# US 11,111,151 B2 · Layered silicate powder granules and method for producing the same

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

- Number: US 11,111,151 B2
- Document ID: US11111151B2
- Status: Granted
- Kind: B2
- Application number: 16/308,249
- Filed: 2017-09-04
- Published: 2019-08-29
- Granted: 2021-09-07
- Earliest claimed: 2016-09-13
- Assignees: National Institute for Materials Science
- Applicants: National Institute for Materials Science
- Inventors: Hiroshi Sakuma; Kenji Tamura
- Web page: https://patentgrep.com/patent/US11111151B2

## CPC

- C01B 33/325: {After-treatment, e.g. purification or stabilisation of solutions, granulation; Dissolution; Obtaining solid silicate, e.g. from a solution by spray-drying, flashing off water or adding a coagulant}
- C01B 33/405: {not containing aluminium}
- B01J 20/12: Naturally occurring clays or bleaching earth
- B01J 20/283: based on silica
- B01J 20/30: Processes for preparing, regenerating, or reactivating
- B01J 21/16: Clays or other mineral silicates
- B01J 37/0072: {Preparation of particles, e.g. dispersion of droplets in an oil bath}
- C01B 33/20: Silicates (persilicates C01B15/14 {; containing aluminium C01B33/26})
- C01B 33/42: Micas {; Interstratified clay-mica products (delaminated mica or vermiculite platelets obtained by a process involving cation-exchange C04B14/208)}
- C09D 1/02: alkali metal silicates
- C09D 5/031: {characterised by particle size or shape}
- C09D 17/007: {Metal oxide}
- C01P 2002/22: layered hydroxide-type, e.g. of the hydrotalcite-type
- C01P 2002/70: defined by measured X-ray, neutron or electron diffraction data
- C01P 2004/02: obtained by optical microscopy
- C01P 2004/03: obtained by SEM
- C01P 2004/24: Nanoplates, i.e. plate-like particles with a thickness from 1-100 nanometer
- C01P 2004/52: highly monodisperse size distribution
- C01P 2004/64: Nanometer sized, i.e. from 1-100 nanometer
- C01P 2004/90: Other morphology not specified above
- C01B: NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; {METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C}
- B01J: CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- C09D: COATING COMPOSITIONS, e.g. PAINTS, VARNISHES OR LACQUERS; FILLING PASTES; CHEMICAL PAINT OR INK REMOVERS; INKS; CORRECTING FLUIDS; WOODSTAINS; PASTES OR SOLIDS FOR COLOURING OR PRINTING; USE OF MATERIALS THEREFOR (cosmetics A61K; processes for applying liquids or other fluent materials to surfaces, in general, B05D; staining wood B27K5/02; glazes or vitreous enamels C03C; natural resins, French polish, drying-oils, driers, turpentine, per se, C09F; polishing compositions other than French polish, ski waxes C09G; adhesives or use of materials as adhesives C09J; materials for sealing or packing joints or covers C09K3/10; materials for stopping leaks C09K3/12; processes for the electrolytic or electrophoretic production of coatings C25D)
- C01P: INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS

## Abstract

The invention has for its object to use an evaporation-spray drying process thereby providing layered silicate powder granules, each one containing a flat particle having an opening or recess in its surface center. Each of the layered silicate powder granule contains a flat particle including a layered silicate formed by evaporation-spray drying and a rheology modifier for modifying the crystal edge face of the layered silicate and having an opening or recess in its surface center.

## Claims

### Claim 1

A layered silicate powder granule comprising flat particles, each particle comprising an evaporation-spray-dried layered silicate and a rheology modifier for modifying a crystal edge face of the layered silicate, and having an opening or recess in its surface center,
wherein the layered silicate is at least one selected from the group consisting of smectites, swelling synthetic micas, and vermiculites.

### Claim 2 (depends on 1)

A layered silicate granule as recited in claim 1, wherein the layered silicate has the following general formula:
(En+)a/n(M1cM2d)(Si4-eAle)O10(OHfF2-f)
where n is a natural number of 1 to 3; 0.1≤a≤0.8, 0≤c≤3, 0≤d≤2, 2≤c+d≤3, 0≤e<4, and 0≤f≤2; E is an interlayer n-valent cation and at least one atom selected from the group consisting of H, Li, Na, Mg, Ca, Zn, Sr, Fe, Ba, Ni, Cu, Co, Mn, Al, and Ga; and M1 being at least one metal selected from the group consisting of Mg, Fe, Mn, Ni, Zn, and Li, and M2 being at least one metal selected from the group consisting of Al, Fe, Mn, and Cr.

