IP Library Granted Patent US 11,081,690
Granted Patent B2
US 11,081,690 · App. 16/332,122 · Granted Aug 3, 2021

Compositions and uses thereof

Inventors: Pirmin Ulmann (Giubiasco, CH); Sergio Pacheco Benito (Biasca, CH); Simone Zürcher (Origlio, CH); Patrick Lanz (Bellinzona, CH); Michael Spahr (Bellinzona, CH)
Assignee: IMERYS GRAPHITE & CARBON SWITZERLAND LTD.
H01M4/1393H01M4/04H01M4/133H01M4/134H01M4/1395H01M4/364H01M4/386H01M4/583H01M10/052H01M10/0525H01M2004/021H01M2004/027Y02T10/70
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Quick Facts
Patent No.
US 11,081,690
App. No.
16/332,122
Granted
Aug 3, 2021
Kind
B2
Abstract

A silicon-carbon particulate composite suitable for use as active material in a negative electrode of a Li-ion battery, a precursor composition comprising the silicon-carbon particulate composite, a negative electrode comprising the silicon-carbon particulate composite and/or precursor composition, a Li-ion battery comprising the negative electrodes, a method of manufacturing the silicon-carbon particulate composite, precursor composition, negative electrode and Li-ion battery, the use of the silicon-carbon particulate composite in a negative electrode of a Li-ion battery to inhibit or prevent silicon pulverization during cycling, for example, during 1st cycle Li intercalation or de-intercalation and/or to maintain electrochemical capacity after 100 cycles, and a device, energy storage cell, or energy storage and conversion system comprising the silicon-carbon particulate composite and/or precursor composition.

Claims (34)

1. A silicon-carbon particulate composite suitable for use as active material in a negative electrode of a Li-ion battery, comprising:

(i) a microporosity of from about 5.0% to about 25.0%;

(ii) a BJH average pore width of less than about 250 Å; and

(iii) a BJH volume of pores of from about 0.05 cm 3 /g to about 0.25 cm 3 /g;

wherein the carbon comprises natural graphite, synthetic graphite, or a mixture of natural and synthetic graphite.

2. The silicon-carbon particulate composite according to claim 1 , comprising one or more of:

(i) a BET SSA of equal to or lower than about 400 m 2 /g;

(ii) an average particle size of from about 50-2000 Å;

(iii) a microporosity of from about 5% to about 20%;

(iv) a BJH average pore width of from about 75 Å to about 150 Å; and

(v) a BJH volume of pores of at least about 0.50 cm 3 /g.

3. The silicon-carbon particulate composition according to claim 1 , comprising one or more of:

(i) a microporosity of from about 5% to about 15%;

(ii) a BJH average pore width of from about 100 Å to about 180 Å;

(iii) a BJH volume of pores of at least about 0.10 cm 3 /g;

(iv) a BET specific surface area (SSA) of from about 10 m 2 /g to about 100 m 2 /g; and

(v) an average particle size of from about 250 Å to about 1000 Å.

4. The silicon-carbon particulate composite according to claim 1 , wherein the silicon-carbon particulate composite is a co-milled composite.

5. The silicon-carbon particulate composite of claim 1 , wherein the natural or synthetic graphite is exfoliated graphite or expanded graphite.

6. A negative electrode comprising a silicon-carbon particulate composite according to claim 1 .

7. A device comprising the negative electrode according to claim 6 , wherein the device is an electric vehicle or a hybrid electric vehicle, or a plug-in hybrid electric vehicle.

8. A device comprising the negative electrode according to claim 6 , wherein the device comprises an energy storage cell or an energy storage and conversion system.

9. The device according to claim 8 , wherein the energy storage and conversion system comprises a capacitor or a fuel cell.

10. A Li-ion battery comprising an electrode according to claim 6 , wherein silicon pulverization does not occur during 1 st cycle lithium intercalation and de-intercalation and/or wherein electrochemical capacity is maintained after 100 cycles.

11. A negative electrode of a Li-ion battery comprising a silicon-carbon particulate composite according to claim 1 , wherein:

(i) the electrode exhibits reduced silicon pulverization during 1st cycle Li intercalation or de-intercalation,

(ii) the electrode maintains electrochemical capacity after 100 cycles; and

(iii) Li is electrochemically extracted from an amorphous lithium silicon phase and in the substantial absence of two crystalline phases containing crystalline Si silicon metal and crystalline Li 15 S 4 alloy.

12. A negative electrode of a Li-ion battery comprising a silicon-carbon particulate composite according to claim 1 , wherein the electrode exhibits improved cycling stability of the Li-ion battery compared to a Li-ion battery that comprises an active material which is a mixture of silicon particulate and carbonaceous particulate which is not a composite and/or does not have a nanostructure which inhibits or prevents silicon pulverization during cycling, and/or which is not prepared by co-milling and/or does not have a nanostructure which maintains electrochemical after 100 cycles.

13. A precursor composition for a negative electrode of a Li-ion battery, the precursor composition comprising a silicon-carbon particulate composite according to claim 1 , and a further carbonaceous particulate, wherein the further carbonaceous particulate comprises at least two different types of carbonaceous particulate.

14. The precursor composition according to claim 13 , wherein:

(i) the BET SSA of the precursor composition is lower than the BET SSA of the silicon-carbon particulate composite;

(ii) the BET SSA of the precursor composition is equal to or lower than about 10 m 2 /g; and

(iii) the amounts of silicon-carbon particulate composite and further carbonaceous particulate are such that the precursor composition comprises from about 1 wt. % to about 90 wt. % silicon, based on the total weight of the precursor composition.

Assignments (1)
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Mar 12, 2019
From: ULMANN, PIRMIN; PACHECO BENITO, SERGIO; ZÜRCHER, SIMONE; LANZ, PATRICK; SPAHR, MICHAEL
To: IMERYS GRAPHITE & CARBON SWITZERLAND LTD.
Reel/Frame 048567/0324 →
Priority Claims (1)
EP 16188389 · Sep 12, 2016 · regional
Continuity (1)
Related Publication 20190237749A1 · Aug 1, 2019