# US 11,992,828 B2 · Molecular sieves with intergrown phases of AEI and CHA topologies and catalyst thereof

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- Number: US 11,992,828 B2
- Document ID: US11992828B2
- Status: Granted
- Kind: B2
- Application number: 18/337,070
- Filed: 2023-06-19
- Published: 2023-10-19
- Granted: 2024-05-28
- Earliest claimed: 2022-01-05
- Assignees: China Automotive Technology and Research Center Co., Ltd; Catarc Automotive Test Center (Tianjin) Co., Ltd
- Applicants: China Automotive Technology and Research Center Co., Ltd; Catarc Automotive Test Center (Tianjin) Co., Ltd
- Inventors: Kaixiang Li; Zhenguo Li; Xiaoning Ren; Yuankai Shao; Jianhai Wang; Li Zhang; Lingfeng Jia; Cheng Lv
- Web page: https://patentgrep.com/patent/US11992828B2

## CPC

- B01J 29/80: Mixtures of different zeolites
- B01J 29/005: {Mixtures of molecular sieves comprising at least one molecular sieve which is not an aluminosilicate zeolite, e.g. from groups B01J29/03 - B01J29/049 or B01J29/82 - B01J29/89}
- B01J 29/061: {containing metallic elements added to the zeolite}
- B01J 29/068: Noble metals
- B01J 29/072: Iron group metals or copper
- B01J 29/076: containing arsenic, antimony, bismuth, vanadium, niobium, tantalum, polonium, chromium, molybdenum, tungsten, manganese, technetium or rhenium
- B01J 29/70: of types characterised by their specific structure not provided for in groups B01J29/08 - B01J29/65
- B01J 29/7015: {CHA-type, e.g. Chabazite, LZ-218}
- B01J 29/74: Noble metals
- B01J 29/743: {CHA-type, e.g. Chabazite, LZ-218}
- B01J 29/76: Iron group metals or copper
- B01J 29/763: {CHA-type, e.g. Chabazite, LZ-218}
- B01J 29/783: {CHA-type, e.g. Chabazite, LZ-218}
- B01J 29/83: Aluminophosphates [APO compounds]
- B01J 29/85: Silicoaluminophosphates [SAPO compounds]
- B01J 37/0018: {Addition of a binding agent or of material, later completely removed among others as result of heat treatment, leaching or washing,(e.g. forming of pores; protective layer, desintegrating by heat)}
- B01J 37/0236: {Drying, e.g. preparing a suspension, adding a soluble salt and drying}
- B01J 37/033: {Using Hydrolysis}
- B01J 37/036: {to form a gel or a cogel}
- B01J 37/06: Washing {(B01J37/0009, B01J37/0018 take precedence)}
- B01J 37/082: {Decomposition and pyrolysis}
- C07C 2/84: catalytic
- C10G 11/05: Crystalline alumino-silicates, e.g. molecular sieves
- B01J 2029/062: {Mixtures of different aluminosilicates}
- B01J 2229/18: to introduce other elements into or onto the molecular sieve itself
- B01J 2229/186: not in framework positions
- B01J 2229/62: in or on other molecular sieves
- Y02P 20/52: using catalysts, e.g. selective catalysts
- Y02P 30/20: using bio-feedstock
- Y02P 30/40: Ethylene production
- B01J: CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- C07C: ACYCLIC OR CARBOCYCLIC COMPOUNDS
- C10G: CRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION (cracking to hydrogen or synthesis gas C01B; cracking or pyrolysis of hydrocarbon gases to individual hydrocarbons or mixtures thereof of definite or specified constitution C07C; cracking to cokes C10B); RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
- Y02P: CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS

## Abstract

The present disclosure provides molecular sieves with intergrown phases of AEI and CHA topologies and a catalyst thereof. A preparation method for the molecular sieves include the following steps: mixing a hydroxyphosphono organic alkali R with an aluminum source and a silicon source to obtain a sol-gel precursor, putting the sol-gel precursor into a closed hydrothermal synthesis reactor for reaction, filtering the reaction solution, washing, drying, and calcination to obtain the molecular sieves with intergrown phases of AEI and CHA topologies. The molecular sieves and the catalyst thereof can be directly synthesized under mild conditions with a hydroxyphosphono organic alkali as a structure-directing agent and a phosphorus source, have a pH value of 6-9 and low requirements for corrosion resistance of production devices, and are suitable for large-scale production.

## Claims

### Claim 1

Molecular sieves with intergrown phases of AEI and CHA topologies, wherein a method for preparing the molecular sieves comprise the following steps:
(1) dissolving a hydroxyphosphono organic alkali R in water and stirring evenly; adding an aluminum source, stirring and dispersing the mixture to be gelatinous, slowly adding a silicon source, stirring and reacting for 2 h-6 h, then standing for fully aging to obtain a sol-gel precursor, wherein the aluminum source and the silicon source are calculated based on Al2O3 and SiO2 respectively, a mass ratio of the silicon source, the aluminum source, the hydroxyphosphono organic alkali R, and the deionized water is SiO2:Al2O3:R:H2O=(0.01-30):1:(0.2-30):(5-300), and depending on acidity and alkalinity of raw materials, a pH value of the sol-gel precursor is in a range of 6-9; and
(2) putting the sol-gel precursor into a closed hydrothermal synthesis reactor for isothermal hydrothermal reaction at 130° C.-220° C. for 6.5 h-48 h, followed by pressure relief, solid-liquid separation, thorough washing of a filter cake, drying, and calcination, to obtain H-type molecular sieves with the intergrown phases of AEI and CHA topologies;
wherein the hydroxyphosphono organic alkali R has a molecular weight of less than 5,000, and contains at least one of cations shown in Formulas I-XI:
and
an anion of the hydroxyphosphono organic alkali R is at least one selected from a group consisting of OH−, NO3−, Br−, HCO3−, CO32−, HSO3−, and HSO4−.

### Claim 2 (depends on 1)

The molecular sieves according to claim 1, wherein a molecule of the hydroxyphosphono organic alkali R has a size of less than 3.7 angstroms in an aqueous phase.

### Claim 3 (depends on 1)

The molecular sieves according to claim 1, wherein the molecular sieves include at least one of AlPO4-18, SAPO-18, and SSZ-39 with the AEI topology and at least one of SSZ-13, SAPO-34, SAPO-44, ZK-14, and AlPO-34 with the CHA topology.

### Claim 4 (depends on 1)

A catalyst, comprising the molecular sieves with the AEI and CHA symbiotic topologies according to claim 1 and an active metal element M.

### Claim 5 (depends on 4)

The catalyst according to claim 4, wherein the active metal element M is at least one selected from a group consisting of Cu, Fe, Co, Mo, Mn, Sm, Pd, Pt, Rh, Au, Ag, Ru, Ni, Nb, and Cr.