# US 10,373,748 B2 · Temperature-stable soft-magnetic powder

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- Number: US 10,373,748 B2
- Document ID: US10373748B2
- Status: Granted
- Kind: B2
- Application number: 15/034,039
- Filed: 2014-11-04
- Published: 2016-09-22
- Granted: 2019-08-06
- Earliest claimed: 2013-11-06
- Assignees: BASF SE
- Applicants: BASF SE
- Inventors: Sandro Pagano; Jae Hyung Hwang; Ralf Liebscher; Frank Prechtl; Oliver Koch; Otto Watzenberger; Volker Klock
- Web page: https://patentgrep.com/patent/US10373748B2

## CPC

- B22F 1/00: Metallic powder; Treatment of metallic powder, e.g. to facilitate working or to improve properties
- B22F 1/102: Metallic powder coated with organic material
- B22F 1/16: Metallic particles coated with a non-metal (coated with lubricating or binding agents or with organic material B22F1/10)
- C23C 30/00: Coating with metallic material characterised only by the composition of the metallic material, i.e. not characterised by the coating process (C23C26/00, C23C28/00 take precedence)
- H01F 1/20: in the form of particles, e.g. powder (H01F1/147 takes precedence)
- H01F 1/26: by macromolecular organic substances
- H01F 1/36: in the form of particles {(H01F1/346, H01F1/348 and H01F1/38 take precedence)}
- H01F 3/08: made from powder (powder coatings on sheets H01F3/02; on strips or ribbons H01F3/04; on wires H01F3/06)
- H01F 41/0246: {Manufacturing of magnetic circuits by moulding or by pressing powder (magnetic cores made by moulding or by pressing powder H01F27/255; soft magnetic particles H01F1/20, H01F1/36)}
- B22F: WORKING METALLIC POWDER; MANUFACTURE OF ARTICLES FROM METALLIC POWDER; MAKING METALLIC POWDER (making alloys by powder metallurgy C22C); APPARATUS OR DEVICES SPECIALLY ADAPTED FOR METALLIC POWDER
- C23C: COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; SURFACE TREATMENT OF METALLIC MATERIAL BY DIFFUSION INTO THE SURFACE, BY CHEMICAL CONVERSION OR SUBSTITUTION; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL (making metal-coated products by extrusion B21C23/22; covering with metal by connecting pre-existing layers to articles, see the relevant places, e.g. B21D39/00, B23K; metallising of glass C03C; metallising mortars, concrete, artificial stone, ceramics or natural stone C04B41/00; enamelling of, or applying a vitreous layer to, metals C23D; treating metal surfaces or coating of metals by electrolysis or electrophoresis C25D; single-crystal film growth C30B; by metallising textiles D06M11/83; decorating textiles by locally metallising D06Q1/04)
- H01F: MAGNETS; INDUCTANCES; TRANSFORMERS; SELECTION OF MATERIALS FOR THEIR MAGNETIC PROPERTIES

## Abstract

The invention relates to a soft-magnetic powder coated with a silicon based coating, wherein the silicon based coating comprises at least one of the following fluorine containing compositions: a) a fluorine containing composition of formula (I) Si1-0,25aM1aO2-0,5bFb (I) wherein a is in the range of 0.015 to 0.52, b is in the range of 0.015 to 0.52, M1 is H, K, Rb, Cs or NR14, wherein each R1 is independently selected from the group consisting of H, C1-6 alkyl, phenyl and benzyl; or b) a fluorine containing composition of formula (II) Si1-0,75cM2cO2-0,5dFd (II) wherein c is in the range of 0.005 to 0.17, d is in the range of 0.015 to 0.52, M2 is B or Al; or c) a fluorine containing composition of formula (III) Si1-1,25ePeO2-0,5fFf (III) wherein e is in the range of 0.003 to 0.10, f is in the range of 0.015 to 0.52. The invention further relates to a process of coating the soft-magnetic powder, the use of such soft-magnetic powder and an electronic component including such soft-magnetic powder.

