# US 11,078,084 B2 · Aerogel precursor and aerogel prepared using the same

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

- Number: US 11,078,084 B2
- Document ID: US11078084B2
- Status: Granted
- Kind: B2
- Application number: 15/736,725
- Filed: 2016-12-15
- Published: 2018-06-14
- Granted: 2021-08-03
- Earliest claimed: 2016-03-16
- Assignees: LG Chem, Ltd.
- Applicants: LG Chem, Ltd.
- Inventors: Hee Jung Choi; Kyoung Shil Oh; Yeong Rae Chang; Je Kyun Lee
- Web page: https://patentgrep.com/patent/US11078084B2

## CPC

- C01B 33/1585: {Dehydration into aerogels}
- B01J 13/0091: {Preparation of aerogels, e.g. xerogels}
- C01B 33/158: Purification; Drying; Dehydrating
- C07F 7/08: Compounds having one or more C—Si linkages
- C07F 7/087: {Compounds of unknown structure containing a Si-O-Si sequence}
- C07F 7/0874: {Reactions involving a bond of the Si-O-Si linkage}
- C07F 7/28: Titanium compounds
- C08G 77/06: Preparatory processes
- C08G 77/18: to alkoxy or aryloxy groups
- C08G 77/38: Polysiloxanes modified by chemical after-treatment
- C09K 3/30: for aerosols (aerosol containers B65D83/14)
- C01P 2006/11: Powder tap density
- C01P 2006/12: Surface area
- C01P 2006/14: Pore volume
- C01P 2006/16: Pore diameter
- C01P 2006/37: Stability against thermal decomposition
- 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
- C07F: ACYCLIC, CARBOCYCLIC OR HETEROCYCLIC COMPOUNDS CONTAINING ELEMENTS OTHER THAN CARBON, HYDROGEN, HALOGEN, OXYGEN, NITROGEN, SULFUR, SELENIUM OR TELLURIUM (metal-containing porphyrins C07D487/22)
- C08G: MACROMOLECULAR COMPOUNDS OBTAINED OTHERWISE THAN BY REACTIONS ONLY INVOLVING UNSATURATED CARBON-TO-CARBON BONDS
- C09K: MATERIALS FOR MISCELLANEOUS APPLICATIONS, NOT PROVIDED FOR ELSEWHERE
- C01P: INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS

## Abstract

The present disclosure provides an aerogel precursor including an alkoxydisiloxane-based prepolymer and having a functional group derived from a hydrophobic sol-gel forming agent of the following Chemical Formula 1 on a surface thereof, and therefore, capable of enhancing high temperature thermal stability of an aerogel providing hydrophobic pores having uniform pore size distribution when preparing an aerogel, and an aerogel prepared using the same: (in Chemical Formula 1, M, R, R1 to R4 are the same as defined in the specification.)

## Claims

### Claim 1

An aerogel precursor comprising an alkoxydisiloxane-based prepolymer, and having a functional group derived from a hydrophobic sol-gel forming agent of the following Chemical Formula 2 on a surface thereof:
wherein:
M11 is any one selected from the group consisting of group 4 elements and group 14 elements;
R11 is a halogen group;
R12 and R13 each independently is selected from the group consisting of an alkyl group having 1 to 20 carbon atoms, an alkenyl group having 2 to 20 carbon atoms, an alkynyl group having 2 to 20 carbon atoms, a cycloalkyl group having 3 to 20 carbon atoms, an aryl group having 6 to 20 carbon atoms, an arylalkyl group having 7 to 20 carbon atoms and an alkylaryl group having 7 to 20 carbon atoms; and
R14 is selected from the group consisting of an alkyl group having 2 to 20 carbon atoms, an alkenyl group having 2 to 20 carbon atoms, an alkynyl group having 2 to 20 carbon atoms, a cycloalkyl group having 3 to 20 carbon atoms, an aryl group having 6 to 20 carbon atoms, an arylalkyl group having 7 to 20 carbon atoms and an alkylaryl group having 7 to 20 carbon atoms,
wherein the alkoxydisiloxane-based prepolymer has a degree of hydrolysis of 50% to 85%, and
the alkoxydisiloxane-based prepolymer includes an alkoxydisiloxane-derived repeating unit having a molecular weight of 60 Da to 140 Da and a molecular weight distribution with an m/z (ratio of mass to charge) value of 620 to 1,800 when analyzing the mass by MALDI-TOF.

