IP Library Granted Patent US 10,130,932
Granted Patent B2
US 10,130,932 · App. 14/769,846 · Granted Nov 20, 2018

Organic-inorganic hybrid material of use for extracting uranium (VI) from aqueous media containing phosphoric acid, processes for preparing same and uses thereof

Inventors: Sabah El Mourabit (Sorgues, FR); Frédéric Goettmann (Les Angles, FR); Raphaël Turgis (Sabran, FR); Agnès Grandjean (Saint Marcel de Careiret, FR); Guilhem Arrachart (Saint-Laurent-des-Arbres, FR); Stéphane Pellet-Rostaing (Villeurbanne, FR)
Assignees: COMMISSARIAT A L'ENERGIE ATOMIQUE ET AUX ÉNERGIES ALTERNATIVES; CENTRE NATIONAL DE LA RECHERCHE SCIENTIFIQUE; UNIVERSITE DE MONTPELLIER
B01J20/3251B01J20/28083B01J20/28085B01J20/3204B01J20/3219B01J20/3259B01J45/00C22B60/0269C22B60/0273C22B60/0282
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Quick Facts
Patent No.
US 10,130,932
App. No.
14/769,846
Granted
Nov 20, 2018
Kind
B2
Abstract

The invention relates to an organic-inorganic hybrid material which comprises an inorganic solid support on which are grafted organic molecules of the general formula (I) hereafter: and relates to methods allowing preparation of this hybrid material as well as to the uses of the hybrid material for extracting uranium(VI) from an aqueous medium comprising phosphoric acid.

Claims (42)

1. An organic-inorganic hybrid material, which comprises an inorganic solid support on which is covalently grafted a plurality of organic molecules of formula (I):

wherein:

x, y and z are equal to 0 or 1, with the proviso that at least one of x, y and z is equal to 1;

m is an integer ranging from 1 to 6;

v and w are equal to 0 or 1, with the proviso that v is equal to 1 when w is equal to 0 and v is equal to 0 when w is equal to 1;

if x is equal to 0, R 1 represents a hydrogen atom or a linear or branched, saturated or unsaturated hydrocarbon group comprising from 1 to 12 carbon atoms, and, if x is equal to 1, R 1 represents a group bound to the inorganic solid support through at least one covalent bond represented by the dotted line;

if y is equal to 0, R 2 represents a hydrogen atom or a linear or branched, saturated or unsaturated hydrocarbon group comprising from 1 to 12 carbon atoms, and, if y is equal to 1, R 2 represents a group bound to the inorganic solid support through at least one covalent bond represented by the dotted line;

if z is equal to 0, R 3 represents a hydrogen atom or a linear or branched, saturated or unsaturated hydrocarbon group comprising from 1 to 12 carbon atoms, and, if z is equal to 1, R 3 represents a group bound to the inorganic solid support through at least one covalent bond represented by the dotted line;

R 4 and R 5 represent, independently of each other, a hydrogen atom, a linear or branched, saturated or unsaturated hydrocarbon group comprising from 2 to 8 carbon atoms, or a monocyclic aromatic group.

2. The organic-inorganic hybrid material of claim 1 , wherein the inorganic solid support comprises a metal oxide, a mixed metal oxide, a mixture of metal oxides, or carbon.

3. The organic-inorganic hybrid material of claim 1 , wherein the inorganic solid support is a porous material.

4. The organic-inorganic hybrid material of claim 3 , wherein the porous material is a mesoporous or macroporous material.

5. The organic-inorganic hybrid material of claim 4 , wherein the porous material is a mesoporous silica, a mesoporous titanium oxide, a mesoporous zirconia or a mesoporous carbon.

6. The organic-inorganic hybrid material of claim 5 , wherein the inorganic solid support is a SBA mesoporous silica or a CMK mesoporous carbon.

7. The organic-inorganic hybrid material of claim 1 , wherein R 3 represents —(CH 2 ) q —X 1 — wherein q is an integer ranging from 0 to 12, and X 1 represents a group selected from the group consisting of:

and —CH═CH—.

8. The organic-inorganic hybrid material of claim 1 , wherein at least one of R 1 and R 2 represents a group of formula (a), (b), (c), (d), (e), (f) or (g):

—(CH 2 ) p —C(O)—NH—(CH 2 ) q —X 2 —  (a)

—(CH 2 ) p —NH—C(O)—(CH 2 ) q —X 2 —  (b)

—(CH 2 ) p —C(O)—O—(CH 2 ) q —X 2 —  (c)

—(CH 2 ) p —O—C(O)—(CH 2 ) q —X 2 —  (d)

—(CH 2 ) p —O—(CH 2 ) q —X 2 —  (e)

—(CH 2 ) p -triazole-(CH 2 ) q —X 2 —  (f)

—(CH 2 ) q —X 2 —  (g)

wherein p is an integer ranging from 1 to 6, q is an integer ranging from 0 to 12, and X 2 represents a group selected from the group consisting of:

and —CH═CH—.

