COMPOSITIONS FOR USE IN NEGATIVE ELECTRODES

1 . A method of making a negative electrode composition, the method comprising:

preparing and mixing a slurry comprising: a polymer containing material and a crosslinking containing material in an aqueous solvent;

adding and mixing a silicon containing material;

drying under an inert atmosphere, and

annealing under an insert atmosphere to provide the negative electrode composition, wherein

the silicon containing material is in the form of grains having a Sherrer grain size of less than 50 nm, being free of doped lithium,

the negative electrode composition has a surface area of less than 20 m 2 /g;

the polymer containing material is a vinylic monomer comprising one or more functional groups selected from the group comprising vinyl groups, propargyl groups, azide groups, carboxylic acid groups, phosphonic acid groups, hydroxyl groups, N-methylolamido groups or alkoxysilyl groups;

the crosslinking containing material is an aziridine.

2 . The method of claim 1 , wherein in addition to the silicon containing material, one or more additional electrochemically active materials are added selected from the group comprising one or more of graphite, binders, conductive diluents, fillers, adhesion promoters, thickening agents for dispersion viscosity modifications or any combinations thereof.

3 . The method of claim 2 , wherein the graphite is present in the negative electrode composition in an amount of greater than 10 wt. %, greater than 20 wt. %, greater than 50 wt. %, greater than 70 wt. % or greater, based upon the total weight of the negative electrode composition.

4 . The method of claim 2 , wherein the graphite is present in the negative electrode composition in an amount of between 20 wt. % and 90 wt. %, between 30 wt. % and 80 wt. %, between 40 wt. % and 60 wt. %, between 45 wt. % and 55 wt. %, between 80 wt. % and 90 wt. %, or between 85 wt. % and 90 wt. %, based upon the total weight of the electrode composition.

5 . The method of claim 2 , wherein the binder is selected from the group comprising one or more of styrene-butadiene-rubber/sodium carboxymethylcellulose, acrylic acid (co)polymers and their alkali metal salts, fluoropolymer/acrylic (co)polymer blends.

6 . The method of claim 5 , wherein the binder is present in the electrode composition in an amount of less than 50 wt. %, less than 40 wt. %, less than 30 wt. %, less than 20 wt. %, less than 10 wt. %, less than 5 wt. %, less than 1 wt. %, or less than 0.1 wt. %, based on the total weight of the binder.

7 . The method of claim 1 , wherein the vinylic monomer is selected from one or more additional or alternative cross-linkable vinylic monomers which may include allyl (meth)acrylate, 2-hydroxyethyl (meth)acrylate, 3-trimethoxysilylpropyl(meth)acrylate, and 3-triethoxysilylpropyl (meth)acrylate or any combinations thereof.

8 . The method of claim 1 , wherein in addition to the vinylic monomers, the vinylic monomers may be selected from the group comprising monofunctional vinylic monomers, alkali metal salts of (meth)acrylic acid, alkyl esters or amides of (meth)acrylic acid containing 1 to 18 carbon atoms in the alkyl group, methyl (meth)acrylate or 2 ethylhexyl (meth)acrylate or stearyl (meth)acrylate or dimethylacrylamide, or substituted alkyl esters or amides of (meth)acrylic acid, hydroxyethyl acrylate or tetrahydrofurfuryl acrylate or glycidyl methacrylate or methoxy-poly(ethylene glycol)(meth)acrylate.

9 . The method of claim 8 , wherein the monofunctional vinylic monomers are selected from the group comprising one or more styrenic compounds selected from styrene, alpha-methyl styrene; N-vinylimidazole; 4-vinylpyridine; organic nitriles selected from the group comprising acrylonitrile; N-vinylcaprolactam, or N-vinylpyrrolidone; vinylphosphonic acid; or fluorine-containing vinylic monomers.

10 . The method of claim 1 , wherein the silicon containing material is selected from the group comprising elemental silicon, silicon oxide, silicon carbide, or a silicon containing alloy.

11 . The method of claim 10 , wherein the silicon containing alloy in which the silicon has the formula: SixMyCz, where x, y, and z represent atomic % values and (a) x+y+z=100%; (b) x>2y+z; (c) x and y are greater than 0; z is equal to or greater than 0; (d) M is iron and optionally one or more other metals selected from manganese, molybdenum, niobium, tungsten, tantalum, copper, titanium, vanadium, chromium, nickel, cobalt, zirconium, yttrium, or combinations thereof.

12 . The method of claim 11 , wherein 65%≤x≤85%, 70%≤x≤80%, 72≤x≤74%, or 75≤x≤77%; 5%≤y≤20%, 14≤y≤7%, or 13≤y≤14%; and 5%≤z≤15%, 5%≤z≤8%, or 9≤z≤12%.

13 . The method of claim 11 , wherein x, y, and z are greater than 0.

14 . The method of claim 1 , wherein the negative electrode composition is in the form of particles having a D10 of at least 0.5 μm, at least 1.0 μm, at least 1.5 μm, at least 2 μm, at least 2.5 μm, at least 3.0 μm, or at least 5.0 μm; a D50 of no greater than 20 μm, no greater than 10 μm, no greater than 7 μm, no greater than 5 μm, or no greater than 3 μm; and D90 of no greater than 50 μm, no greater than 40 μm, no greater than 30 μm, no greater than 25 μm, no greater than 20 μm, no greater than 15 μm, or no greater than 10 μm.

15 . The method of claim 1 , wherein the negative electrode composition is in the form of particles and has a surface area of less than less than 12 m 2 /g, less than 10 m 2 /g, less than 5 m 2 /g, less than 4 m 2 /g, or even less than 2 m 2 /g.

16 . The method of claim 1 , wherein the silicon containing material is coated with one or more coatings disposed on and at least partially surrounding the silicon containing material.