### Claim 2 (depends on 1)

The aerogel precursor of claim 1, wherein M is selected from the group consisting of Ti, Hf, Si and Zr.

### Claim 3 (depends on 1)

The aerogel precursor of claim 1, wherein:
M11 is Si;
R11 is a chloro group, a bromo group or an iodo group; and
R12 and R13 each independently is selected from the group consisting of an alkyl group having 1 to 12 carbon atoms, an aryl group having 6 to 12 carbon atoms, an arylalkyl group having 7 to 13 carbon atoms and an alkylaryl group having 7 to 13 carbon atoms; and
R14 is selected from the group consisting of an alkyl group having 2 to 12 carbon atoms, an aryl group having 6 to 12 carbon atoms, an arylalkyl group having 7 to 13 carbon atoms and an alkylaryl group having 7 to 13 carbon atoms.

### Claim 4 (depends on 3)

The aerogel precursor of claim 3, wherein, in Chemical Formula 2:
R11 is a chloro group or a bromo group;
R12 and R13 each independently is selected from the group consisting of an alkyl group having 1 to 12 carbon atoms, an aryl group having 6 to 12 carbon atoms, an arylalkyl group having 7 to 13 carbon atoms and an alkylaryl group having 7 to 13 carbon atoms; and
R14 is selected from the group consisting of an alkyl group having 2 to 12 carbon atoms, an aryl group having 6 to 12 carbon atoms, an arylalkyl group having 7 to 13 carbon atoms and an alkylaryl group having 7 to 13 carbon atoms.

### Claim 5 (depends on 1)

The aerogel precursor of claim 1, wherein the hydrophobic sol-gel forming agent includes any one or a mixture of two or more selected from the group consisting of chlorotriethylsilane, bromotriethylsilane and chloro(methyl)diphenylsilane.

### Claim 6 (depends on 1)

The aerogel precursor of claim 1, wherein the functional group derived from the hydrophobic sol-gel forming agent is included in 0.1 mol % to 60 mol % with respect to a total mole of the alkoxy group in the alkoxydisiloxane-based prepolymer.

### Claim 7 (depends on 1)

The aerogel precursor of claim 1, which has a carbon content of 20% by weight or greater with respect to a total weight of the aerogel precursor.

### Claim 8 (depends on 1)

A method for preparing the aerogel precursor of claim 1, the method comprising:
preparing the alkoxydisiloxane-based prepolymer having a molecular weight distribution with an m/z (ratio of mass to charge) value of 620 to 3,000 when analyzing the mass by MALDI-TOF by hydrolyzing and polycondensation reacting an alkoxysilane-based compound; and
reacting the alkoxydisiloxane-based prepolymer with the hydrophobic sol-gel forming agent of Chemical Formula 2:
wherein:
M11 is any one selected from the group consisting of group 4 elements and group 14 elements;
R11 is a halogen group;
R12 and R13 each independently is selected from the group consisting of an alkyl group having 1 to 20 carbon atoms, an alkenyl group having 2 to 20 carbon atoms, an alkynyl group having 2 to 20 carbon atoms, a cycloalkyl group having 3 to 20 carbon atoms, an aryl group having 6 to 20 carbon atoms, an arylalkyl group having 7 to 20 carbon atoms and an alkylaryl group having 7 to 20 carbon atoms; and
R14 is selected from the group consisting of an alkyl group having 2 to 20 carbon atoms, an alkenyl group having 2 to 20 carbon atoms, an alkynyl group having 2 to 20 carbon atoms, a cycloalkyl group having 3 to 20 carbon atoms, an aryl group having 6 to 20 carbon atoms, an arylalkyl group having 7 to 20 carbon atoms and an alkylaryl group having 7 to 20 carbon atoms.

