) to an ion-exchange procedure, wherein one or more ionic extra-framework elements contained in the framework structure of the zeolitic material is ion-exchanged against Na. The process of embodiment 48 or 49, further comprising

(7) calcining the zeolitic material obtained in (5) or (6). The process of any one of embodiments 46 to 50, wherein the temperature of calcination in (3) and/or (6) is in the range of from 300 to 1000°C, preferably of from 400 to 800°C, more preferably of from 450 to 650°C, and more preferably of from 500 to 600°C. The process of any one of embodiments 46 to 51 , wherein calcining in (3) and/or (6) is conducted for a period in the range of from 0.5 to 20 h, 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, and more preferably from 4.5 to 6.5 h. The process of any one of embodiments 29 to 52, wherein the mixture in (1 ) further comprises seed crystals, wherein the seed crystals preferably comprise a zeolitic material having an AEl-type framework structure, wherein more preferably the zeolitic material consists of a zeolitic material having an AEl-type framework structure. The process of embodiment 53, wherein the zeolitic material having an AEl-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 preferably the zeolitic material having an AEl-type framework structure comprised in the seed crystals is SSZ-39, preferably calcined SSZ-39. The process of embodiment 53 or 54, 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 SiO ₂ in the mixture prepared in (1), 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 SIO ₂ in the mixture prepared in (1) calculated as SiO ₂ . The present invention is further illustrated by the following reference examples, examples and comparative examples.

EXAMPLES

Reference Example 1 : Determination of ²⁹ Si MAS NMR

Solid-state ²⁹ Si MAS NMR spectra were measured on a JEOL ECA-600 spectrometer at a resonance frequency of 156.4 MHz using a 4 mm sample rotor with a spinning rate of 15.0 kHz. The ²⁹ Si chemical shifts were referenced to polydimethylsiloxane (PDMS) at -34.12 ppm. The percentage of framework Al (AI _F ) distribution was calculated based on the area of the deconvoluted peak of ²⁹ Si MAS NMR. For the deconvolution of NMR, the software "Peakfit" by the Gaussian Fitting method was used. The software "Origin" by the Gaussian Fitting method could be used as well. The following boundaries according to D. Freude, J. Karger in Handbook of porous solids, 2002 were used to assign the signal to specific species:

Q4(2AI): -107 to -115 ppm,

Q3(0AI): -103 to -107 ppm,

Q4(1AI): -99 to -103 ppm,

Q4(0AI): -96 to -98 ppm.

Reference Example 1 : Determination of X-ray powder diffraction

XRD pattern was collected on a Rint-Ultima III (Rigaku) using a Cu Ka X-ray source (40 kV, 20 mA).

Reference Example 3: Elemental analysis

Elemental analyses of the s ample were performed on an inductively coupled plasma-atomic emission spectrometer (ICP-AES, Shimadzu ICPE-9000).

Reference Example 4: Determination of micro- and meso-porosities

Nitrogen adsorption and desorption measurements to obtain the information on the micro- and meso-porosities (BET specific surface area as well as total micropore volume) were conducted at 77 K on a Belsorp-mini II (MicrotracBEL).

Reference Example 5: Determination of temperature programmed desorption of ammonia

(NH3-TPD)

Temperature-programmed ammonia desorption (NH3-TPD) profiles were recorded on Multitrack TPD equipment (Japan BEL). Typically, 25 mg of catalyst was pretreated at 873 K in He (50 mL min ^-1 ) for 1 h and then cooled to 373 K. Prior to the adsorption of NH3, the sample was evacuated at 373 K for 1 h. Approximately 2500 Pa of NH ₃ was allowed to make contact with the sample at 373 K for 10 min. Subsequently, the sample was evacuated to remove weakly adsorbed NH3 at the same temperature for 30 min. Finally, the sample was cooled to 373 K and heated from 373 to 873 K at a ramping rate of 10 K min ^-1 in a He flow (50 mL min ^-1 ). A TCD was used to monitor desorbed NH3. The amount of acid sites was determined by using the area in the profiles. For the deconvolution of NH3-TPD, the software “ChemMaster” by the DFP method (Da- vidon-Fletcher-Powell algorithm) that comes with the instrument was used.