9. The organic-inorganic hybrid material of claim 8 , wherein R 3 represents —(CH 2 ) q —X 1 — wherein q is an integer ranging from 0 to 12 and X 1 is identical with X 2 .

10. The organic-inorganic hybrid material of claim 1 , wherein the organic molecules have the formula (Ia):

11. The organic-inorganic hybrid material of claim 10 , wherein x and y are 0, R 1 and R 2 represent, independently of each other, a linear or branched alkyl group comprising from 1 to 12 carbon atoms; z is 1 and R 3 represents a group bound to the inorganic solid support through at least one covalent bond, and R 4 and R 5 represent, independently of each other, a hydrogen atom or a linear or branched alkyl group comprising from 2 to 8 carbon atoms.

12. The organic-inorganic hybrid material of claim 11 , wherein R 1 and R 2 are identical with each other and represent a branched alkyl group comprising from 6 to 12 carbon atoms.

13. The organic-inorganic hybrid material of claim 11 , wherein R 4 and R 5 represent, independently of each other, a hydrogen atom or a linear or branched alkyl group comprising from 2 to 4 carbon atoms.

14. The organic-inorganic hybrid material of claim 10 , wherein the inorganic solid support is based on a metal oxide, a mixed metal oxide or on a mixture of metal oxides and R 3 represents:

wherein q is 1 to 5.

15. The organic-inorganic hybrid material of claim 10 , wherein the inorganic solid support is based on carbon and R 3 represents:

wherein q is 1 to 5.

16. A method for extracting uranium(VI) from an aqueous medium comprising phosphoric acid comprising contacting the aqueous medium with the organic-inorganic hybrid material of claim 1 and then separating the aqueous medium and the organic-inorganic hybrid material.

17. The method of claim 16 , wherein the aqueous medium comprises from 0.012 mol/L to 9 mol/L of phosphoric acid.

18. The method of claim 17 , wherein the aqueous medium results from the attack of a phosphate ore with sulfuric acid.

19. A method for recovering uranium(VI) from an aqueous medium comprising phosphoric acid, comprising:

extraction of uranium(VI) from the aqueous medium, the extraction comprising contacting the aqueous medium with the organic-inorganic hybrid material of claim 1 , and then separating the aqueous medium and the organic-inorganic hybrid material; and

stripping of uranium(VI) from the organic-inorganic hybrid material obtained at the end of the extraction, the stripping comprising contacting the organic-inorganic hybrid material with a basic aqueous solution, and then separating the organic-inorganic hybrid material and the basic aqueous solution.

20. The method of claim 19 , wherein the aqueous medium results from the attack of a phosphate ore with sulfuric acid.

Assignments (3)
CORRECTIVE ASSIGNMENT TO CORRECT THE SPELLING OF MONTEPELLIER TO MONTPELLIER PREVIOUSLY RECORDED ON REEL 046553 FRAME 0774. ASSIGNOR(S) HEREBY CONFIRMS THE MERGER AND CHANGE OF NAME. Recorded Aug 6, 2018
From: UNIVERSITÉ DE MONTPELLIER I; UNIVERSITÉ MONTPELLIER 2 SCIENCES ET TECHNIQUES
To: UNIVERSITÉ DE MONTPELLIER
Reel/Frame 046772/0632 →
MERGER AND CHANGE OF NAME Recorded May 7, 2018
From: UNIVERSITÉ DE MONTEPELLIER I; UNIVERSITE MONTPELLIER 2 SCIENCES ET TECHNIQUES; UNIVERSITÉ DE MONTEPELLIER
To: UNIVERSITÉ DE MONTEPELLIER
Reel/Frame 046553/0774 →
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Aug 27, 2015
From: EL MOURABIT, SABAH; GOETTMANN, FRÉDÉRIC; TURGIS, RAPHAËL; GRANDJEAN, AGNÈS; ARRACHART, GUILHEM; PELLET-ROSTAING, STÉPHANE
To: COMMISSARIAT À L'ÉNERGIE ATOMIQUE ET AUX ÉNERGIES ALTERNATIVES; CENTRE NATIONAL DE LA RECHERCHE SCIENTIFIQUE; UNIVERSITE DE MONTPELLIER 2, SCIENCES ET TECHNIQUES
Reel/Frame 036439/0265 →
Priority Claims (1)
FR 13 51639 · Feb 25, 2013 · national
Continuity (1)
Related Publication 20160016150A1 · Jan 21, 2016