Volume change compensated silicon-silicon oxide-lithium composite material having nano silicon particles embedded in a silicon:silicon lithium silicate composite matrix, and cyclical ex-situ manufacturing processes

1. A method for producing a volume change compensated silicon-silicon oxide-lithium composite (SSLC) material, the method comprising:

producing an initially prelithiated SSLC material;

delithiating the initially prelithiated material to produce a delithiated SSLC material; and

performing at least one iteration of a volume change compensation process comprising:

(a) re-prelithiating the delithiated SSLC material to produce a re-prelithiated SSLC material, and

(b) delithiating the re-prelithiated SSLC material produced in (a),

wherein at least one of the following is satisfied:

(i) prior to performing the at least one iteration of the volume change compensation process the initially prelithiated SSLC material is completely lithiated, and

(ii) the at least one iteration of the volume change compensation process produces a re-prelithiated SSLC material that is completely prelithiated,

wherein in a final iteration of the volume change compensation process, delithiating the re-prelithiated SSLC material produced in (a) comprises completely delithiating the re-prelithiated SSLC material to produce the volume change compensated SSLC material, and

wherein the volume change compensated SSLC material is produced ex situ with respect to fabrication of an anode that contains the produced volume change compensated SSLC material.

2. The method of claim 1 , wherein the volume change compensated SSLC material comprises a porous plastically deformable Si:Lithium Silicate Composite (Si:LSC) matrix having nano silicon particles embedded therein.

3. The method of claim 1 , wherein the initially prelithiated SSLC material and the re-prelithiated material produced during each iteration of the volume change compensation process are produced in slurry form.

4. The method of claim 1 , wherein the volume change compensation process is repeated 3-12 times.

5. The method of claim 1 , wherein in each iteration of the volume change compensation process, the re-prelithiated SSLC material is completely prelithiated.

6. The method of claim 1 , wherein in a selected iteration of the volume change compensation process, the re-prelithiated SSLC material has a higher lithium content than in another iteration of the volume change compensation process.

7. The method of claim 1 , wherein each delithiating of the re-prelithiated SSLC material completely delithiates the re-prelithiated SSLC material.

8. The method of claim 1 , wherein delithiating the initially prelithiated SSLC material and delithiating the re-prelithiated SSLC material comprises exposing the initially prelithiated SSLC material and exposing the re-prelithiated SSLC material, respectively, to a delithiating agent comprising at least one of a carboxylic acid, a sulfonic acid, and an alcohol.

9. The method of claim 8 , wherein the delithiating agent comprises at least one of: formic acid (methanoic acid), HCOOH (pK a =3.8); acetic acid (ethanoic acid), CH 3 COOH (pK a =4.7); propionic acid (propanoic acid), CH 3 CH 2 COOH (pK a =4.9); butyric acid (butanoic acid), CH 3 CH 2 CH 2 COOH (pK a =4.8);valeric acid (pentanoic acid), CH 3 CH 2 CH 2 CH 2 COOH (pK a =4.8); caprioc acide (hexanoic acide), CH 3 CH 2 CH 2 CH 2 CH 2 COOH (pK a =4.9); oxalic acid (ethanedioic acid), (COOH)(COOH)(pK a =1.2);lactic acid (2-hydroxypropanoic acid), CH 3 CHOHCOOH (pK a =3.9); malic acid (2-hydroxybutanedioic acid), (COOH)CH 2 CHOH(COOH) (pK a =3.4); citric acid (2-hydroxypropane- 1,2,3 -tricarboxylic acid), CH 2 (COOH)COH(COOH)CH 2 (COOH) (pK a =3.1); benzoic acid (Benzenecarboxylic acid [IUPAC ] or phenylmethanoic acid, non-IUPAC), C 6 H 5 COOH (pK a =4.2); carbonic acid (hydroxymethanoic acid, non-IUPAC name), OHCOOH or H 2 CO 3 (pK a =3.6); phenol (carbolic acid or hydroxybenzene, non-IUPAC names), C 6 H 5 OH (pK a =9.9); uric acid (7,9-Dihydro-1H -purine-2,6,8(3H)-trione), C 5 H 4 N 4 O 3 (pK a =−1.1); taurine (2-aminoethanesulfonic acid), C 2 H 7 NO 3 S (pK a =9.0); p-toluenesulfonic acid (4-methylbenzenesulfonic acid), CH 3 C 6 H 4 SO 3 H (pK a =−2.8); and trifluoromethanesulfonic acid, CF 3 SO 3 H (pk a =−12).

10. The method of claim 8 , wherein the delithiating agent comprises at least one of:

(a) a monohydric alcohol selected from among: methanol, CH 3 OH; ethanol, C 2 H 5 OH; propan-2-ol, C 3 H 7 OH; butan-1-ol, C 4 H 9 OH; pentan-1-ol, C 5 H 11 OH; and hexadecan-1-ol, C 16 H 33 OH;

(b) a polyhydric alcohol selected from among: ethane-1,2-diol, C 2 H 4 (OH) 2 ; propane-1,2-diol, C 3 H 6 (OH) 2 ; propane-1,2,3-triol, C 3 H 5 (OH) 3 ; butane-1,2,3,4-tetraol, C 4 H 6 (OH) 4 ; pentane-1,2,3,4,5-penotol, C 5 H 7 (OH) 5 ; hexane-1,2,3,4,5,6-hexol, C 6 H 8 (OH) 6 ; and heptane-1,2,3,4,5,6,7-heptol, C 7 H 9 (OH) 7 ;

(c) an unsaturated aliphatic alcohol selected from among prop-2-ene-1-ol, C 3 H 5 OH; 3,7-dimethylocta-2,6-dien-1-ol, C 10 H 17 OH; and prop-2-yn-1-ol, C 3 H 3 OH;

(d) an alicyclic alcohol selected from among: cyclohexane-1,2,3,4,5,6-hexol, C 6 H 6 (OH) 6 ; and 2-(2-propyl)-5-methyl-cyclohexane-1-ol, C 10 H 19 OH; and

(e) polyvinyl alcohol (PVA) [CH 2 CH(OH)] n .

11. A method for fabricating an anode for a lithium ion battery, comprising:

producing a volume change compensated silicon:silicon oxide:lithium composite (SSLC) material by:

producing an initially prelithiated SSLC material;

delithiating the initially prelithiated material to produce a delithiated SSLC material; and

performing at least one iteration of a volume change compensation process comprising:

(a) re-lithiating the delithiated SSLC material to produce a re-prelithiated SSLC material, and

(b) delithiating the re-prelithiated SSLC material produced in (a);

wherein at least one of the following is satisfied:

(i) prior to performing the at least one iteration of the volume change compensation process the initially prelithiated SSLC material is completely lithiated, and

(ii) at least one iteration of the volume change compensation process produces a re-prelithiated SSLC material that is completely prelithiated,

wherein in a final iteration of the volume change compensation process, delithiating the re-prelithiated SSLC material produced in (a) comprises completely delithiating the re-prelithiated SSLC material to produce the volume change compensated SSLC material, and

after producing the volume change compensated SSLC material, fabricating an anode structure containing the produced volume change compensated SSLC material.