### Claim 9 (depends on 8)

The method for preparing the aerogel precursor of claim 8, wherein the alkoxysilane-based compound includes tetraethoxysilane.

### Claim 10 (depends on 1)

The aerogel precursor of claim 1, wherein M11 is Si.

### Claim 11

An aerogel precursor comprising an alkoxydisiloxane-based prepolymer, and having a functional group derived from a hydrophobic sol-gel forming agent of the following Chemical Formula 3 on a surface thereof, wherein the hydrophobic sol-gel forming agent includes a compound of the following Chemical Formula 3:
wherein, in Chemical Formula 3,
M21 is Ti or Zr; and
R21 to R24 are each independently a hydrophobic functional group selected from the group consisting of an alkyl group having 1 to 10 carbon atoms, a cycloalkyl group having 3 to 12 carbon atoms, an aryl group having 6 to 12 carbon atoms, an arylalkyl group having 7 to 13 carbon atoms, an alkylaryl group having 7 to 13 carbon atoms; or a functional group reactive with the alkoxydisiloxane-based prepolymer that is a halogen group or an alkoxy group having 1 to 10 carbon atoms, however, R21 to R24 are not a hydrophobic functional group or a functional group reactive with the alkoxydisiloxane-based prepolymer at the same time,
wherein the alkoxydisiloxane-based prepolymer has a degree of hydrolysis of 50% to 85%, and
the alkoxydisiloxane-based prepolymer includes an alkoxydisiloxane-derived repeating unit having a molecular weight of 60 Da to 140 Da and a molecular weight distribution with an m/z (ratio of mass to charge) value of 620 to 1,800 when analyzing the mass by MALDI-TOF.

### Claim 12 (depends on 11)

The aerogel precursor of claim 11, wherein, in Chemical Formula 3, M12 is Ti.

### Claim 13

An aerogel precursor comprising an alkoxydisiloxane-based prepolymer, and having a functional group derived from a hydrophobic sol-gel forming agent of the following Chemical Formula 2 on a surface thereof:
wherein:
M11 is any one selected from the group consisting of group 4 elements and group 14 elements;
R11 is a halogen group;
R12 and R13 each independently is selected from the group consisting of an alkyl group having 1 to 20 carbon atoms, an alkenyl group having 2 to 20 carbon atoms, an alkynyl group having 2 to 20 carbon atoms, a cycloalkyl group having 3 to 20 carbon atoms, an aryl group having 6 to 20 carbon atoms, an arylalkyl group having 7 to 20 carbon atoms and an alkylaryl group having 7 to 20 carbon atoms; and
R14 is selected from the group consisting of an alkyl group having 2 to 20 carbon atoms, an alkenyl group having 2 to 20 carbon atoms, an alkynyl group having 2 to 20 carbon atoms, a cycloalkyl group having 3 to 20 carbon atoms, an aryl group having 6 to 20 carbon atoms, an arylalkyl group having 7 to 20 carbon atoms and an alkylaryl group having 7 to 20 carbon atoms,
wherein the alkoxydisiloxane-based prepolymer has a degree of hydrolysis of 50% to 85%, and
the alkoxydisiloxane-based prepolymer includes an alkoxydisiloxane-derived repeating unit having a molecular weight of 60 Da to 140 Da and
the alkoxydisiloxane-based prepolymer has a molecular weight distribution with an m/z (ratio of mass to charge) value of 650 to 3,000 when analyzing the mass by MALDI-TOF.

### Claim 14 (depends on 13)

The aerogel precursor of claim 13, wherein M11 is Si.