Process for the continuous preparation of phyllomineral synthetic particles

Patent metadata

Field	Value
Publication number	US-10221072-B2
Application number	US-201515304124-A
Country	US
Kind code	B2
Filing date	Apr 13, 2015
Priority date	Apr 14, 2014
Publication date	Mar 5, 2019
Grant date	Mar 5, 2019

Abstract

A process for preparing phyllomineral synthetic particles formed from constituent chemical elements in stoichiometric proportions including at least one chemical element selected from the group formed from silicon and germanium, and at least one chemical element selected from the group formed from divalent metals and trivalent metals, by a continuous solvothermal treatment at a pressure above 1 MPa and at a temperature between 100° C. and 600° C., by making the reaction medium circulate continuously in a solvothermal treatment zone of a continuous reactor (15) with a residence time of the reaction medium in the solvothermal treatment zone that is suitable for continuously obtaining, at the outlet of the solvothermal treatment zone, a suspension including the phyllomineral synthetic particles.

First claim

The invention claimed is:

1. A process for preparing phyllomineral synthetic particles formed from chemical elements, named constituent chemical elements, in predetermined proportions, named stoichiometric proportions, said constituent chemical elements comprising at least one chemical element selected from the group consisting of silicon and germanium, and at least one chemical element selected from the group consisting of divalent metals and trivalent metals, via a solvothermal treatment of a reaction medium comprising a liquid medium and containing said stoichiometric proportions of said constituent chemical elements of said phyllomineral synthetic particles, said phyllomineral synthetic particles belonging to the group of non-swelling phyllosilicates,
in which:
said solvothermal treatment is performed continuously at a pressure greater than 1 MPa and at a temperature of between 100° C. and 600° C.,
the reaction medium is continuously circulated in a solvothermal treatment zone of a continuous reactor with a residence time of the reaction medium in said solvothermal treatment zone that is suitable for continuously obtaining, at the outlet of said solvothermal treatment zone, a suspension comprising said phyllomineral synthetic particles.

2. The process according to claim 1 , wherein a constant-volume continuous reactor is used.

3. The process according to claim 1 , wherein the solvothermal treatment zone of the reactor comprises at least one pipe, named the reaction pipe, in which the reaction medium continuously circulates between at least one inlet suitable for allowing the continuous introduction of at least one starting composition and at least one outlet via which the suspension comprising said phyllomineral synthetic particles is continuously recovered.

4. The process according to claim 3 , wherein the temperature is controlled by controlling the temperature of the reaction pipe.

5. The process according to claim 1 , wherein said solvothermal treatment is performed at a pressure of between 2 MPa and 50 MPa.

6. The process according to claim 1 , wherein the duration of the continuous solvothermal treatment is adjusted by controlling the residence time of the reaction medium in the solvothermal treatment zone, in which said reaction medium is subjected to the temperature and pressure of the solvothermal treatment.

7. The process according to claim 1 , wherein the reaction medium is continuously circulated in the reactor so that said reaction medium has a residence time in the solvothermal treatment zone of less than 10 minutes.

8. The process according to claim 1 , wherein said reaction medium is introduced into the solvothermal treatment zone with a flow rate chosen to obtain the appropriate residence time.

9. The process according to claim 1 , wherein said solvothermal treatment is performed under temperature and pressure conditions such that said reaction medium is under supercritical conditions.

10. The process according to claim 1 , wherein the reaction medium is prepared continuously from at least one first starting composition comprising at least one compound, named mineral compound, chosen from silicates and/or germanates, solid solutions thereof and mixtures thereof, and of at least one second starting composition comprising at least one metal salt of at least one metal M selected from the group consisting of divalent metals and trivalent metals, said first and second compositions being placed in contact continuously upstream of at least one inlet of said solvothermal treatment zone.

11. The process according to claim 10 , wherein said first starting composition is introduced continuously into at least one first pipe portion and said second starting composition is introduced continuously into at least one second pipe portion, each of the first pipe portion and of the second pipe portion being connected together upstream of the solvothermal treatment zone to allow the continuous placing in contact of these two compositions.

12. The process according to claim 11 , wherein the first pipe portion and the second pipe portion join together upstream of at least one inlet of the solvothermal treatment zone, in a third pipe portion connecting together each of the first and second pipe portions and the inlet of the solvothermal treatment zone.

13. The process according to claim 1 , wherein, for the preparation of phyllosilicate synthetic particles belonging to the group consisting of lamellar silicates, lamellar germanates, lamellar germanosilicates and mixtures thereof, wherein a precursor silico/germano-metallic hydrogel is used as precursor gel, and said solvothermal treatment is performed in the form of a continuous hydrothermal treatment of this precursor silico/germano-metallic hydrogel.

14. The process according to claim 13 , wherein use is made, as precursor gel, of a precursor silico/germano-metallic hydrogel comprising:
4 silicon and/or germanium atoms according to the following chemical formula: 4 (Si x Ge 1-x ), x being a real number of the interval [0; 1],
3 atoms of at least one metal M, M denoting at least one divalent metal having the formula Mg y(1) Co y(2) Zn y(3) Cu y(4) Mn y(5) Fe y(6) Ni y(7) Cr y(8) in which each y(i) represents a real number of the interval [0; 1], and such that

∑

i
=
1

8

⁢

y
⁡

(
i
)

=
1

,

(10−ε) oxygen atoms ((10−ε) O), ε being a real number of the interval [0; 10],
(2+ε) hydroxyl groups ((2+ε) (OH)), ε being a real number of the interval [0; 10],
and said hydrothermal treatment is performed so as to obtain continuously a suspension comprising phyllosilicate particles having the chemical formula (II) below:
(Si x Ge 1-x ) 4 M 3 O 10 (OH) 2   (II)

in which:
Si denotes silicon,
Ge denotes germanium,
M denotes at least one divalent metal having the formula Mg y(1) Co y(2) Zn y(3) Cu y(4) Mn y(5) Fe y(6) Ni y(7) Cr y(8) ; each y(i) representing a real number of the interval [0; 1], and such that

∑

i
=
1

8

⁢

y
⁡

(
i
)

=
1

,

x is a real number of the interval [0; 1].

15. A process for preparing phyllomineral synthetic particles formed from chemical elements, named constituent chemical elements, in predetermined proportions, named stoichiometric proportions, said constituent chemical elements comprising at least one chemical element selected from the group consisting of silicon and germanium, and at l

Assignees

• Centre Nat Rech Scient
• Univ Toulouse 3 Paul Sabatier

Inventors

• Aymonier Cyril
• Slostowski Cedric
• Dumas Angela
• Micoud Pierre
• Le Roux Christophe
• Martin Francois

Classifications

• C01B33/22 Primary

  Magnesium silicates · CPC title

• C01B33/40

  Clays · CPC title

• C01B33/38 Primary

  Layered base-exchange silicates, e.g. clays, micas or alkali metal silicates of kenyaite or magadiite type {(activation of naturally occurring clays B01J20/12; pillared layered base-exchange silicates B01J29/049)} · CPC title

• C01B33/42

  Micas {; Interstratified clay-mica products (delaminated mica or vermiculite platelets obtained by a process involving cation-exchange C04B14/208)} · CPC title

• B01J2208/00017

  Controlling the temperature · CPC title