IP Library › Granted Patent US 10,305,107
Granted Patent B2
US 10,305,107 · App. 14/390,411 · Granted May 28, 2019

Surface-modified low surface area graphite, processes for making it, and applications of the same

Inventors: Michael E. Spahr (Bellinzona, CH); Pirmin A. Ulmann (Giubiasco, CH); Simone Zurcher (Bellinzona, CH); Michal Gulas (Malvaglia, CH); Flavio Mornaghini (Breganzona, CH)
Assignee: Imerys Graphite & Carbon Switzerland Ltd.
H01M4/587C01B32/21C23C16/00C23C16/26C23C16/56Y10T428/2982
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Quick Facts
Patent No.
US 10,305,107
App. No.
14/390,411
Granted
May 28, 2019
Kind
B2
Abstract

Surface-modified, low surface area synthetic graphite may have a BET surface from 1.0 to 4.0 m 2 /g and a crystallite size L c to crystallite size L a ratio of greater than 1. Processes for modifying the surface of low surface area synthetic graphite may result in surface-modified, low surface area synthetic graphite have a BET surface from 1.0 to 4.0 m 2 /g and a crystallite size L c to crystallite size L a ratio of greater than 1. Such synthetic graphite may have many uses, including for example, as a negative electrode material in lithium-ion batteries.

Claims (78)

1. Surface-modified synthetic graphite, wherein the surface-modified synthetic graphite:

has a BET surface area from about 1.0 to about 4 m 2 /g;

has a crystallite size L c (as measured by XRD) from 50 to 200 nm;

has a crystallite size L a (as measured by Raman spectroscopy) from 5 to 100 nm; and

exhibits a ratio (L c /L a ) of the perpendicular axis crystallite size L c (measured by XRD) to the parallel axis crystallite size L a (measured by Raman spectroscopy) of greater than 1.5.

2. The surface-modified synthetic graphite of claim 1 , further characterized by at least one of the following characteristics:

i) a BET surface area ranging from 1 to 3.5 m 2 /g;

ii) an ash content of below 0.04%;

iii) a particle size distribution (D90) ranging from 10 to 50 μm;

iv) a particle size distribution (D50) ranging from 5 to 40 μm;

v) an Fe content of below 20 ppm;

vi) an oxygen content of greater than 50 ppm; and

vii) a tapped density of greater than 0.8 g/cm 3 .

3. The surface-modified synthetic graphite of claim 1 , further characterized by at least one of the following characteristics:

i) a pH value ranging from 5.0 to 6.5;

ii) a xylene density from 2.24 to 2.26 g/cm 3 ; and

iii) exhibiting an ID/IG ratio (R(ID/IG)) of below about 0.3 when measured with a laser having excitation wavelength of 632.8 nm.

4. The surface-modified synthetic graphite of claim 3 , characterized by the following characteristics:

i) a BET surface ranging from 2.3 to 3 m 2 /g;

ii) a crystallite size L c ranging from 100 to 180 nm;

iii) a crystallite size L a ranging from 10 to 40 nm;

iv) a pH value ranging from 5.2 to 6.0;

v) an oxygen content of greater than 90 ppm;

vi) a tapped density of greater than 0.98 g/cm 3 ; and

vii) a particle size distribution (D90) ranging from 25 to 35 μm.

5. The surface-modified synthetic graphite of claim 3 , wherein the graphite is obtainable by oxidation of synthetic graphite with a BET surface area ranging from 1 m 2 /g to about 3.5 m 2 /g at temperatures from 500 to 1100° C. with treatment times ranging from 2 to 30 minutes.

6. Surface-modified synthetic graphite, wherein the surface-modified synthetic graphite:

has a BET surface area from about 1.0 to about 4 m 2 /g;

has a crystallite size L c (as measured by XRD) from 50 to 200 nm;

has a crystallite size L a (as measured by Raman spectroscopy) from 5 to 100 nm;

exhibits a ratio (L c /L a ) of the perpendicular axis crystallite size L c (measured by XRD) to the parallel axis crystallite size L a (measured by Raman spectroscopy) of greater than 1.5; and

has an oxygen content of greater than 50 ppm.

7. The surface-modified synthetic graphite of claim 6 , further characterized by at least one of the following characteristics:

i) a pH value ranging from 5.0 to 6.5;

ii) a xylene density from 2.24 to 2.26 g/cm 3 ; and

iii) exhibiting an ID/IG ratio (R(ID/IG)) of below about 0.3 when measured with a laser having excitation wavelength of 632.8 nm.

