Carbon-Coated Silicon Particle Powder as the Anode Material for Lithium Ion Batteries and Method of Making the Same

a lithium ion battery and carbon-coated silicon technology, applied in the field of carbon-coated silicon particles as lithium ion battery anode material, can solve the problems of low relative lithium capacity, high cost of lithium ion batteries using synthetic graphite electrodes, and low efficiency of lithium ion batteries. achieve good powder flowability, high efficiency, and high capacity

Inactive Publication Date: 2009-05-21
CONOCOPHILLIPS CO
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Benefits of technology

[0008]The compositions of the invention provide high capacity and high efficiency carbon-coated silicon / carbon composite particles that can be derived from a wide variety of carbon sources. In a further aspect of the invention, the silicon / carbon composite particle may be coated with multiple layers of carbon residue forming material. In a still further aspect of the invention, the coating layer(s) of the composite particle may be optionally carbonized.
[0009]The compositions of the present invention provide carbon-coated silicon / carbon composite particles with substantially smooth coatings. Additionally, the compositions feature good powder flowability, which is particularly beneficial during the handling or manufacturing steps necessary to form these materials into useful electrodes or into other articles not specifically described herein.
[0010]In further aspects of the invention there are provided methods for the manufacture of such carbon-coated silicon / carbon composite particles. The carbon-coated powders prepared in accordance with the invention not only increase charge efficiency but also provide excellent processability for electrode fabrication. In a yet further aspect of the invention there are provided methods for the manufacture of electrical storage cells, particularly rechargeable batteries that include said carbon-coated composite particles. A still further aspect of the invention relates to the use of said carbon-coated composite particles in electrical storage cells, particularly in rechargeable batteries.

Problems solved by technology

Nonetheless, rechargeable lithium ion storage cells are not without deficiencies.
Commercial lithium ion batteries which use synthetic graphite electrodes are expensive to produce and have low relatively lithium capacities.
Additionally, graphite products currently used in lithium ion electrodes are near their theoretical limits for energy storage (372 mAhr / g).
However, pure silicon is a poor electrode material because its unit cell volume can increase to more than 300% when lithiated.
This volume expansion during cycling destroys the mechanical integrity of the electrode and leads to a rapid capacity loss during battery cycling.
Although silicon can hold more lithium than carbon, when lithium is introduced to silicon, the silicon disintegrates and results in less electrical contact which ultimately results in decreased ability to recharge the storage cell.
Continuous research efforts in solving silicon volume expansion problems have yielded limited results.
However, chemical vapor deposition methods typically used to apply silicon coatings or carbon coatings have intrinsic shortcomings that include slow deposition rates and / or expensive precursors for deposition.
Vapor deposited silicon films may be extremely expensive relative to the cost of bulk silicon powders.

Method used

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  • Carbon-Coated Silicon Particle Powder as the Anode Material for Lithium Ion Batteries and Method of Making the Same
  • Carbon-Coated Silicon Particle Powder as the Anode Material for Lithium Ion Batteries and Method of Making the Same
  • Carbon-Coated Silicon Particle Powder as the Anode Material for Lithium Ion Batteries and Method of Making the Same

Examples

Experimental program
Comparison scheme
Effect test

example 1

Material Preparation

[0057]The silicon powder used in this example had an average particle size of 5 μm (from Johnson Matthey Company). The pitch used for the coating layer was a petroleum pitch from Conoco, Inc. that was approximately 27% insoluble in xylene. The procedure for coating pitch on silicon powder is as follows. First, 20 grams of the silicon powder was mixed with about 100 ml of xylene so that silicon particles were uniformly dispersed in xylene in a glass flask. Concurrently, 14 grams of the pitch was mixed with an equal amount of xylene in another flask so that the pitch was completely dissolved in xylene. Both the solutions were heated to approximately 110° C. and the pitch solution was added into the silicon solution while being continuously mixed. The resulting solution was then heated to 140° C. and continuously stirred for about 15 minutes. The solution was removed from the heater and the solution gradually cooled to ambient temperature (˜25° C.). While the soluti...