Comparative Example 1 : Preparation of a FER-type zeolitic materials ion-exchanged with Cu

A FER-type zeolitic material ion-exchanged with Cu was prepared by using NH4-form FER zeolite (CP914C, Si/AI=28, Zeolyst) to exchange with 5 mmol/L Cu(NO ₃ ) ₂ solution at a 100 mL/g liq- uid-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 denoted as 5 Cu/FER.

Comparative Example 2: Preparation of a CHA-type zeolitic material ion-exchanged with Cu

The CHA-type aluminosilicate zeolite was synthesized according to R. Xu et. al., H ₂ O-Built Proton Transfer Bridge Enhances Continuous Methane Oxidation to Methanol over Cu-BEA Zeolite in Angew. Chem. Int. Ed. 2021 , 60, 16634-16640. The molar composition of the mother gel was 1 SiO ₂ : 0.05 AI ₂ OS: 0.2 NaOH: 0.2 TMAdaOH: 20 H ₂ O: 5wt.% seed. The prepared mother gel was crystallized at 423 K in a rotating oven under tumbling condition with 40 rpm for 5 days. Subsequently, the following steps, including the preparation of the CHA-type zeolitic material ion-exchanged with Cu were the same as described below for the AEl-type zeolitic materials ion-exchanged with Cu. The resulting product is also designated as 5 Cu/CHA herein.

Example 3: Preparation of AEl-type zeolitic materials ion-exchanged with Cu

The AEl-type aluminosilicate zeolite, i.e. SSZ-39, has been prepared by the interzeolitic conversion (IZC) method from FER zeolite (CP914C, Si/AI=28, Zeolyst) in the guidance of 1 ,1 ,3,5-tet- ramethylpiperidinium hydroxide under hydrothermal conditions as follows. The prepared gel with molar ratio of 1 SIO ₂ : 0.017 AI ₂ O ₃ : 0.155 OSDA: 0.36 NaOH: 20 H ₂ O with 5% seed crystals (calcined SSZ-39, based on 100 weight-% SiO ₂ in the synthesis gel) was crystallized at 150 °C in a rotating oven at 40 rpm for 1 day. The obtained as-synthesized product was filtered, dried overnight and calcined for 10 h in air. To regulate the Al distribution, 550, 750 and 950 °C were adapted as the calcination temperature, respectively. The calcined samples were remarked as AEl-t, where t meant the calcination temperature.

Afterwards, these samples were exchanged twice with 2.5 M NH4NO3 aqueous solution at 80 °C for 3 h to obtain the NH ₄ -form samples. Subsequently, the NH ₄ -form samples were exchanged with 5 mmol/L Cu(NO ₃ ) ₂ solution 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 denoted as 5Cu/AEI-t. To investigate the effect of Cu content, 1 , 10 and 50 mmol/L CU(NOS)2 solutions were used to exchange with the NH4-type AEI-550 zeolite at a 100 mL/g liq- uid-to-solid ratio stirring at 80 °C for 24 h. The suspension was filtered, washed, dried and cal- cined in air at 550 °C for 5 h. The obtained samples were noted as xCu/ AEI-550, where x meant the concentration in mmol/L of the Cu(NC>3)2 solution.

The 5Cu/AEI-550 sample were calcined in air at 550, 750, 950 °C for 10 h, respectively. The obtained samples were denoted as [5Cu/AEI-550]-t, where t meant the calcination temperature.

Table 1 :

Overview on the analytical data for the samples after calcination and prior to Cu-exchange according to Example 3 as determined according to Reference example 1.

(*) peak maxima from deconvolution of the signal in the ²⁹ Si MAS NMR spectrum; (**) calculated by deconvolution of the ²⁹ Si MAS NMR spectrum, Q ⁴ (nAI) and Q ³ (0AI) represent

Si(OSi) ₄ -n(OAI) _n and Si(OH)-(OSi)3, respectively.

Table 2

Overview on the analytical data for the samples according to Example 3.