## Claims

### Claim 1

A soft-magnetic powder coated with a silicon based coating, wherein the silicon based coating comprises at least one of the following fluorine containing compositions:
a) a fluorine containing composition of formula (I)
Si1-0,25aM1aO2-0,5bFb (I)
wherein
a is in the range of 0.015 to 0.52,
b is in the range of 0.015 to 0.52,
M1 is H, K, Rb, Cs or NR14, wherein each R1 is independently selected from the group
consisting of H, C1-6 alkyl, phenyl and benzyl;
b) a fluorine containing composition of formula (II)
Si1-0,75cM2cO2-0,5dFd (II)
wherein
c is in the range of 0.005 to 0.17,
d is in the range of 0.015 to 0.52,
M2 is B or Al;
or
c) a fluorine containing composition of formula (III)
Si1-1,25ePeO2-0,5fFf (III)
wherein
e is in the range of 0.003 to 0.10, and
f is in the range of 0.015 to 0.52.

### Claim 2 (depends on 1)

The soft-magnetic powder of claim 1, comprising at least one fluorine containing composition of formula (I), wherein M1 is H, Cs or NH4 and at least one fluorine containing composition of formula (II), wherein M2 is B.

### Claim 3 (depends on 1)

The soft-magnetic powder of claim 1, wherein silicon based coating comprises between 0.1 to 5 wt.-% of the at least one fluorine containing composition of formula (I), (II) or (III).

### Claim 4 (depends on 1)

The soft-magnetic powder of claim 1, wherein the fluorine component of the fluorine containing composition is embedded within a SiO2-matrix and/or bonded to a surface of a SiO2-coating.

### Claim 5 (depends on 1)

The soft-magnetic powder of claim 1, wherein the silicon based coating has an average thickness of 2 to 100 nm.

### Claim 6

A process for coating the soft-magnetic powder, the coating comprising at least one of the following fluorine containing compositions:
a) a fluorine containing composition of formula (I)
Si1-0,25aM1aO2-0,5bFb (I)
wherein
a is in the range of 0.015 to 0.52,
b is in the range of 0.015 to 0.52,
M1 is 1H, K, Rb, Cs or NR14, wherein each R1 is independently selected from the group consisting of H, C1-6 alkyl, phenyl and benzyl;
b) a fluorine containing composition of formula (II)
Si1-0,75cM2cO2-0,5dFd (II)
wherein
c is in the range of 0.005 to 0.17,
d is in the range of 0.015 to 0.52,
M2 is B or Al;
or
c) a fluorine containing composition of formula (III)
Si1-1,25ePeO2-0,5fFf (III)
wherein
e is in the range of 0.003 to 0.10, and
f is in the range of 0.015 to 0.52
wherein the soft-magnetic powder is mixed with a silicon based solution containing a soluble fluorination agent (F).

### Claim 7 (depends on 6)

The process of claim 6, wherein the soft-magnetic powder is mixed with a silicon based solution and soluble fluorination agent (F) is added after at least partial treatment of the soft-magnetic powder with the silicon based solution.

### Claim 8 (depends on 6)

The process of claim 6, wherein the at least one soluble fluorination agent (F) is
(A) a salt of formula (IVa) or (IVb)
M1F (IVa)
M2F3 (IVb)
wherein
M1 is defined as in formula (I),
M2 is defined as in formula (II);
(B) a compound of formula (V)
(M3)2(SiF6) (V)
wherein
M3 is H, Na, K, Rb, Cs or NR14, wherein R1 is defined as in formula (I);
(C) a compound of formula (VI)
M3PF6 (VI);
wherein
M3 is defined as in formula (V);
or
(D) a Lewis acid-Lewis base adduct, wherein the Lewis acid is M2F3
with
M2 is defined as in formula (II).

