# US 10,478,810 B2 · Zeolite catalyst and method for producing lower olefin

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- Number: US 10,478,810 B2
- Document ID: US10478810B2
- Status: Granted
- Kind: B2
- Application number: 15/988,744
- Filed: 2018-05-24
- Published: 2018-09-20
- Granted: 2019-11-19
- Earliest claimed: 2015-11-25
- Assignees: Mitsubishi Chemical Corporation; Japan Technological Research Association of Artificial Photosynthetic Chemical Process
- Applicants: Mitsubishi Chemical Corporation; Japan Technological Research Association of Artificial Photosynthetic Chemical Process
- Inventors: Hiroaki Onozuka; Masahiro Hara; Masato Yoshioka; Toshiyuki Yokoi
- Web page: https://patentgrep.com/patent/US10478810B2

## CPC

- B01J 29/70: of types characterised by their specific structure not provided for in groups B01J29/08 - B01J29/65
- B01D 53/00: Separation 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, (recovery of volatile solvents by condensation B01D5/00; sublimation B01D7/00; cold traps, cold baffles B01D8/00; working-up undefined gaseous mixtures obtained by cracking hydrocarbon oils C10G70/00; cleaning coal gas C10K; working-up of natural gas, or synthetic natural gas, C10L3/10; separation of difficult-to-condense gases or air by liquefaction F25J; for investigating materials G01N30/00)
- B01D 53/9418: {for removing nitrogen oxides by selective catalytic reduction [SCR] using a reducing agent in a lean exhaust gas}
- B01J 20/18: Synthetic zeolitic molecular sieves
- B01J 20/28002: {characterised by their physical properties}
- B01J 20/28004: {Sorbent size or size distribution, e.g. particle size}
- B01J 20/28011: {Other properties, e.g. density, crush strength}
- B01J 29/48: containing arsenic, antimony, bismuth, vanadium, niobium tantalum, polonium, chromium, molybdenum, tungsten, manganese, technetium or rhenium
- B01J 29/72: containing iron group metals, noble metals or copper
- B01J 29/76: Iron group metals or copper
- B01J 35/40: characterised by dimensions, e.g. grain size (in a colloidal state B01J35/23; crystallite size B01J35/77)
- B01J 35/45: Nanoparticles
- B01J 35/70: characterised by their crystalline properties, e.g. semi-crystalline (catalysts comprising carbon B01J21/18; molecular sieves B01J29/00)
- B01J 37/04: Mixing {(B01J37/0009, B01J37/0018 take precedence)}
- C01B 39/48: using at least one organic template directing agent
- C07C 1/20: starting from organic compounds containing only oxygen atoms as heteroatoms
- C07C 11/04: Ethene
- C07C 11/06: Propene
- C07C 11/08: with four carbon atoms
- B01D 2255/1021: Platinum
- B01D 2255/1023: Palladium
- B01D 2255/1028: Iridium
- B01D 2255/104: Silver
- B01D 2255/106: Gold
- B01D 2255/2063: Lanthanum
- B01D 2255/2065: Cerium
- B01D 2255/2066: Praseodymium
- B01D 2255/20707: Titanium
- B01D 2255/20715: Zirconium
- B01D 2255/20738: Iron
- B01D 2255/20746: Cobalt
- B01D 2255/20761: Copper
- B01D 2255/50: Zeolites
- B01D 2255/9202: Linear dimensions
- B01D 2255/9205: Porosity
- B01D 2255/9207: Specific surface
- B01J 35/30: characterised by their physical properties
- B01J 2235/00: Indexing scheme associated with group B01J35/00, related to the analysis techniques used to determine the catalysts form or properties
- B01J 2235/05: Nuclear magnetic resonance [NMR]
- B01J 2235/15: X-ray diffraction
- B01J 2235/30: Scanning electron microscopy; Transmission electron microscopy
- C01B 39/04: using at least one organic template directing agent, e.g. an ionic quaternary ammonium compound or an aminated compound
- C07C 2529/70: of types characterised by their specific structure not provided for in groups C07C2529/08 - C07C2529/65
- 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
- B01D: SEPARATION (separating solids from solids by wet methods B03B, B03D; by pneumatic jigs or tables B03B; by other dry methods B07; magnetic or electrostatic separation of solid materials from solid materials or fluids, separation by high-voltage electric fields B03C; centrifuges, vortex apparatus B04; presses per se for squeezing-out liquid from liquid-containing material B30B9/02; treatment of water C02F, e.g. softening by ion-exchange C02F1/42; {arrangements of air intake cleaners in gas turbine plants F02C7/05} ; arrangements or mounting of filters in air-conditioning, air-humidification or ventilation F24F13/28)
- C01B: NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; {METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C}
- C07C: ACYCLIC OR CARBOCYCLIC COMPOUNDS
- Y02P: CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS

## Abstract

A zeolite catalyst capable of maintaining a high conversion of raw materials over a long period of time, and a method of producing a lower olefin stably over a long period of time using the zeolite catalyst is to be provided. A CON zeolite catalyst containing aluminum (Al) as a constituent element, wherein the CON zeolite catalyst has a ratio ((A2/A1)×100 (%)) of an integrated intensity area (A2) of signal intensity in a range from 57.5 ppm to 70 ppm to an integrated intensity area (A1) of signal intensity in a range from 45 ppm to 70 ppm is not less than 49.0% when analyzed by 27Al-MAS-NMR is prepared, and a lower olefin is produced by a MTO process using the zeolite catalyst.

## Claims

### Claim 1

A CON zeolite catalyst comprising aluminum (Al) as a constituent element, wherein the CON zeolite catalyst has an integrated intensity area (A2) of signal intensity in a range from 57.5 ppm to 70 ppm to an integrated intensity area (A1) of signal intensity in a range from 45 ppm to 70 ppm such that (A2/A1)×100(%) is not less than 49.0% when analyzed by 27Al-MAS-NMR.

### Claim 2 (depends on 1)

The zeolite catalyst according to claim 1, wherein an average primary particle diameter is not more than 1000 nm.

### Claim 3 (depends on 1)

The zeolite catalyst according to claim 1, wherein a molar ratio (Si/Al) of silicon (Si) to aluminum (Al) is not less than 10.

### Claim 4 (depends on 1)

A method of producing a lower olefin, comprising a step of making a raw material containing methanol and/or dimethyl ether come into contact with the zeolite catalyst according to claim 1.

### Claim 5 (depends on 1)

The zeolite catalyst according to claim 1, wherein the (A2/A1)×100(%) is 90.0% or less when analyzed by 27Al-MAS-NMR.

### Claim 6 (depends on 1)

The zeolite catalyst according to claim 1, wherein a molar ratio (Si/Al) of silicon (Si) to aluminum (Al) is 1500 or less.

### Claim 7 (depends on 1)

The zeolite catalyst according to claim 1, wherein the zeolite catalyst comprises boron and the molar ratio (Si/B) of silicon (Si) to boron (B) is 50 or more.

### Claim 8 (depends on 1)

The zeolite catalyst according to claim 1, wherein the zeolite catalyst comprises zinc and the molar ratio (Si/Zn) of silicon (Si) to zinc (Zn) is 50 or more.

### Claim 9 (depends on 1)

The zeolite catalyst according to claim 1, wherein an average primary particle diameter is 20 nm or more.

### Claim 10 (depends on 1)

The zeolite catalyst according to claim 1, wherein the BET specific surface area of the zeolite catalyst is 200 m2/g or more.

### Claim 11 (depends on 1)

The zeolite catalyst according to claim 1, wherein the BET specific surface area of the zeolite catalyst is 1000 m2/g or less.