# US 10,500,572 B2 · Catalytic extruded, solid honeycomb body

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- Number: US 10,500,572 B2
- Document ID: US10500572B2
- Status: Granted
- Kind: B2
- Application number: 15/928,316
- Filed: 2018-03-22
- Published: 2018-07-26
- Granted: 2019-12-10
- Earliest claimed: 2014-01-23
- Assignees: Johnson Matthey Catalysts (Germany) GMBH
- Applicants: Johnson Matthey Catalysts (Germany) GmbH
- Inventors: Juergen Bauer; Ralf Dotzel; Joerg Walter Jodlauk; Rainer Leppelt; Joerg Werner Muench
- Web page: https://patentgrep.com/patent/US10500572B2

## CPC

- B01J 29/763: {CHA-type, e.g. Chabazite, LZ-218}
- B01D 53/9418: {for removing nitrogen oxides by selective catalytic reduction [SCR] using a reducing agent in a lean exhaust gas}
- B01J 21/12: Silica and alumina
- B01J 21/16: Clays or other mineral silicates
- 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 29/049: {Pillared clays}
- B01J 35/57: Honeycombs
- B01J 35/58: Fabrics or filaments
- B01J 37/0009: {Use of binding agents; Moulding; Pressing; Powdering; Granulating; Addition of materials ameliorating the mechanical properties of the product catalyst}
- 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 37/0215: {Coating}
- B01J 37/04: Mixing {(B01J37/0009, B01J37/0018 take precedence)}
- C04B 35/18: rich in aluminium oxide
- C04B 35/26: based on ferrites
- C04B 35/447: based on phosphates {, e.g. hydroxyapatite}
- C04B 38/0006: {Honeycomb structures (from one or more corrugated sheets by winding or stacking C04B38/0083)}
- F01N 3/0814: {combined with catalytic converters, e.g. NOx absorption/storage reduction catalysts}
- F01N 3/0842: {Nitrogen oxides}
- F01N 3/103: {Oxidation catalysts for HC and CO only}
- F01N 3/2066: {Selective catalytic reduction [SCR]}
- F01N 3/2835: {fibrous}
- B01D 2251/2062: Ammonia
- B01D 2255/20738: Iron
- B01D 2255/20761: Copper
- B01D 2255/2092: Aluminium
- B01D 2255/30: Silica
- B01D 2255/50: Zeolites
- B01D 2257/404: Nitrogen oxides other than dinitrogen oxide
- B01J 37/32: Freeze drying, i.e. lyophilisation
- B01J 2229/186: not in framework positions
- B01J 2229/42: Addition of matrix or binder particles
- C04B 2111/00793: {as filters or diaphragms}
- C04B 2111/0081: {as catalysts or catalyst carriers}
- C04B 2235/3217: Aluminum oxide or oxide forming salts thereof, e.g. bauxite, alpha-alumina
- C04B 2235/3218: Aluminium (oxy)hydroxides, e.g. boehmite, gibbsite, alumina sol
- C04B 2235/322: Transition aluminas, e.g. delta or gamma aluminas
- C04B 2235/3272: Iron oxides or oxide forming salts thereof, e.g. hematite, magnetite
- C04B 2235/3281: Copper oxides, cuprates or oxide-forming salts thereof, e.g. CuO or Cu2O
- C04B 2235/3418: Silicon oxide, silicic acids or oxide forming salts thereof, e.g. silica sol, fused silica, silica fume, cristobalite, quartz or flint
- C04B 2235/3463: Alumino-silicates other than clay, e.g. mullite
- C04B 2235/3481: Alkaline earth metal alumino-silicates other than clay, e.g. cordierite, beryl, micas such as margarite, plagioclase feldspars such as anorthite, zeolites such as chabazite
- C04B 2235/349: Clays, e.g. bentonites, smectites such as montmorillonite, vermiculites or kaolines, e.g. illite, talc or sepiolite
- C04B 2235/407: Copper
- C04B 2235/522: Oxidic
- F01N 2330/30: Honeycomb supports characterised by their structural details
- Y02A 50/20: Air quality improvement or preservation, e.g. vehicle emission control or emission reduction by using catalytic converters
- Y02T 10/12: Improving ICE efficiencies
- 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)
- C04B: LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE {(roofing granules E04D7/005)}; CERAMICS (devitrified glass-ceramics C03C10/00); REFRACTORIES; TREATMENT OF NATURAL STONE
- F01N: GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL-COMBUSTION ENGINES (arrangements in connection with gas exhaust of propulsion units in vehicles B60K13/00; combustion-air intake silencers specially adapted for, or arranged on, internal-combustion engines F02M35/00; protecting against, or damping, noise in general G10K11/16)
- Y02A: TECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE
- Y02T: CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO TRANSPORTATION