### Claim 9 (depends on 8)

The process of claim 8, wherein the at least one Lewis acid-Lewis base adduct is selected from the group consisting of
(D1) an adduct of formula (VIIa)
L1•sM2F3 (VIIa)
wherein
M2 is defined as in formula (II);
L1 is R2—O—R3 or NR4R5R6;
s is a number in the range of 0.5 to 1.0;
R2, R3 are independently from each other selected from the group consisting of H; C1-6 alkyl, optionally substituted with halogen or hydroxy; C3-8 cycloalkyl, optionally substituted with halogen, hydroxy, C1-6 alkyl, C1-6 haloalkyl, C1-6 hydroxyalkyl, C2-6 alkenyl, C1-6 alkoxy or C2-6 alkenoxy; phenyl, optionally substituted with halogen, C1-6 alkyl, C1-6 haloalkyl, C1-6 hydroxyalkyl, C2-6 alkenyl, C1-6 alkoxy or C2-6 alkenoxy; and benzyl, optionally substituted with halogen, C1-6 alkyl, C1-6 haloalkyl, C1-6 hydroxyalkyl, C2-6 alkenyl, C1-6 alkoxy or C2-6 alkenoxy;
or R2, R3 form, together with the oxygen atom they are bonded to, a 3-8-membered ring;
R4, R5, R6 are independently from each other selected from the group consisting of H; C1-6 alkyl, optionally substituted with halogen or hydroxyl; phenyl, optionally substituted with halogen, C1-6 alkyl, C1-6 haloalkyl, C1-6 hydroxyalkyl, C2-6 alkenyl, C1-6 alkoxy or C2-6 alkenoxy; and benzyl, optionally substituted with halogen, C1-6 alkyl, C1-6 haloalkyl, C1-6 hydroxyalkyl, C2-6 alkenyl, C1-6 alkoxy or C2-6 alkenoxy;
or two of R4, R5, R6 form, together with the nitrogen atom they are bonded to, a 3-8-membered ring;
(D2) an adduct of formula (VIIb)
wherein
each M2 is independently as defined in formula (II);
t is a number in the range of 0.8 to 2;
G is a single bond or a linking group selected from the group consisting of C1-6 alkyl, optionally substituted with halogen, hydroxy, C1-6 alkoxy or C2-6 alkenoxy; C2-6 alkenyl, optionally substituted with halogen, hydroxy, C2-6 alkenyl, C1-6 alkoxy or C2-6 alkenoxy; C3-8 cycloalkyl, optionally substituted with halogen, hydroxy, C1-6 alkyl, C1-6 haloalkyl, C1-6 hydroxyalkyl, C2-6 alkenyl, C1-6 alkoxy or C2-6 alkenoxy; C4-8 cycloalkenyl, optionally substituted with halogen, hydroxy, C1-6 alkyl, C1-6 haloalkyl, C1-6 hydroxyalkyl, C2-6 alkenyl, C1-6 alkoxy or C2-6 alkenoxy; and C6-14 aryl, optionally substituted with halogen, hydroxy, C1-6 alkyl, C1-6 haloalkyl, C1-6 hydroxyalkyl, C2-6 alkenyl, C1-6 alkoxy or C2-6 alkenoxy; m and n are independently from each other 0, 1, 2, 3, or 4, under the proviso that m+n≠0, when G is a single bond;
each L2 is independently selected from the group consisting of NR7R8 and OR9, wherein
R7, R8 are independently from each other selected from the group consisting of H, C1-6 alkyl, optionally substituted with halogen, hydroxy, C2-6 alkenyl, C1-6 alkoxy or C2-6 alkenoxy; phenyl, optionally substituted with halogen, hydroxy, C1-6 alkyl, C1-6 haloalkyl, C1-6 hydroxyalkyl, C2-6 alkenyl, C1-6 alkoxy or C2-6 alkenoxy; and benzyl, optionally substituted with halogen, hydroxy, C1-6 alkyl, C1-6 haloalkyl, C4-6 hydroxyalkyl, C2-6 alkenyl, C1-6 alkoxy or C2-6 alkenoxy;
or R7, R8 form, together with the nitrogen atom they are bonded to, a 3-8-membered ring;