### Claim 3 (depends on 1)

The layered silicate granule as recited in claim 1, wherein the layered silicate has a 2:1 type structure.

### Claim 4 (depends on 1)

A layered silicate granule as recited in claim 1, wherein the smectites are selected from montmorillonite, beidellite, nontronite, saponite, hectorite and stevensite.

### Claim 5 (depends on 1)

A layered silicate granule as recited in claim 1, wherein the swelling synthetic micas are selected from Na-tetrasilisic mica or Na-taeniolite.

### Claim 6 (depends on 1)

A layered silicate granule as recited in claim 1, wherein the vermiculites are selected from dioctahedral type vermiculite or trioctahedral type vermiculite.

### Claim 7 (depends on 1)

A layered silicate granule as recited in claim 1, wherein the rheology modifier is an anionic compound.

### Claim 8 (depends on 1)

A layered silicate granule as recited in claim 1, wherein the rheology modifier contains an amount of 1 to 20 parts by mass per 100 parts by mass of the layered silicate.

### Claim 9 (depends on 1)

A layered silicate granule as recited in claim 1, wherein the flat particle has an outer diameter of greater than 500 nm and less than 50 μm as observed and measured under a microscope, and a specific surface area (St/Vt) of the flat particle that is defined by a surface area (St) to volume (Vt) ratio is 1.1 to 2.0 times as large as that of a sphere having the same volume.

### Claim 10 (depends on 9)

A layered silicate granule as recited in claim 9, wherein the layered silicate granule contains 60% or greater of the flat particles (counted as a number of particles) and 20% or less of spherical particles (counted as a number of particles), and the flat particle has a maximum particle diameter of 50 μm or less.

### Claim 11 (depends on 1)

The functional granule for chromatography, adsorbents, drug delivery, catalysts, biologically active agent protection, pigments, or coatings, to which the layered silicate granule as recited in claim 1 is applied.

### Claim 12 (depends on 1)

A method for producing a layered silicate granule according to claim 1, the method comprising:
spraying a suspension containing the layered silicate and the rheology modifier for modifying the crystal edge face of the layered silicate in an atmosphere in which a dispersion medium evaporates, and
evaporating and drying the dispersion medium.

### Claim 13 (depends on 12)

A method for producing a layered silicate granule as recited in claim 12, wherein droplets of the suspension containing the layered silicate and the rheology modifier for modifying the crystal edge face of the layered silicate are sprayed and blown onto a centrifugal disc, and a film of the suspension formed in a disc shape is scattered by fast rotation of the centrifugal disc, after which the dispersion medium is evaporated and dried.

### Claim 14 (depends on 12)

A method for producing a layered silicate granule as recited in claim 12, wherein the layered silicate has the following general formula:
(En+)a/n(M1cM2d)(Si4-eAle)O10(OHfF2-f)
where n is a natural number of 1 to 3; 0.1≤a≤0.8, 0≤c≤3, 0≤d≤2, 2≤c+d≤3, 0≤e<4, and 0≤f≤2; E is an interlayer n-valent cation and at least one atom selected from the group consisting of H, Li, Na, Mg, Ca, Zn, Sr, Fe, Ba, Ni, Cu, Co, Mn, Al, and Ga; and M1 being at least one metal selected from the group consisting of Mg, Fe, Mn, Ni, Zn, and Li, and M2 being at least one metal selected from the group consisting of Al, Fe, Mn, and Cr.

### Claim 15 (depends on 12)

A method for producing a layered silicate granule as recited in claim 12, wherein the layered silicate use is made of the layered silicate having a mean primary particle diameter of 10 nm to 100 nm as found by choosing particles at random, measuring one direction diameters of them along the crystal ab-axes under a microscope and taking an average.

### Claim 16 (depends on 12)

A method for producing a layered silicate granule as recited in claim 12, wherein the suspension containing the layered silicate and the rheology modifier for modifying the crystal edge face of the layered silicate has a solid matter concentration of 0.1 to 20% by mass.

### Claim 17 (depends on 12)

A method for producing a layered silicate granule as recited in claim 12, wherein the layered silicate powder granules are heated at a temperature of 350 to 800° C.