8. The surface-modified synthetic graphite of claim 6 , characterized by the following characteristics:

i) a BET surface ranging from 2.3 to 3 m 2 /g;

ii) a crystallite size L c ranging from 100 to 180 nm;

iii) a crystallite size L a ranging from 10 to 40 nm;

iv) a pH value ranging from 5.2 to 6.0;

v) an oxygen content of greater than 90 ppm;

vi) a tapped density of greater than 0.98 g/cm 3 ; and

vii) a particle size distribution (D90) ranging from 25 to 35 μm.

9. The surface-modified synthetic graphite of claim 6 , further characterized by at least one of the following characteristics:

i) a BET surface area ranging from 1 and 2 m 2 /g; and

ii) a xylene density ranging from 2.1 to 2.26 g/cm 3 .

10. The surface-modified synthetic graphite of claim 6 , wherein the surface-modified synthetic graphite is characterized by the following characteristics:

i) a BET surface area ranging from 1.3 to 1.8 g/cm 3 ;

ii) a crystallite size L c ranging from 100 to 160 nm; and

iii) a crystallite size L a ranging from 20 to 60 nm.

11. The surface-modified synthetic graphite of claim 6 , wherein said graphite is obtainable by chemical vapor deposition (CVD) on a synthetic graphite starting material at temperatures from 500 to 1000° C. with hydrocarbon gas and treatment times ranging from 3 to 120 minutes.

12. Surface-modified synthetic graphite, wherein the surface-modified synthetic graphite:

has a BET surface area from about 1.0 to about 4 m 2 /g;

has a crystallite size L c (as measured by XRD) from 50 to 200 nm;

has a crystallite size L a (as measured by Raman spectroscopy) from 5 to 100 nm;

exhibits a ratio (L c /L a ) of the perpendicular axis crystallite size L c (measured by XRD) to the parallel axis crystallite size L a (measured by Raman spectroscopy) of greater than 1.5; and

has a particle size distribution (D50) ranging from 5 to 40 μm.

13. The surface-modified synthetic graphite of claim 12 , further characterized by at least one of the following characteristics:

i) a pH value ranging from 5.0 to 6.5;

ii) a xylene density from 2.24 to 2.26 g/cm 3 ; and

iii) exhibiting an ID/IG ratio (R(ID/IG)) of below about 0.3 when measured with a laser having excitation wavelength of 632.8 nm.

14. The surface-modified synthetic graphite of claim 12 , characterized by the following characteristics:

i) a BET surface ranging from 2.3 to 3 m 2 /g;

ii) a crystallite size L c ranging from 100 to 180 nm;

iii) a crystallite size L a ranging from 10 to 40 nm;

iv) a pH value ranging from 5.2 to 6.0;

v) an oxygen content of greater than 90 ppm;

vi) a tapped density of greater than 0.98 g/cm 3 ; and

vii) a particle size distribution (D90) ranging from 25 to 35 μm.

15. The surface-modified synthetic graphite of claim 12 , further characterized by at least one of the following characteristics:

i) a BET surface area ranging from 1 and 2 m 2 /g; and

ii) a xylene density ranging from 2.1 to 2.26 g/cm 3 .

16. The surface-modified synthetic graphite of claim 12 , wherein the surface-modified synthetic graphite is characterized by the following characteristics:

i) a BET surface area ranging from 1.3 to 1.8 g/cm 3 ;

ii) a crystallite size L c ranging from 100 to 160 nm; and

iii) a crystallite size L a ranging from 20 to 60 nm.

17. The surface-modified synthetic graphite of claim 12 , wherein said graphite is obtainable by chemical vapor deposition (CVD) on a synthetic graphite starting material at temperatures from 500 to 1000° C. with hydrocarbon gas and treatment times ranging from 3 to 120 minutes.

Assignments (1)
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Dec 3, 2014
From: SPAHR, MICHAEL E.; ULMANN, PIRMIN A.; ZURCHER, SIMONE; GULAS, MICHAL; MORNAGHINI, FLAVIO
To: IMERYS GRAPHITE & CARBON SWITZERLAND LTD.
Reel/Frame 034364/0494 →
Priority Claims (1)
EP 12163479 · Apr 5, 2012 · regional
Continuity (1)
Related Publication 20150079477A1 · Mar 19, 2015