## Abstract

An extruded, solid honeycomb body comprises a copper-promoted, small pore, crystalline molecular sieve catalyst for converting oxides of nitrogen in the presence of a reducing agent, wherein the crystalline molecular sieve contains a maximum ring size of eight tetrahedral atoms, which extruded, solid honeycomb body comprising: 20-50% by weight matrix component comprising diatomaceous earth, wherein 2-20 weight % of the extruded, solid honeycomb body is diatomaceous earth; 80-50% by weight of the small pore, crystalline molecular sieve ion-exchanged with copper; and 0-10% by weight of inorganic fibres.

## Claims

### Claim 1

An extruded, solid honeycomb body comprising a copper-promoted, small pore, crystalline molecular sieve catalyst for converting oxides of nitrogen in the presence of a reducing agent, wherein the crystalline molecular sieve contains a maximum ring size of eight tetrahedral atoms, which extruded, solid honeycomb body comprising:
20-50% by weight matrix component comprising diatomaceous earth, wherein 2-20 weight % of the extruded, solid honeycomb body is diatomaceous earth, and wherein the diatomaceous earth contains iron oxide;
80-50% by weight of the small pore, crystalline molecular sieve ion-exchanged with copper; and
0-10% by weight of inorganic fibres.

### Claim 2 (depends on 1)

The extruded, solid honeycomb body of claim 1, wherein a weight ratio of Fe:Cu in the extruded, solid honeycomb body is 1:5-1:20.

### Claim 3 (depends on 1)

The extruded, solid honeycomb body of claim 1, wherein a wall porosity of the extruded, solid honeycomb body is from 40-60%.

### Claim 4 (depends on 1)

The extruded, solid honeycomb body of claim 1, coated with a catalytic coating, wherein the catalytic coating is for converting NOx using a nitrogenous reductant.

### Claim 5

A method of making an extruded, solid honeycomb body comprising the steps of:
(a) forming a plastic mixture by mixing and/or kneading together a powdered diatomaceous earth matrix component; powdered additional matrix component; powdered small pore, crystalline molecular sieve, wherein the small pore, crystalline molecular sieve contains a maximum ring size of eight tetrahedral atoms; a copper component; optional inorganic fibres; and an acid or alkaline aqueous solution, wherein the copper component comprises copper which has been ion-exchanged in the small pore, crystalline molecular sieve prior to the mixing step and/or the copper component is added as an ion-exchange precursor to the mixture, wherein the powdered small pore, crystalline molecular sieve is added to the mixture as the H+ or NH4+ form thereof and the small pore, crystalline molecular sieve is ion-exchanged with the copper in situ, and wherein the plastic mixture is formed including an organic auxiliary;
(b) extruding the plastic mixture into a wet honeycomb body, drying the extruded honeycomb body and calcining it to form an extruded, solid honeycomb body; and
(c) selecting quantitative proportions of the starting materials such that the extruded, solid honeycomb body contains 20-50% by weight matrix component comprising diatomaceous earth, wherein 2-20 weight % of the extruded, solid honeycomb body is diatomaceous earth, and wherein the diatomaceous earth contains iron oxide; 80-50% by weight of the small pore, crystalline molecular sieve ion-exchanged with copper; and 0-10% by weight of inorganic fibres.

### Claim 6 (depends on 5)

The method of claim 5, wherein the additional matrix component in the extruded, solid honeycomb body comprises alumina, wherein the plastic mixture comprises boehmite as an alumina precursor and/or an alumina sol.

### Claim 7 (depends on 5)

The method of claim 5, wherein the plastic mixture comprises clay as an additional matrix component.

### Claim 8 (depends on 7)

The method of claim 7, wherein the clay is a combination of bentonite clay, kaolin clay and a fire clay.

### Claim 9 (depends on 8)

The method of claim 8, wherein the fire clay is in a majority by weight % relative to the total quantity of clay present.

### Claim 10 (depends on 5)

The method of claim 5, wherein the small pore, crystalline molecular sieve is ion-exchanged with the copper in situ, the ion-exchange precursor is copper acetate.

### Claim 11 (depends on 5)

The method of claim 5, wherein the organic auxiliary agent is at least one of acrylic fibres, a cellulose derivative, an organic plasticizer, a lubricant or a water-soluble resin.