Example 4: Catalytic testing

The prepared zeolitic materials were tested with respect to their catalytic activity in a continuous reaction oxidation of methane. The continuous oxidation of methane reaction was performed in a fixed-bed flow reactor. The online-reaction-analysis system was equipped with two six-port inlet valves (Figure 1). In each run, 100 mg of a zeolite catalyst in a granular form (particle size 500-1000 pm) 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 flow. The reaction was conducted at temperatures ranging from 300 to 450 °C in a flowing gas mixture of CH ₄ , N2O, H2O and Ar with flow rates of 10, 10, 2 and 3 mL-min ^-1 , respectively (Figure 2). The weight hourly space velocity was set to 15000 mL g- ¹ IT ¹ . The outlet gas, containing the products, unreacted CH4 and N2O, were analyzed using two on-line gas chromatographs (GC; GC-2014, Shinn adzu) . One of the GCs was used with a Shin carbon ST 50/80 packed column (Agilent T ech- nologies, inner diameter 3 mm, length 6 m) and a TCD detector. Specifically, GC-TCD was used to detect H ₂ , N ₂ O, CO, CO ₂ and CH ₄ . The other GC was equipped with a Porapak Q 80/100 packed column (Agilent Technologies, inner diameter 3 mm, length 6 m), a flame ionization detector (FID), and a methanizer. The GC-FID was used to investigate CH ₄ , and the produced methanol (MeOH), dimethyl ether (DME), alkane and alkenes. The yield of each carbon-containing product was calculated by considering the number of carbon atoms. The methane conversion in this study was defined as the total obtained products, and calculated as:

C _CH4 = Z(i*Ci)/(Z(i*Ci)+CH4) where CCH ₄ is the CH4 conversion, i is the number of carbon atoms in product Ci, Z(i*Ci) is the total amount of carbon of all the products, and CH4 is the amount of CH ₄ detected at the same time.

The N ₂ O conversion was calculated as:

CN2O = (ni - na)/ni where CN2O is the N2O conversion, ni is the initial N2O molar weight, na is the N2O molar weight after reaction.

The product selectivity is calculated as:

S _Ci = (i*Ci)/Z(i*Ci) where Sci is the selectivity of the product Ci, Z(i*Ci) is the total amount of carbon of all the products. The product yield is calculated as:

Y _Ci = (i*Ci)/(Z(i*Ci)+CH4) where Yci is the yield of the product Ci, Z(i*Ci) is the total amount of carbon of all the products, and CH4 is the amount of CH ₄ detected at the same time.

The products formation rates are calculated as:

Rci - Yci*FcH4/m _cat where Rci is the formation rate of product Ci, FCH ₄ is the initial flow rate of CH4, m _ca t is the mass of catalyst.

The catalytic stability, i.e. the variation of reaction performance with time in continuous oxidation of methane was performed in the same reaction system, whereby the reaction temperature was set to 350 °C, and the reaction was performed continually at this temperature. The temperature program was sketched in Figure 3. The other process and details were alike to the abovementioned continuous partial oxidation of methane reaction.

The results for the catalytic testing are shown in table 3 below.

Table 3:

Overview on the analytical data for the samples 5Cu/AEI-550, 10Cu/AEI-750, and [5Cu/AEI- 550]-750 according to Example 3, as well as for 5 Cu/FER according to Comparative Example 1.

It is worth mentioning that the zeolite catalysts realized much higher than the 5Cu/FER and 5Cu/CHA zeolite catalysts. The 10Cu/AEI-750 sample presented a similar result, the initial outstanding result of 30.7 pmol-g- ¹ -min- ¹ methanol rate with 30.8 % selectivity sustained 6 hours.

The results of the catalytic testing with respect to the conversion of N ₂ O are shown in tables 4 and 5 below.

Table 4 Results for the N2O conversion in the continuous direct oxidation of methane to methanol (cDMTM) over Cu/AEI-550, Cu/AEI-750, Cu/AEI-950, 1 Cu/AEI-550, 10Cu/AEI-550, and 50Cu/AEI-550, in relation to the reaction temperature. As can be gathered from the results shown in table 4, the zeolitic material according to the present invention achieves a good conversion of N ₂ O, especially at temperatures of 400 to 450 °C.

Table 5

Results for the N2O conversion in the continuous direct oxidation of methane to methanol (cDMTM) over 5Cu/AEI-550 and 50Cu/AEI-550 zeolite catalysts in the cDMTM reaction.

As can be gathered from the results shown in table 5, the zeolitic materials of the present invention achieve a stable conversion rate of N ₂ O over a long period of time.

Brief description of figures

Figure 1 : shows the reactor set-up for the catalytic testing according to Example 4.

Figure 2: shows the program for conducting the catalytic testing according to Example 4, wherein the reaction temperature was varied in the range of from 300 to 450 °C.

Figure 3: shows the program for conducting the catalytic testing according to Example 4, wherein the reaction temperature was set to 350 °C.

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