R9 is selected from the group consisting of H; C1-6 alkyl; phenyl, optionally substituted with halogen, hydroxy, C1-6 alkyl, C1-6 haloalkyl, C1-6 hydroxyalkyl, C2-6 alkenyl, C1-6 alkoxy or C2-6 alkenoxy; and benzyl, optionally substituted with halogen, hydroxy, C1-6 alkyl, C1-6 haloalkyl, C1-6 hydroxyalkyl, C2-6 alkenyl, C1-6 alkoxy or C2-6 alkenoxy;
and
(D3) an adduct of formula (VIIc)
wherein
each M2 is independently as defined in formula (II);
each L2 is independently as defined in formula (VIIb);
u is a number in the range of 0.8 to 3.0;
G1, G2 are independently from each other a single bond or a linking group selected from the group consisting of C1-6 alkyl, optionally substituted with halogen, hydroxy, C2-6 alkenyl, C1-6 alkoxy or C1-6 alkenoxy; C2-6 alkenyl, optionally substituted with halogen, hydroxy, C1-6 alkyl, C1-6 haloalkyl, C1-6 hydroxyalkyl, C1-6 alkoxy or C2-6 alkenoxy; C3-8 cycloalkyl, optionally substituted with halogen, hydroxy, C1-6 alkyl, C1-6 haloalkyl, C1-6 hydroxyalkyl, C2-6 alkenyl, C1-6 alkoxy or C2-6 alkenoxy; C4-8 cycloalkenyl, optionally substituted with halogen, hydroxy, C1-6 alkyl, C1-6 haloalkyl, C1-6 hydroxyalkyl, C2-6 alkenyl, C1-6 alkoxy or C2-6 alkenoxy; and C6-14 aryl, optionally substituted with halogen, hydroxy, C1-6 alkyl, C1-6 haloalkyl, C1-6 hydroxyalkyl, C2-6 alkenyl, C1-6 alkoxy or C2-6 alkenoxy;
L3 is NR10 or O,
each R10 is independently selected from the group consisting of H; C1-6 alkyl; phenyl, optionally substituted with halogen, hydroxy, C1-6 alkyl, C1-6 haloalkyl, C1-6 hydroxyalkyl, C2-6 alkenyl, C4-6 alkoxy or C2-6 alkenoxy; and benzyl, optionally substituted with halogen, hydroxy, C1-6 alkyl, C1-6 haloalkyl, C1-6 hydroxyalkyl, C2-6 alkenyl, C1-6 alkoxy or C2-6 alkenoxy; o, p, q and r are independently from each other 0, 1, 2, 3 or 4 with the proviso that o+p≠0, when G1 is a single bond, and q+r≠0, when G2 is a single bond.

### Claim 10 (depends on 6)

The process of claim 6, wherein the soluble fluorination agent (F) is selected from the group consisting of CsF, NH4F, N2SiF6, (NH4)2SiF6, BF3-isophorone diamine, BF3-isopropylamine, BF3-ethyl amine and BF3-benzyl amine.

### Claim 11 (depends on 6)

The process of claim 6, wherein the soluble fluorination agent is added during treatment with the silicon based solution or immediately after the treatment with the silicon based solution.

### Claim 12 (depends on 6)

The process of claim 6, wherein 0.05 to 3 mol.-% fluorine are added to the silicon based solution via the soluble fluorination agent.

### Claim 13 (depends on 6)

The process of claim 6, wherein the silicon based solution contains a silicon alkoxide, which is added in one or more steps to a reaction mixture.

### Claim 14 (depends on 1)

A process for the manufacture of electronic components using the soft-magnetic powder of claim 1.

### Claim 15 (depends on 6)

A process for the manufacture of electronic components obtained from the process of claim 6.

### Claim 16 (depends on 1)

An electronic component comprising the soft-magnetic powder of claim 1.