Chemistry: electrical current producing apparatus – product – and – Current producing cell – elements – subcombinations and... – Electrode
Reexamination Certificate
1998-07-10
2001-07-03
Chaney, Carol (Department: 1745)
Chemistry: electrical current producing apparatus, product, and
Current producing cell, elements, subcombinations and...
Electrode
C429S231900, C429S231600, C429S231500, C429S209000
Reexamination Certificate
active
06255017
ABSTRACT:
BACKGROUND OF THE INVENTION
This invention relates to electrode materials useful in secondary lithium batteries.
Two classes of materials have been proposed as anodes for secondary lithium batteries. One class includes materials such as graphite and carbon which are capable of intercalating lithium. While the intercalation anodes generally exhibit good cycle life and coulombic efficiency, their capacity is relatively low. A second class includes metals that alloy with lithium metal. Although these alloy-type anodes generally exhibit higher capacities relative to intercalation-type anodes, they suffer from relatively poor cycle life and coulombic efficiency.
SUMMARY OF THE INVENTION
The invention provides electrode materials, and electrode compositions based on these materials, that are suitable for use in secondary lithium batteries. The electrode materials exhibit high initial specific and volumetric capacities that are retained even after repeated cycling, as well as high coulombic efficiencies. The electrode materials, and batteries incorporating these materials, are also readily manufactured.
To achieve these objectives, the invention features, in a first aspect, an electrode composition that includes an electrode material consisting essentially of a plurality of electrochemically active metal elements. The composition may further include additional materials such as carbon, graphite, and combinations thereof. The electrode material has a microstructure that includes the electrochemically active metal elements in the form of a mixture that is essentially free of domains measuring greater than about 1000 angstroms (preferably no greater than about 500 angstroms, more preferably no greater than about 100 angstroms, and even more preferably no greater than about 20 angstroms). Preferably, at least 50% (more preferably at least 80%) by volume of the electrode material is in the form of this mixture. The mixture does not exhibit a discernible electron diffraction or x-ray diffraction pattern characteristic of a crystalline material.
An “electrochemically active metal element” is an element that reacts with lithium under conditions typically encountered during charging and discharging in a lithium battery. The metal element is preferably in the form of an elemental metal.
“Metal element” is used throughout this application to refer to both metals and to metalloids such as silicon and germanium.
A “domain” is a region that consists essentially of a single electrochemically active metal element. The domain may be crystalline (i.e., it gives rise to a discernible electron or x-ray diffraction pattern characteristic of a crystalline material) or non-crystalline. The size of the domain refers to the longest dimension of the domain.
When incorporated in a lithium battery, the electrode composition preferably exhibits (i) a specific capacity of at least about 100 mAh/g for 30 full charge-discharge cycles and (ii) a coulombic efficiency of at least 99% (preferably at least 99.5%, more preferably at least 99.9%) for 30 full charge-discharge cycles when cycled to realize about 100 mAh/g of the composition. Preferably, this level of performance is realized for 500 cycles, more preferably for 1000 cycles.
In another preferred embodiment, the electrode composition, when incorporated in a lithium battery, exhibits (i) a specific capacity of at least about 500 mAh/g for 30 full charge-discharge cycles and (ii) a coulombic efficiency of at least 99% (preferably at least 99.5%, more preferably at least 99.9%) for 30 full charge-discharge cycles when cycled to realize about 500 mAh/g of the composition. Preferably, this level of performance is realized for 200 cycles, more preferably for 500 cycles.
In yet another preferred embodiment, the electrode composition, when incorporated in a lithium battery, exhibits (i) a specific capacity of at least about 1000 mAh/g for 30 full charge-discharge cycles and (ii) a coulombic efficiency of at least 99% (preferably at least 99/5%, more preferably at least 99/9%) for 30 full charge-discharge cycles when cycled to realize about 1000 mAh/g of the composition. Preferably, this level of performance is realized for 100 cycles, more preferably for 300 cycles.
The electrode composition may be in the form of a powder or a thin film. Examples of preferred electrochemically active metal elements include aluminum, silicon, tin, antimony, lead, germanium, magnesium, zinc, cadmium, bismuth, and indium. Particularly preferred electrode compositions feature a combination of (a) aluminum and silicon or (b) tin and silicon.
In a second aspect, the invention features a method of preparing the above-described electrode composition that includes sequentially sputter-depositing sources of electrochemically active metal elements to form the electrode composition in the form of a thin film.
Other features and advantages of the invention will be apparent from the following description of the preferred embodiments thereof, and from the claims.
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Yang et
3M Innovative Properties Co.
Alejandro R.
Chaney Carol
Weiss Lucy C.
Whelan Dorothy A.
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