# US 9,517,942 B2 · Transition-metal-containing zeolite

> Agents: this data is available as JSON from the patentgrep API and MCP server — see https://patentgrep.com/llms.txt

- Number: US 9,517,942 B2
- Document ID: US9517942B2
- Status: Granted
- Kind: B2
- Application number: 14/616,889
- Filed: 2015-02-09
- Published: 2015-08-06
- Granted: 2016-12-13
- Earliest claimed: 2011-06-27
- Assignees: Mitsubishi Plastics, Inc.
- Applicants: Mitsubishi Plastics, Inc.
- Inventors: Haijun Chen; Takahiko Takewaki; Takeshi Matsuo
- Web page: https://patentgrep.com/patent/US9517942B2

## CPC

- C01B 39/54: Phosphates, e.g. APO or SAPO compounds
- B01D 53/28: Selection of materials for use as drying agents
- B01D 53/94: by catalytic processes
- 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 20/28064: {being in the range 500-1000 m2/g}
- B01J 20/3078: {Thermal treatment, e.g. calcining or pyrolizing}
- B01J 29/763: {CHA-type, e.g. Chabazite, LZ-218}
- B01J 29/84: Aluminophosphates containing other elements, e.g. metals, boron
- B01J 29/85: Silicoaluminophosphates [SAPO compounds]
- B01J 35/617: {500-1000 m2/g}
- B01J 37/10: in the presence of water, e.g. steam
- B01D 2251/2062: Ammonia
- B01D 2253/108: Zeolites
- B01D 2253/1085: characterized by a silicon-aluminium ratio
- B01D 2253/25: Coated, impregnated or composite adsorbents
- B01D 2255/20738: Iron
- B01D 2255/20761: Copper
- B01D 2255/50: Zeolites
- B01D 2255/9207: Specific surface
- B01J 35/30: characterised by their physical properties
- B01J 2229/186: not in framework positions
- B01J 2235/00: Indexing scheme associated with group B01J35/00, related to the analysis techniques used to determine the catalysts form or properties
- B01J 2235/15: X-ray diffraction
- B01J 2235/30: Scanning electron microscopy; Transmission electron microscopy
- Y10T 428/2982: Particulate matter [e.g., sphere, flake, etc.]
- C01B: NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; {METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C}
- 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)
- B01J: CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- Y10T: TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION

## Abstract

A transition-metal-containing silicoaluminophosphate zeolite having excellent high-temperature hydrothermal durability is easily and efficiently produced. A method for producing a transition-metal-containing zeolite that contains a silicon atom, a phosphorus atom, and an aluminum atom in at least its framework structure includes hydrothermal synthesis using an aqueous gel containing a silicon atom raw material, an aluminum atom raw material, a phosphorus atom raw material, a transition metal raw material, and a polyamine (other than diamines). A transition-metal-containing silicoaluminophosphate zeolite produced by hydrothermal synthesis using a zeolite raw material and the aqueous gel containing the transition metal raw material and the polyamine has excellent high-temperature hydrothermal durability and high catalytic activity.

## Claims

### Claim 1

An aluminophosphate zeolite containing 3% by weight or more transition metal M, wherein element mapping of the transition metal M in the zeolite determined with an electron probe microanalyzer shows that the coefficient of variation in intensity of the transition metal M is 33% or less and that the molar ratio of an aluminum atom to the total of a silicon atom and a phosphorus atom is 0.9 or more, and wherein the transition metal M is copper.

### Claim 2 (depends on 1)

The transition-metal-containing zeolite according to claim 1, wherein the zeolite has an 8-membered ring structure in its framework structure.

### Claim 3 (depends on 1)

The transition-metal-containing zeolite according to claim 1, wherein the zeolite has a BET specific surface area of 500 m2/g or more.

### Claim 4 (depends on 1)

The transition-metal-containing zeolite according to claim 1, wherein the zeolite has a framework density of 10.0 T/1000 cubic angstroms or more and 16.0 T/1000 cubic angstroms or less in accordance with a zeolite structure defined by the International Zeolite Association (IZA).

### Claim 5 (depends on 1)

The transition-metal-containing zeolite according to claim 1, wherein the zeolite has a zeolite structure of CHA as defined by the International Zeolite Association (IZA).

### Claim 6 (depends on 1)

An exhaust gas treatment catalyst, comprising the transition-metal-containing zeolite according to claim 1.

### Claim 7 (depends on 1)

A water vapor adsorbent, comprising the transition-metal-containing zeolite according to claim 1.

### Claim 8 (depends on 1)

The transition-metal-containing zeolite according to claim 1, produced by the method for producing a transition-metal-containing zeolite that contains at least a silicon atom, a phosphorus atom, and an aluminum atom in its framework structure, comprising: hydrothermal synthesis using an aqueous gel containing a silicon atom raw material, an aluminum atom raw material, a phosphorus atom raw material, a transition metal raw material, and a polyamine (other than diamines).

### Claim 9 (depends on 8)

The transition-metal-containing zeolite according to claim 8, wherein the aqueous gel further contains at least one selected from the group consisting of alicyclic heterocyclic compounds containing at least a nitrogen atom as a heteroatom, alkylamines, cycloalkylamines, and tetraalkylammonium hydroxides.

### Claim 10 (depends on 8)

The transition-metal-containing zeolite according to claim 8, wherein the polyamine has a general formula of H2N—(CnH2nNH)x—H (wherein n denotes an integer in the range of 2 to 6, and x denotes an integer in the range of 2 to 10).

### Claim 11 (depends on 8)

The transition-metal-containing zeolite according to claim 8, wherein
the molar ratios of the aluminum atom raw material, the silicon atom raw material, the phosphorus atom raw material, and the transition metal (M) raw material of the aqueous gel on an oxide basis are as follows:
the SiO2/Al2O3 ratio is 0.1 or more and 0.8 or less,
the P2O5/Al2O3 ratio is 0.6 or more and 1.2 or less, and
the MaOb/Al2O3 ratio is 0.05 or more and 1 or less (wherein a and b denote the atomic ratios of M and O, respectively).

### Claim 12 (depends on 1)

The aluminophosphate zeolite according to claim 1, wherein the coefficient of variation in intensity of the transition metal M is 31% or less.

### Claim 13 (depends on 1)

The aluminophosphate zeolite according to claim 1, wherein the coefficient of variation in intensity of the transition metal M is 29% or less.

### Claim 14 (depends on 1)

The aluminophosphate zeolite according to claim 1, wherein the molar ratio of an aluminum atom to the total of a silicon atom and a phosphorus atom is 0.93 or more.