example 2

[0064]Twenty grams of a natural flake graphite powder (average particle size 5 μm from China) were coated with 10 wt % petroleum pitch according to the procedure as described in Example 1. The coated graphite powder was stabilized, carbonized, and graphitized at 3000° C. in argon. Concurrently, a silicon powder (average particle size 2 μm, purchased from Johnson Matthey company) was coated with 10 wt % pitch as described in Example 1, stabilized, and carbonized at 1050° C. A mixture of the coated natural graphite powder and the coated silicon powder were combined in the proportion of 6 parts coated graphite and 4 parts of coated silicon powder and coated with 15 wt % solution of the same pitch using the same method. After stabilization in air, the resulting composite powder was carbonized at 1050° C. in nitrogen atmosphere. The resulting graphite / silicon / carbon composite particle powder has morphology as shown in FIG. 3. It can be seen that small silicon particles are embedded in th...

example 3

[0066]Twenty grams of a natural flake graphite powder (average particle size 5 μm from China) were coated with 7 wt % petroleum pitch according to the procedure as described in example 1. The coated graphite powder was stabilized and carbonized at 1200° C. The coated graphite powder was mixed with the coated silicon powder as described in Example 2, in the same proportions. The mixture was then coated with 15 wt % pitch as described in Example 1 and stabilized. Subsequently, the resulting composite particle powder was coated again with 10 wt % pitch, stabilized, and carbonized at 1050° C. in nitrogen atmosphere. The material was evaluated as the anode material for Li-ion batteries in the same manner as described previously. The capacity and efficiency of this material are shown in FIG. 5 for the first five cycles. A significant increase in the rechargeability of the silicon powder is displayed.

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Abstract

A process for the production of coated silicon / carbon particles comprising:providing a carbon residue forming material;providing silicon particles;coating said silicon particles with said carbon residue forming material to form coated silicon particles;providing particles of a carbonaceous material;coating said particles of carbonaceous material with said carbon residue forming material to form coated carbonaceous particles;embedding said coated silicon particles onto said coated carbonaceous particles to form silicon / carbon composite particles;coating said silicon / carbon composite particles with said carbon residue forming material to form coated silicon / carbon composite particles; andstabilizing the coated composite particles by subjecting said coated composite particles to an oxidation reaction.The coated composite particles will have a substantially smooth coating. The particles may be coated with multiple layers of carbon residue forming material /

Description

TECHNICAL FIELD OF THE INVENTION[0001]The present invention relates to silicon / carbon composite materials that are useful as electrode active materials in batteries. More particularly, the present invention relates to carbon-coated silicon particles that find particular use as electrode materials, as well as methods for the manufacture of said carbon-coated silicon particles.BACKGROUND OF THE INVENTION[0002]Synthetic graphites are widely used as standard negative electrode materials in lithium ion batteries. Other carbonaceous materials are also widely used in such batteries due to their efficiency and reasonable cost. Lithium ion batteries are primarily used as power sources in portable electronic devices. Compared to other classes of rechargeable batteries such as nickel-cadmium and nickel-metal hydride storage cells, lithium ion cells have become increasingly popular due to relatively high storage capacity and rechargeability.[0003]Due to increased storage capacity per unit mass ...

Claims

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Application Information

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Patent Type & Authority Applications(United States)
IPC IPC(8): H01M4/58B32B9/00H01M10/00H01M6/00B05D7/00B23P19/00C25D17/10H01M4/02H01M4/04H01M4/13H01M4/133H01M4/134H01M4/36H01M4/38H01M4/583H01M10/0525H01M10/36H01M50/541
CPCC25D17/10Y10T428/2995H01M4/0471H01M4/13H01M4/133H01M4/134H01M4/366H01M4/38H01M4/583H01M10/0525H01M2004/021H01M2004/027Y02E60/122Y10T29/53135Y10T29/49108H01M4/0416Y02E60/10H01M4/36H01M4/58
Inventor MAO, ZHENHUACHAHAR, BHARAT
Owner CONOCOPHILLIPS CO
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